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| 1.
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小村, 和久 ; 稲垣, 美幸 ; 西川, 方敏 ; 中西, 孝 ; 早川, 和一 ; 唐, 寧 ; 楊, 小陽 ; 飯田, 孝夫 ; 森泉, 純 ; Komura, Kazuhisa ; Inagaki, Miyuki ; Nishikawa, Katatoshi ; Hayakawa, Kazuichi ; Tang, Ning ; Yang, Xiaoyang ; Iida, Takao ; Moriizumi, Jyun
概要:
金沢大学環日本海域環境研究センター<br />Variations of radiation levels before and after the Noto Hanto Earthquake in 2007 have been analy
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zed from the point of view of environmental radioactivity. The 210Pb activities in the airborne particles are collected from Nishi-Futamata in Wajima, are analyzed. The Radon activity at Hegura Island located 50km North of Wajima, and the spatial gamma rays at Nishi-Futamata are measured since April 21, 2007. Abnormal increase of 210Pb activity started 3 weeks before the earthquake are found, suggesting the maximum value just before the earthquake, because it decrease to normal level after 2 weeks. Increase of radon level was not observed at Hegura Island, however, increase of radiation level at Nishi-Futamata area continued for 6 weeks after the earthquake, and settled to normal level in middle of May 2007.<br />環境放射能の観点から能登半島地震発生前後の放射能関連のデータの解析を試みた.解析したのは,輪島市西二又地区で採取した大気浮遊塵中の210Pb,輪島沖50kmに位置する舳倉島のラドン濃度,地震発生後の4月21日から西二又地区で連続測定を実施した空間γ線レベルの3項目である.その結果,地震発生約3週間前から大気浮遊塵試料のラドンの娘核種210Pbの濃度が増加し,地震直前にピークに達した後に低下に転じ,約2週間後にほぼ平常値に回復していたことが分かった.舳倉島のラドンには地震の影響は見られなかったが,西二又における空間γ線レベルはラドンに由来すると考えれる高い値が約6週間後も続き5月中頃に平常値に戻ったことが明らかになった.
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Hayakawa, Kazuichi ; Miyoshi, Yasuko ; Kurimoto, Hiroaki ; Matzushima, Yuko ; Takayama, Nariaki ; Tanaka, Seishi ; Miyazaki, Motoichi ; 早川, 和一 ; 三好, 裕子 ; 栗本, 博昭 ; 松島, 優子 ; 高山, 成明 ; 田中, 星司 ; 宮崎, 元一
概要:
金沢大学理工研究域自然システム学系<br />A HPLC determination method for methamphetamine (MA) and its metabolites in the urine samples of
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abusers has been developed. MA, amphetamine (AP), norephedrine (NE), p-hydroxymethamphetamine (pOHMA), p-hydoroxyamphetamine (pOHAP) and an internal standard, namely β-phenylethylamine (PEA) were derivatized with dansyl chloride. They were separated on a reversed phase column with gradient elution using an acetonitrile/tetrahydrofuran/imidazole buffer mobile phase and chemilumigenically determined using bis(2, 4, 6-trichlorophenyl)-oxalate/hydrogen peroxide as post column reagents. The lower determination limits were as low as 1×10-14-3×10-14mol. AP, NE, pOHAP and PEA were derivatized with naphthalene-2, 3-dicarboxaldehyde, and were separated on a reversed phase column using an acetonitrile/imidazole buffer mobile phase and chemilumigenically determined. The lower determination limits were 3×10-16-1.5×10-15mol. Enzymatic hydrolysis of glucuronides of pOHMA (pOHMAG) and pOHAP (pOHAPG) allowed them to be determined as pOHMA and pOHAP, respectively. After adjusting the pH of the urine samples to 10.5 and adding PEA, all metabolites except glucuronides were extracted quantitatively into chloroform-isopropanol (3 : 1). Utilizing the two methods, MA and all metabolites were determined in urine samples of MA abusers. The tendency, in order of decreasing concentration was : [MA]>[A]>[pOHMAG]>[pOHMA]>[NE]>[pOHAPG]>[pOHAP]. Although ephedrine (EP) was detected in several samples, it was not considered to be a metabolite of MA but rather a component derived from cough medicine.
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早川, 和一 ; Hayakawa, Kazuichi
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金沢大学理工研究域自然システム学系
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山本, 敦 ; 早川, 和一 ; Yamamoto, Atsushi ; Hayakawa, Kazuichi
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金沢大学理工研究域自然システム学系
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早川, 和一 ; Hayakawa, Kazuichi
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金沢大学理工研究域自然システム学系
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後藤, 純雄 ; 峯木, 茂 ; 杉田, 和俊 ; 遠藤, 治 ; 村山, 留美子 ; 内山, 巌雄 ; 田中, 基裕 ; 早川, 和一 ; Goto, Sumio ; Mineki, Shigeru ; Sugita, Kazutoshi ; Endo, Osamu ; Murayama, Rumiko ; Uchiyama, Iwao ; Tanaka, Motohiro ; Hayakawa, Kazuichi
概要:
金沢大学理工研究域自然システム学系<br />ナホトカ号から流出し日本海沿岸に漂着した重油の汚染状況を把握するための調査研究の一環として, 平成9年1月16日に採取した漂着重油, ナホトカ号船首部分の重油および市販C重油中に含まれる多環芳香
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族炭化水素 (PAH) の分析及び抽出物の変異原性を測定した。その結果, 漂着重油のベンゾ (a) ピレン (BaP) 含有量は1984年に採取された東京都市部の土砂51試料の平均値の約1/4であることやその変異原比活性は同土砂の約4倍であることなどを認めた。<br />As a part of research studies on the pollution at heavy-oil coated parts of the Sea of Japan coastline, resulting from the wrecked Russian tanker Nakhodka on Jan. 2, the following experiments were performed using three heavy oil samples. Polycyclic aromatic hydrocarbons (PAH) were analyzed by HPLC in the heavy oil that washed ashore, which was collected at Mikuni-cho in Fukui Prefecture on Jan. 16, 1997, heavy oil in the oil compartment of the bow of the tanker, and commercial heavy oil (class C) .Mutagenicities of the extracts of these oil samples were also measured. The amount of benzo (a) pyrene (BaP) contained in the heavy oil that washed ashore was about a quarter of the average in 51 soil extracted samples, which were collected at an urban area in Tokyo in 1984, and mutagenicity of the extract from the oil was about 4-fold higher than the average in the extracts from the soil samples.
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佐川, 岳人 ; 西, 香菜子 ; 納富, 美穂 ; 平岡, 龍之 ; 塚本, 和巳 ; 早川, 和一 ; Sagawa, Takehito ; Nishi, Kanako ; Notomi, Miho ; Hiraoka, Tatsuyuki ; Tsukamoto, Kazumi ; Hayakawa, Kazuichi
概要:
金沢大学理工研究域自然システム学系<br />生スィートバジルを乾燥する際に引き起こされる香りの変化を，香気成分バランスやスィートバジルの組織構造とそのレオロジー特性について，比較解析を行う事で，生スィートバジルの香りを維持する為に必要とさ
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れる因子の探索を行った．スィートバジルの香気寄与成分として特定したシネオール，リナロール，オイゲノール，オクタナール，1-オクタノール，(E)-2-ヘキセナール，(Z)-3-ヘキセノールの7種類の香気成分は官能評価の特徴を説明する因子となると考えられる．その中でも，生スィートバジルの香りを特徴づける因子としては，微量成分バランスが大きな役割を果たし，ハーブ自体には (E)-2ヘキセナールや (Z)-3-ヘキセノールが存在するが，それがハーブティーに溶出されずオクタナールが高い比率で溶出されることが重要であった．そのような性質を持つ組織構造は，葉内部の細胞壁の形状が乾燥工程を経ても維持されており，その状態は貯蔵弾性率の測定でも比較説明が可能であることが明らかになった．これらの結果により，ハーブの組織構造とハーブティーとして溶出される香気成分バランスに密接な関係がある可能性が示唆された．但し，今回確認された (E)-2-ヘキセナールや (Z)-3-ヘキセノールはみどりの香りと称される物質の1つである．これらの物質は植物中のリノレン酸や配糖体を前駆体として酵素が関与し発現するものであり12)，食品加工時に発生することも知られている14）～16) ．今後は配糖体量の変化と酵素の関係についても検討を行い，組織構造変化の香りに対する影響をより明確にしてゆく必要があると考える．しかしながら，細胞壁の損傷が少ない状態であった真空乾燥スィートバジルが生特有の香りを保持していたという事実から，乾燥工程を経ることで喫食時に感じる香りの違いは，単純な香気成分の増減という因子だけではなく，組織構造変化という因子からも説明できる可能性が示唆された．乾燥ハーブの香りに対する品質評価を行う上で，乾燥ハーブからハーブティーに抽出されてゆく香気成分のバランス変化や内部組織構造変化の比較といった多面的なアプローチは，今後の有効な評価手法の1つとなることが期待できる．<br />A quality evaluation method for dried herbs was studied with sweet basil leaves (fresh, air-dried, freeze-dried and vacuum-dried sweet basil leaves) as herbal teas, involving hot-water extraction. Sensory evaluation revealed that the flavor of herbal tea with vacuum-dried sweet basil leaves was similar to that with fresh leaves. Seven odor-active compounds (cineole, linalool, eugenol, octanal, 1-octanol, (E)-2-hexenal and (Z)-3-hexenol) from herbal teas were identified by capillary gas chromatographic-mass spectrometry and olfactometry analysis, and it was considered that three compounds (octanal, (E)-2-hexenal and (Z)-3-hexenol) were key compounds for describing the results of sensory evaluation. The structure of dried sweet basil leaves with water-absorption and fresh leaves was observed by differential interference contact microscopy, and their rheological characteristics were measured for storage modulus. As a result, the characteristics of vacuum-dried sweet basil were similar to those of fresh basil. These results suggest that investigation of the aroma using hot-water extraction, tissue structure and rheological characteristics could be effective approaches to qualitatively evaluate dried herbs.
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神山, 和夫 ; 小池, 益人 ; 平尾, 宜司 ; 鳥羽, 陽 ; 早川, 和一 ; Koyama, Kazuo ; Koike, Masuhito ; Hirao, Takashi ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
金沢大学理工研究域自然システム学系<br />製造工程中に起きるデンプンの部分糊化が，レトルトカレーの最終粘度に及ぼす影響を調べた．レトルトカレーの粘度は，煮込みとそれに続くレトルト殺菌工程で，原料中のデンプンが糊化することで上昇する．しか
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し，煮込み工程前の原料混合工程の温度が高過ぎると，最終粘度が十分に上昇しないことが経験的にわかっている．そこで，原料混合工程の温度とデンプンの糊化状態をアミロース溶出度，膨潤度，動的粘弾性および示差走査熱量分析から調べ，最終粘度との関係を考察した．その結果，原料混合工程の温度が65℃以上であると，デンプンの部分糊化が起こるため，その後の煮込み工程と殺菌工程での粘度上昇は抑制されることがわかった．<br />The effect of partial gelatinization of starch during precooking operation on the final viscosity of retort curry at serving temperature was investigated. While the increase in the viscosity of retort curry is largely due to the starch gelatinization during the heating processes of cooking and sterilization, it is known empirically that a high temperature during the material mixing operation before cooking may result in a lower final viscosity. The relationship between the temperature and the partial starch gelatinization during material mixing was therefore studied by measuring amylose leaching, swelling ratio, dynamic viscoelasticity, and by differential scanning calorimetry (DSC). When the mixing temperature was at or higher than 65℃, the starch was partially gelatinized under the low water condition, and as the result, the increase in the viscosity during cooking and sterilization was suppressed. This finding is expected to be useful in controlling the viscosity of starch-containing retort foods.
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鳥羽, 陽 ; 笠原, 千栄子 ; 戸次, 加奈江 ; 佐溝, 将之 ; 唐, 寧 ; 早川, 和一 ; Toriba, Akira ; Kasahara, Chieko ; Bekki, Kanae ; Samizo, Masayuki ; Ning, Tang ; Hayakawa, Kazuichi
概要:
金沢大学理工研究域自然システム学系<br />大気中の粒子状物質（PM）中の水酸化多環芳香族炭化水素（OHPAH）を定量することを目的とするGC/MSによる分析法を開発した．母核の環数が2〜4環のOHPAH 10種を分析対象とし，トリメチル
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シリル（TMS）誘導体化したうえで検出し，3種類の重水素化，または安定同位体標識化OHPAHを内部標準物質として用いてPM試料の定量に適用した．OHPAHのTMS誘導体の選択イオン検出（SIM）における検出限界（S/N＝3）は，12〜930 fgの範囲で，すべての分析対象物質について10.5分で分離・検出することができた．都市大気標準粉じんや金沢で捕集したPM試料はジクロロメタンで抽出したのち，シリカゲル固相により精製しTMS誘導体化して定量した．金沢で捕集したPM試料中の8種のOHPAHを定量することに成功し，それらの濃度範囲は，20〜4100 fg m−3であり，3-hydroxyfluorantheneのPM中濃度の報告は本研究が初めてである．確立した分析法は，大気粉じん中のOHPAHを定量する際の分析法の選択肢の一つとして有用である．<br />A GC/MS method was developed for the quantification of hydroxylated polycyclic aromatic hydrocarbons (OHPAHs) in airborne particulate matter (PM). Ten OHPAHs having 2 - 4 rings were detected after trimethylsilyl (TMS) derivatization, and the derivatives in PM samples were quantified with three kinds of deuterated or stable isotope labeled OHPAHs as internal standards. The detection limits (S/N = 3) of the derivatives of OHPAHs in the selected ion monitoring (SIM) mode ranged from 12 to 930 fg and all analytes were separated and detected within 10.5 min. A commercially available urban PM sample and PM samples collected in Kanazawa were extracted with dichloromethane, and then the extracts were purified with silica gel solid phase and derivatized OHPAHs in the extracts were quantified. We successfully quantified 8 OHPAHs in PM samples collected in Kanazawa, and their concentrations were in the range of 20 - 4100 fg m−3 and the levels of 3-hydroxyfluoranthene were reported for the first time. This method should be useful as an optional analytical method to quantify OHPAHs in PM samples.
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Bekki, Kanae ; Toriba, Akira ; Ning, Tang ; Kameda, Takayuki ; Hayakawa, Kazuichi ; 戸次, 加奈江 ; 鳥羽, 陽 ; 唐, 寧 ; 亀田, 貴之 ; 早川, 和一
概要:
金沢大学理工研究域自然システム学系<br />Polycyclic aromatic hydrocarbons (PAHs) are included in various environmental pollutants such as
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airborne particles and have been reported to induce a variety of toxic effects. On the other hand, PAH derivatives are generated from PAHs both through chemical reaction in the atmosphere and metabolism in the body.PAH derivatives have become known for their specific toxicities such as estrogenic/antiestrogenic activities and oxidative stress, and correlations between the toxicities and structures of PAH derivatives have been shown in recent studies. These studies are indispensable for demonstrating the health effects of PAH derivatives, since they would contribute to the comprehensive toxicity prediction of many kinds of PAH derivatives.<br />多環芳香族炭化水素類（PAHs）は大気粉塵などの多種類の環境汚染物質に含まれ，長年の研究によって多様な生体影響を引き起こすことが知られている．一方で，PAHsは生体内での代謝反応や，大気中での化学反応によって多種多様な誘導体を生成することが知られている．近年では，PAHだけでなくPAH誘導体の毒性影響が着目されており，エストロゲン様/抗エストロゲン作用，酸化ストレス反応など，PAHとは異なる誘導体独自の毒性影響の存在が報告されている．また，生成するPAH誘導体には多くの構造異性体が存在するが，PAH誘導体が示す毒性作用と構造との間に相関性，いわゆる構造活性相関があることが示されている．以上の研究は，環境中に存在するPAH 誘導体の生体影響を解明する上で重要な研究であるとともに，多種多様なPAH誘導体の総合的な毒性影響予測に貢献できると考えられる．
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中澤, 章 ; 唐, 寧 ; 井上, 嘉則 ; 上茶谷, 若 ; 加藤, 敏文 ; 齊藤, 満 ; 小原, 健嗣 ; 鳥羽, 陽 ; 早川, 和一 ; Nakazawa, Akira ; Ning, Tang ; Inoue, Yoshinori ; Kamachitani, Waka ; Katoh, Toshifumi ; Saito, Mitsuru ; Obara, Kenji ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
金沢大学理工研究域自然システム学系<br />著者らが開発した繊維状吸着材（DAM不織布）は，両性イオン型高分子であるジアリルアミン‐マレイン酸共重合体（diallylamine-maleic acid copolymer: DAM）を含有
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し，繊維表面に水和層を形成する．本研究では，悪臭物質の一つである半揮発性有機酸（C1－C5）を対象に水溶液だけでなくガス状でもDAM不織布の吸着特性評価を行った．まず，水溶液中のギ酸はDAM不織布の水和層へ溶解した後，DAMのイミノ基との静電相互作用で吸着することがわかった．一方ガス状では，ギ酸，プロピオン酸，酪酸，吉草酸，イソ吉草酸について高い吸着能を有し，吸着量は曝露時間に依存して増加する傾向があった．ガス状有機酸に対する吸着も水溶液と同様の機序で生じていると考えられるが，さらに酢酸を除く有機酸の吸着速度定数と空気 / 水分配係数（log Kaw）が良好な相関性を有したことから，DAM不織布は大気中から不織布表面に形成される水和層へ移行性が高い親水性化合物に対するほど高い選択性をもつことが示された．<br />Diallylamine-maleic acid copolymer (DAM)-nonwoven fabric (DAM-f), a fibrous adsorbent, contains DAM with zwitter-ionic functional groups and forms a hydration layer on the surface. The aim of this report was to evaluate the adsorption selectivity of DAM-f to semi-volatile organic acid (C1-C5). In the aqueous phase, formic acid dissolved in the hydration layer bound to the imino group of DAM-f due to anion exchange interaction. In the gas phase, the adsorption amounts of organic acids increased with the exposure time. Moreover, the adsorption rate constants correlated with the air/water partition coefficients (log Kaw) for formic acid, propionic acid, butyric acid, valeric acid and isovaleric acid, except for acetic acid. These results indicate that DAM-f is highly selective to hydrophilic compounds which easily move from the air to the hydration layer of DAM-f.
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早川, 和一 ; 加賀谷, 重浩 ; Hayakawa, Kazuichi
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早川, 和一 ; 唐, 寧 ; 鳥羽, 陽 ; 亀田, 貴之 ; Hayakawa, Kazuichi ; Ning, Tang ; Toriba, Akira ; Kameda, Takayuki
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東アジア地域では，急速な産業発展に伴って，環境問題も深刻化している。本稿では，筆者（早川）が拠点リーダーを務め平成14～18 年度にわたって実施した文部科学省21世紀COE プログラム「環日本海域の環境計測と長期・短期変動予測」の研究成果を
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含め，東アジアの有害大気汚染物質としてクローズアップされている多環芳香族炭化水素とニトロ多環芳香族炭化水素に焦点を合わせて，分析化学研究の現状を紹介し，今後の課題について展望する。
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小玉, 修嗣 ; 早川, 和一 ; Kodama, Shuji ; Hayakawa, Kazuichi
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早川, 和一 ; Hayakawa, Kazuichi
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早川 , 和一 ; 能村 , 京子 ; 宮崎 , 元一 ; Hayakawa, Kazuichi ; Nomura, Kyoko ; Miyazaki, Motoichi
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早川, 和一 ; 山本 , 敦 ; 宮崎, 元一 ; Hayakawa, Kazuichi ; Yamamoto, Atsushi ; Miyazaki, Motoichi
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早川, 和一 ; 宮崎, 元一 ; Hayakawa, Kazuichi ; Miyazaki, Motoichi
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Higashi, Tomomi ; Ohkura, Noriyuki ; Fujimura, Masaki ; Nakai, Satoshi ; Honda, Yasushi ; Saijoh, Kiyofumi ; Hayakawa, Kazuichi ; Kobayashi, Fumihisa ; Michigami, Yoshimasa ; Olando, Anyenda Enoch ; Hitomi, Yoshiaki ; Nakamura, Hiroyuki ; 東, 朋美 ; 大倉, 徳幸 ; 藤村, 政樹 ; 西條, 淸史 ; 早川, 和一 ; 小林, 史彦 ; 道上, 義正 ; 人見, 嘉哲 ; 中村, 裕之
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金沢大学医薬保健研究域医学系<br />Asian dust, known as kosa in Japanese, is a major public health concern. In this panel study, we eva
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luated the effects of exposure to kosa on daily cough occurrence. The study subjects were 86 patients being treated for asthma, cough variant asthma, or atopic cough in Kanazawa University Hospital from January 2011 to June 2011. Daily mean concentrations of kosa and spherical particles were obtained from light detection and ranging (LIDAR) measurements, and were categorized from Grade 1 (0 μg/m3) to 5 (over 100 μg/m3). The association between kosa and cough was analyzed by logistic regression with a generalized estimating equation. Kosa effects on cough were seen for all Grades with potential time lag effect. Particularly at Lag 0 (the day of exposure), a dose-response relationship was observed: the odds ratios for Grades 2, 3, 4, and 5 above the referent (Grade 1) were 1.111 (95% confidence interval (CI): 0.995-1.239), 1.171 (95% CI: 1.006-1.363), 1.357 (95% CI: 1.029-1.788), and 1.414 (95% CI: 0.983-2.036), respectively. Among the patients without asthma, the association was higher: the odds ratios for Grades 2, 3, 4 and 5 were 1.223 (95% CI: 0.999-1.497), 1.309 (95% CI: 0.987-1.737), 1.738 (95% CI: 1.029-2.935) and 2.403 (95% CI: 1.158-4.985), respectively. These associations remained after adjusting for the concentration of spherical particles or particulate matter with an aerodynamic diameter of less than 2.5 μm (PM2.5). Our findings demonstrate that kosa is an environmental factor which induces cough in a dose-response relationship. © 2014 Elsevier B.V.<br />Embargo Period 12 months
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| 20.
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Kakimoto, Kensaku ; Toriba, Akira ; Ohno, Takanori ; Ueno, Mariko ; Kameda, Takayuki ; Tang, Ning ; Hayakawa, Kazuichi
概要:
金沢大学医薬保健研究域薬学系<br />To evaluate human exposure to polycyclic aromatic hydrocarbons (PAHs), we developed a rapid, simple
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and sensitive method for determining 1-hydroxypyrene-glucuronide (1-OHP-G) in human urine. To improve precision, a deuterated glucuronide was used as an internal standard. The method requires only 1 mL of urine. The urine was treated with a mixed-mode anion-exchange and reversed-phase solid-phase extraction cartridge (Oasis MAX). The analytes were analyzed with a C18 reversed-phase column with a gradient elution, followed by tandem mass spectrometry with electrospray ionization in negative ion mode. The detection limit of 1-OHP-G (corresponding to a signal-to-noise ratio of 3) was 0.13 fmol/injection. Urinary concentrations of 1-OHP-G determined by this method were strongly correlated (r2 = 0.961) with concentrations of 1-hydroxypyrene by conventional HPLC with fluorescence detection. © 2008 Elsevier B.V. All rights reserved.
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| 21.
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Akutsu, Kazuhiko ; Takatori, S. ; Nozawa, S. ; Yoshiike, M. ; Nakazawa, H. ; Hayakawa, Kazuichi ; Makino, T. ; Iwamoto, T.
概要:
Polybrominated diphenyl ethers (PBDEs) are widely used flame retardants; currently, they are identified as ubiquitous en
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vironmental contaminants. Several studies indicate that PBDEs might affect male fertility. We present the results of a pilot study on the relationship between human serum PBDEs and sperm quality. The PBDE levels in Japan are comparable to those found in European countries. Strong inverse correlations were observed between the serum concentration of 2,2′,4,4′,5,5′-hexabromodiphenyl ether and sperm concentration (r = -0.841, p = 0.002) and testis size (r = -0.764, p = 0.01). Extensive studies on the relationship between PBDEs and sperm quality are required. © 2008 Springer Science+Business Media, LLC.
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| 22.
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Hosozumi, Chiemi ; Toriba, Akira ; Chuesaard, Thanyarat ; Kameda, Takayuki ; Tang, Ning ; Hayakawa, Kazuichi
概要:
Urinary 8-hydroxy-2'-deoxyguanosine (8-OHdG) is a widely used noninvasive biomarker of oxidative stress. A selective, se
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nsitive and rapid method for determining 8-OHdG in human urine was developed using hydrophilic interaction chromatography-tandem mass spectrometry (HILIC-MS/MS) with electrospray ionization. 8-OHdG and isotopically labeled 8-OHdG (internal standard) were separated on a HILIC column with a mobile phase of 10. mM ammonium acetate: acetonitrile (1:9, v/v) within 10. min and detected by using a positive electrospray ionization interface under the selected reaction monitoring mode. The detection limits of 8-OHdG (corresponding to a signal-to-noise ratio of 3) for the HILIC-MS/MS system and the conventional method using a reversed-phase column with MS/MS were 1.0 and 26.0. fmol/injection, respectively. The proposed method makes it possible to monitor the basal level of urinary 8-OHdG from non-exposed healthy subjects and can be used for large-scale human studies. © 2012 Elsevier B.V.
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| 23.
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Tang, Ning ; Tokuda, Takahiro ; Izzaki, Akihiko ; Tamura, Kenji ; Ji, Ruonan ; Zhang, Xuemei ; Dong, Lijun ; Kameda, Takayuki ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Airborne particulates were collected in three size fractions by using Anderson low-volume air samplers in Shenyang, Chin
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a, in winter and summer in 2007. Compared with data obtained in 2001 at the same sites, the total concentrations of nine polycyclic aromatic hydrocarbons (PAHs) in winter decreased by 67% at one site and decreased by 40% at the other site, while the total concentrations of four nitropolycyclic aromatic hydrocarbons (NPAHs) did not decrease. This suggests that environmental countermeasures begun in 2001 were effective in decreasing the concentration of PAHs. However, in summer, the concentrations of PAHs and NPAHs rose by the factors of 4 and 5, respectively, possibly because of an increase in the number of motor vehicles. © 2011 Taylor and Francis Group, LLC.
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| 24.
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Sugitate, Kuniyo ; Yamagami, Takashi ; Nakamura, Sadao ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Fenthion, fenthion sulfoxide, fenthion oxon sulfoxide and fensulfothion showed two different mass spectra in GC/MS, depe
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nding on their concentrations. The base peaks shifted to lower levels by 1 m/z at lower concentration, and no retention time shifts were observed. The "shifted base peaks" were not obtained by a general EI fragmentation. The product ion scan spectra of the "shifted base peaks" were coincident with those of molecular ions of their corresponding sulfides. These phenomena can be ascribed to the conversion of sulfoxide into sulfide by the dominant deoxidation reaction than EI fragmentation in an ion source. Adding polyethylene glycol 300 (PEG300) into a test solution prevented sulfoxide deoxidation. © The Japan Society for Analytical Chemistry.
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| 25.
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Koyama, Kazuo ; Hirao, Takashi ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
The quality of starch-containing foods may be significantly impaired by contamination with very small amounts of α-amyla
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se, which can enzymatically hydrolyze the starch and cause viscosity loss. Thus, for quality control, it is necessary to have an analytical method that can measure low amylase activity. We developed a sensitive analytical method for measuring the activity of α-amylase (from Bacillus subtilis) in starch-containing foods. The method consists of six steps: (1) crude extraction of α-amylase by centrifugation and filtration; (2) α-amylase purification by desalting and anion-exchange chromatography; (3) reaction of the purified amylase with boron-dipyrromethene (BODIPY)-labeled substrate, which releases a fluorescent fragment upon digestion of the substrate, thus avoiding interference from starch derivatives in the sample; (4) stopping the reaction with acetonitrile; (5) reversed-phase solid-phase extraction of the fluorescent substrate to remove contaminating dye and impurities; and (6) separation and measurement of BODIPY fluorescence by HPLC. The proposed method could quantify α-amylase activities as low as 10mU/mL, which is enough to reduce the viscosity of starch-containing foods. © 2012 John Wiley & Sons, Ltd.
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| 26.
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26. Characterization and functionality of immidazolium ionic liquids modified magnetic nanoparticles
Li, Ying ; Tang, Ning ; Inagaki, Fuyuhiko ; Mukai, Chisato ; Hayakawa, Kazuichi
概要:
1,3-Dialkylimidazolium-based ionic liquids were chemically synthesized and bonded on the surface of magnetic nanoparticl
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es (MNPs) with easy one-step reaction. The obtained six kinds of ionic liquid modified MNPs were characterized with transmission electron microscopy, thermogravimetric analysis, magnetization, and FTIR, which owned the high adsorption capacity due to the nanometer size and high-density modification with ionic liquids. Functionality of MNPs with ionic liquids greatly influenced the solubility of the MNPs with organic solvents depending on the alkyl chain length and the anions of the ionic liquids. Moreover, the obtained MNPs showed the specific extraction efficiency to organic pollutant, polycyclic aromatic hydrocarbons, while superparamagnetic property of the MNPs facilitated the convenient separation of MNPs from the bulks water samples. © 2013 Ying Li et al.
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| 27.
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Tang, Ning ; Sato, Kousuke ; Tokuda, Takahiro ; Tatematsu, Michiya ; Hama, Hirotaka ; Suematsu, Chikako ; Kameda, Takayuki ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Airborne particulates were collected at a background site (Wajima Air Monitoring Station; WAMS) on the Noto Peninsula, J
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apan from January 2006 to December 2007. 1-, 2-nitropyrenes (1-, 2-NPs) and 2-nitrofluoranthene (2-NFR), in the particulates were determined with a sensitive HPLC method with chemiluminescence detection. The average concentrations were higher in winter than in summer. A meteorological analysis indicated that the air samples collected in winter were transported mainly from Northeast China over the Japan Sea. Both the concentration ratios of 2-NFR to 1-NP and 1-NP to pyrene were similar to those in Shenyang in Northeast China which located along the air transportation route to WAMS, but not in Kanazawa which near WAMS. These results strongly suggest that most of the atmospheric 1-, 2-NPs and 2-NFR at WAMS in winter were long range transported from Northeast China. © 2014 Elsevier Ltd. All rights reserved.
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| 28.
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Tang, Ning ; Yoda, Yoshiko ; Otani, Naruhito ; Kameda, Takayuki ; Toriba, Akira ; Hayakawa, Kazuichi ; Shima, Masayuki
概要:
Twenty-one data sets composed of readings collected by atmospheric ozone monitors worn by individuals on their clothing
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and installed outside their home or office were collected using Ogawa passive ozone samplers in southeastern Hyogo prefecture, Japan from September 12 to 13, 2011. The concentrations of personal and outdoor ozone ranged from not detectable to 23.2 ppb and from 4.7 to 38.3 ppb, respectively. The mean concentration of personal exposure to ozone was 3.7 ppb and was significantly lower than that of outdoor ozone (18.5 ppb). This suggests that the concentrations of outdoor ozone affect personal ozone exposure. However, in this study, we found no correlation between the concentrations of personal ozone and the total time spent outdoors or the time of day the individual was outside. In contrast, the mean concentrations of outdoor ozone were similar to those of ozone measured at the 12 nearest Ambient Monitoring Stations (AMSs). However, when the AMS was situated near a main road, the regional ozone levels were underestimated.
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| 29.
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Li, Ying ; Yoshida, Shota ; Chondo, Yvonne ; Nassar, Hossam ; Tang, Ning ; Araki, Yuki ; Toriba, Akira ; Kameda, Takayuki ; Hayakawa, Kazuichi
概要:
An on‑line concentration and fluorescence determination HPLC for polycyclic aromatic hydrocarbons (PAHs) in seawater was
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proposed. An online concentration column packed with octadecyl polyvinyl alcohol polymer, a pump and a column switching valve were introduced in the conventional HPLC with a fluorescence detector. Only 1.0–100 mL seawater sample was introduced into the concentration column at 1.0 mL min−1 without any other pretreatment except filtration. Then the trapped PAHs totally flew into the separation column and eluted separately to be detected fluorogenically. The proposed method had good linearity with correlation coefficients (r) ranged from 0.951 to 0.998, and limits of detection ranged from 0.002 to 0.50 ng L−1 for 15 PAHs as 100 mL seawater was loaded. The sensitivity of the method was 10 to 100 times higher than those reported by other works. The proposed method was applied to the determination of PAHs in the seawater samples collected in the Japan Sea with satisfactory results and to check the present benzo[a]pyrene concentration at the beaches in Noto peninsula, Japan polluted with C-heavy oil spilled from the tanker in 1997.
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| 30.
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Tamura, Masayoshi ; Mochizuki, Naoki ; Nagatomi, Yasushi ; Harayama, Koichi ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
A high-resolution liquid chromatography-Orbitrap mass spectrometry (LC-Orbitrap MS) method was developed for simultaneou
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s determination of 20 Fusarium toxins (nivalenol, fusarenon-X, deoxynivalenol, 3-acetyl deoxynivalenol, 15-acetyl deoxynivalenol, HT-2 toxin, T-2 toxin, neosolaniol, diacetoxyscirpenol, fumonisin B1, fumonisin B2, fumonisin B3, fumonisin A1, fumonisin A2, fumonisin A3, zearalenone, α-zearalenol, β-zearalenol, α-zearalanol, and β-zearalanol) in cereals. The separation of 20 Fusarium toxins with good peak shapes was achieved using a pentafluorophenyl column, and Orbitrap MS was able to detect accurately from cereal matrix components within ±0.77 ppm. The samples were prepared using a QuEChERS kit for extraction and a multifunctional cartridge for purification. The linearity, repeatability, and recovery of the method were >0.9964, 0.8%–14.7%, and 71%–106%, respectively. Using this method, an analysis of 34 commercially available cereals detected the presence of deoxynivalenol, 15-acetyl deoxynivalenol, fumonisin B1, fumonisin B2, fumonisin B3, fumonisn A1, fumonisin A2, fumonisin A3, and zearalenone in corn samples with high concentration and frequency. Trichothecenes was detected from wheat samples with high frequency; in particular, the concentration of deoxynivalenol was high. Conversely, α-zearalenol, β-zearalenol, α-zearalanol, and β-zearalanol were not detected in any of the samples. © 2015 by the authors; licensee MDPI, Basel, Switzerland.
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| 31.
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Tamura, Masayoshi ; Mochizuki, Naoki ; Nagatomi, Yasushi ; Harayama, Koichi ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Three compounds, hypothesized as fumonisin A1 (FA1), fumonisin A2 (FA2), and fumonisin A3 (FA3), were detected in a corn
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sample contaminated with mycotoxins by high-resolution liquid chromatography-Orbitrap mass spectrometry (LC-Orbitrap MS). One of them has been identified as FA1 synthesized by the acetylation of fumonisin B1 (FB1), and established a method for its quantification. Herein, we identified the two remaining compounds as FA2 and FA3, which were acetylated fumonisin B2 (FB2) and fumonisin B3 (FB3), respectively. Moreover, we examined a method for the simultaneous analysis of FA1, FA2, FA3, FB1, FB2, and FB 3. The corn samples were prepared by extraction using a QuEChERS kit and purification using a multifunctional cartridge. The linearity, recovery, repeatability, limit of detection, and limit of quantification of the method were >0.99, 82.9%–104.6%, 3.7%–9.5%, 0.02–0.60 μg/kg, and 0.05–1.98 μg/kg, respectively. The simultaneous analysis of the six fumonisins revealed that FA1, FA2, and FA3 were present in all corn samples contaminated with FB1, FB2, and FB 3. The results suggested that corn marketed for consumption can be considered as being contaminated with both the fumonisin B-series and with fumonisin A-series. This report presents the first identification and quantification of FA1, FA2, and FA3 in corn samples. © 2015 by the authors; licensee MDPI, Basel, Switzerland.
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| 32.
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Kakimoto, Hitoshi ; Oka, Hideo ; Harada, Yumiko ; Ushijima, Shigeru ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi
概要:
Dioxins are present as impurities in agrochemicals applied to the soil. To examine the possibility that dioxins end up in the atmosphere, we compare the homologue composition and some characteristic isomer distributions of
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polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) in air and soil samples collected at sites in Ishikawa Prefecture, Japan. Tetrachloro dibenzo-p-dioxin (TeCDD) was the most abundant PCDD homologue in the air samples, while octachloro dibenzo-p-dioxin (OCDD) was the most abundant PCDD homologue in the soil samples. However, at several site, the most predominant homologue in the soil sample was not OCDD but TeCDD. The mean ratio of TeCDDs to PCDDs in the air samples was significantly smaller in winter than in other seasons, but no such seasonal variation was observed in the distribution of PCDF homologues. The abundance of PCDF homologues was inversely related to the number of chlorine substitutions in the air samples. The contribution of each toxic isomer (2,3,7,8-chlorine-substituted) to the total toxicity equivalency quantity (TEQ) in the air samples tended to be intermediate between their contributions to the TEQs in the soil and cinder samples. This result suggested that the air samples were influenced by both soil/dust suspension and combustion. In order to clarify the contributions of agrochemicals to dioxins in the air, we focused on the ratios of several characteristic isomers that are indicators of agrochemicals (chloronitrophen: CNP and pentachlorophenol: PCP) to their homologues. Significant decreases in the ratios of the isomers to their homologues in the air samples were observed only in winter, probably as a result of suppression of dust suspension by the snow cover. Therefore, the contribution of combustion to the dioxin concentration in the air was thought to be relatively large in winter.
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| 33.
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Miyazaki, Motoichi ; Okubo, Noboru ; Hayakawa, Kazuichi ; Umeda, Toshihiko
概要:
A flow-injection analysis system is described for the determination of halide (chloride, bromide and iodide) anions. Thi
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s method could be used as a post column detection method for these anions in water samples. The system is based on the specific and selective reaction between halide anion and fluorescein with an oxidant in an acidic flow. The product is detected at 530 nm in an alkaline flow. The detection limits of the three anions under the conditions tentatively established for the determination of bromide anion were as follows ; Cl-, 1×10-8mol ; Br-, 1×10-10mol ; I-, 1×10-10mol.
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| 34.
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Tang, Ning ; Hakamata, Mariko ; Sato, Kousuke ; Okada, Yumi ; Yang, Xiaoyang ; Tatematsu, Michiya ; Toriba, Akira ; Kameda, Takayuki ; Hayakawa, Kazuichi
概要:
Total suspended particulates were collected at a Japanese remote background site (Noto Air Monitoring Station; NAMS) on
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the Noto Peninsula from September 2004 to June 2014. Nine polycyclic aromatic hydrocarbons (PAHs) in the particulates (fluoranthene, pyrene, benz[a]anthracene, chrysene, benzo[b]fluoranthene, benzo[k]fluoranthene, benzo[a]pyrene, benzo[ghi]perylene and indeno[1,2,3-cd]pyrene) were determined by HPLC with fluorescence detection. The mean total concentrations of the nine PAHs in the cold season (November to May for the years 2004-2014) was 670 pg m-3 (range 37-4100 pg m-3). The mean total concentration in the warm season (June to October for the same period) was 170 pg m-3 (range 31-960 pg m-3). The atmospheric PAH level at NAMS decreased in recent years, although no significant change was found in the warm season. An analysis of meteorological conditions showed that the atmospheric PAHs at NAMS were long range transported from Northeast China in the cold seasons and were contributed to by Japanese domestic sources in the warm seasons. Lower concentration ratios of reactive PAHs to their isomers at NAMS also supported these results. Activities associated with the Beijing Olympic and Paralympic Games in 2008 and reconstruction after the 2007 Noto Hanto earthquake may have contributed to the yearly variations of atmospheric PAH levels at NAMS during the period 2007-2009. Source control measures implemented by the Chinese and Japanese governments appear to have been effective in decreasing the atmospheric PAH levels at NAMS in recent years. © 2015 Elsevier Ltd.<br />Embargo Period 24 months
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| 35.
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Tang, Ning ; Tabata, Masahiro ; Mishukov, Vasiliy F. ; Sergineko, Valentine ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi
概要:
Airborne particulates were collected simultaneously at Vladivostok, Kanazawa and Toyama. 1,3-, 1,6-, 1,8-Dinitropyrenes (DNPs), 1-, 2-, 4-nitropyrenes (NPs), 2-nitrofluorene and 6-nitrochrysene in the particulates were analyzed by HPLC
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with chemiluminescence detection. All compounds were detected not only in Kanazawa but also in Vladivostok and Toyama. Moreover, five unknown peaks which might be nitropolycyclic aromatic hydrocarbons were detected only in chromatograms of Vladivostok. The [DNPs]/[1-NP] ratios at all stations were near the value found in diesel-exhaust particulates, suggesting that one of the main contributors of these compounds was diesel-engine vehicles not only in Kanazawa and Toyama but also in Vladivostok. However, the difference in traffic volume at two stations in Vladivostok did not have a significant effect on the concentrations of DNPs and NPs in contrast to two stations in Kanazawa. These results suggested sources other than diesel-engine vehicles also contributing to DNPs and NPs in Vladivostok. Seasonal variations similar to those in Kanazawa were observed in Vladivostok and Toyama. As in Kanazawa, the [2-NP]/[1-NP] ratio in Vladivostok was larger at the lighter traffic station than that at heavier traffic station. This suggested that, as in Kanazawa, 2-NP was formed in the atmosphere in Vladivostok.
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| 36.
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Hayakawa, Kazuichi ; Nakamura, Akio ; Terai, Noriko ; Kizu, Ryoichi ; Ando, Kyoko
概要:
Diesel exhaust particulates were extracted with benzene-ethanol (3 : 1, v/v) and separated into five fractions by silica-gel column chromatography. Direct-acting mutagenic activity was assayed by the Ames test using the Salmonella typhimurium
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YG1024 strain. The total activity of five fractions was about four times greater than that of the crude extract, suggesting that the activities in the fractions were suppressed in the crude extract. Strong activity was observed in fraction 4 which was eluted with dichloromethane (61.5% of the total activity) and fraction 5 which was eluted with ethanol (35.3%). Nitropolycyclic aromatic hydrocarbons (NPAHs) were determined by high-performance liquid chromatography with chemiluminescence detection. They were found mainly in fraction 4, although one NPAH was in fraction 3 which was eluted with n-hexane-dichloromethane (3 : 1, v/v). Based on these results, 53.1% of the activity in fraction 4 was attributed to NPAHs. The contribution of 1-nitropyrene and 1, 3-, 1, 6- and 1, 8-dinitropyrenes was great and that of the other NPAHs was small. The mutagenic compound in fraction 5 was not identified. Fractions 1 and 2, which were eluted with n-hexane, and fraction 3 suppressed the activity of fraction 4. Polycyclic aromatic hydrocarbons in fractions 2 and 3 were considered as possible suppressors of NPAHs.
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| 37.
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Hayakawa, Kazuichi ; Imanari, Toshio ; Tamura, Zenzo ; Kuroda, Shigetoshi ; Ikeda, Hisao ; Tateishi, Jun
概要:
Beagle dogs were orally administered with a fixed dose of clioquinol, 300 mg/kg/day, in gelatin capsules every day. Other beagle dogs were orally administered with powder clioquinol, 300 mg/kg/day after increasing dose, in
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milk twice a day. All beagle dogs administered with clioquinol developed weakness of the hind-limbs and hip swaying in several ten days. Individual differences and daily variations in serum levels of clioquinol, its sulfate and its glucuronide were large. Clioquinol was detected at higher concentrations not only in central nervous system but also in peripheral nervous system, and was retained for a long time.
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| 38.
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Imanari, Toshio ; Ishida, Yuko ; Hayakawa, Kazuichi ; Miyazaki, Motoichi
概要:
Superoxide dismutase (SOD)-like activity was found in rabbit plasma and the active substance was separated. Its properties were similar to those of copper-zinc SOD in cyanide and azide sensitivity and heat-stability, but its
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molecular weight was presumed to be 140000 by Sephadex G-150 column.
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| 39.
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Hayakawa, Kazuichi ; Nomura, Kyoko ; Miyazaki, Motoichi
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| 40.
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Morisaki, Hiroshi ; Nakamura, Shiho ; Tang, Ning ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Benzo[c]fluorene (BcFE) concentrations in benzene/ethanol extracts of airborne particulates were determined by high-perf
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ormance liquid chromatography (HPLC) with fluorescence detection. HPLC conditions were as follows: columns, two ZORBAX Eclipse PAH (4.6 i.d. × 250 mm, 3.5 μm) and one Inertsil ODS-P (4.6 i.d. × 250 mm, 5 μm) in series; mobile phase, acetonitrile–water (98:2, v/v), 0.3 mL/min; detection wavelengths, excitation 309 nm, emission 354 nm. Particulate-phase BcFE concentrations in the atmosphere varied seasonally (winter > summer). The concentrations were 11000 ± 6100 pg m−3 (winter) and 40 ± 12 pg m−3 (summer) in Beijing, China, and 13 ± 5.0 pg m−3 (winter) and 2.7 ± 0.52 pg m−3 (summer), in Kanazawa, Japan. In both cities, the particulate-phase BcFE concentration in the atmosphere was lower than that of benzo[a]pyrene (BaP) by a factor of 0.03 – 0.43. However, the mutagenic contribution of particulate-phase BcFE in the atmosphere in winter calculated from the mutagenicity relative potency factor was greater than that of BaP.
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| 41.
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Hayakawa, Kazuichi ; Kobayashi, Jun ; Ohmori, Mikako ; Ohya, Mayumi ; Kato, Akio ; Miyazaki, Motoichi
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| 42.
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Murahashi, Tsuyoshi ; Miyazaki, Motoichi ; Kakizawa, Ryuichi ; Yamagishi, Yoshihisa ; Kitamura, Moritsugu ; Hayakawa, Kazuichi
概要:
Direct-acting mutagenic 1, 3-dinitropyrene (1, 3-DNP), 1, 6-DNP, 1, 8-DNP and 1-nitropyrene (1-NP) and indirect-acting mutagenic benzo [a] pyrene (BaP) in airborne particulates collected by the side of a busy intersection in downtown
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Kanazawa were determined by high-performance liquid chromatography (HPLC) with chemiluminescence and fluorescence detection. Time courses of their concentrations were high in the morning (8 : 00-10 : 00) and evening (16 : 00-20 : 00) and low from the midnight until early morning (0 : 00-6 : 00). Levels of each DNP (in the range of fmol/m3) and 1-NP (in the range of sub pmol/m3) were, respectively, more than three and about one order of magnitude lower than that of BaP. Large correlation coefficients (0.85-0.91) between their concentrations, traffic volume, and carbon monoxide and nitrogen monoxide concentrations suggested that the main source was vehicles. Utilizing the concentration ratios, ([1, 3-DNP]+[1, 6-DNP]+[1, 8-DNP])/[1-NP], in airborne particulates (0.014), gasoline particulates (0.56) and diesel particulates (0.013), contributions (%) of dieselengine vehicles to the three DNPs and 1-NP in the air were estimated to be 94.3% and 99.8%, respectively.
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| 43.
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Nishimura, Masayuki ; Hayashi, Morimasa ; Hayakawa, Kazuichi ; Miyazaki, Motoichi
概要:
The selective effect of triethylenetetramine (Trien) on the retention behavior of sulfate in ion chromatography was stud
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ied. When Trien was added to an eluant as a counter ion, retention of sulfate was selectively shortened, while retention times of monovalent anions did not change. The cause for this phenomenon was the complexation of sulfate and Trien in an eluant. The stability constants of divalent sulfate-trivalent Trien and -tetravalent Trien complexes were estimated to be 936 and 4213 (40°C), respectively. As a practical application of this phenomenon, weakly retained monovalent species can be very well separated from both water dip and other species without prolonging the interval of injections.
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| 44.
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論文
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Hayakawa, Kazuichi ; Butoh, Mizuka ; Hirabayashi, Yukiko ; Miyazaki, Motoichi
概要:
1, 3-, 1, 6-, 1, 8-Dinitropyrenes (DNPs) and 1-nitropyrene (1-NP) in exhaust particulates from idling gasoline and diesel engines were determined using off-line sodium hydrosulfide reduction followed by HPLC with chemiluminescence
…
detection. The mean concentrations of 1, 3-, 1, 6-, 1, 8-DNPs and 1-NP were 0.22, 0.44, 0.35 and 1.8 pmol/mg, respectively, in gasoline particulates (n=8) and 0.23, 0.23, 0.21 and 51 pmol/mg, respectively, in diesel particulates (n=7). Although the concentrations of DNPs were lower than that of 1-NP in both gasoline and diesel particulates, they cannot be dismissed as negligible because of their extremely high mutagenicity. There was a tendency toward higher DNPs and 1-NP concentrations in particulates, with the lowering of particulate concentration in exhaust gas. The total amount of DNPs and 1-NP emitted from diesel engine vehicles was considered to be remarkably higher than that of gasoline engine vehicles.
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| 45.
論文 |
論文
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Hayakawa, Kazuichi ; Miyazaki, Motoichi
概要:
A HPLC method with peroxyoxalate-chemiluminescence (CL) detection has been developed for the determination of dinitropyrenes (DNPs) and nitropyrene (NP). Both DNPs and NP, which are CL-insensitive, were initially reduced to the
…
corresponding amino-derivatives with sodium hydrosulfide. They were separated on a reversed-phase column and chemilumigenically determined with detection limits in the subfmol range. Utilizing this method, DNPs and NP were determined in gasoline and diesel particulate samples.
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| 46.
論文 |
論文
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Yamamoto, Atsushi ; Hayakawa, Kazuichi ; Matsunaga, Akinobu ; Mizukami, Eiichi ; Miyazaki, Motoichi
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| 47.
論文 |
論文
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Hayakawa, Kazuichi ; Nakamura, Seiji ; Inaki, Kotoe ; Miyazaki, Motoichi
概要:
Carboxylesters, carboxylic and inorganic anions were determined separately by photometric ion chromatography with an enz
…
yme immobilized column. In the system, a carboxylesterase immobilized column (4.6mm i.d.×10mm), which converted carboxylesters to carboxylic anions completely, was set between a sample injector and an analytical column. The other chromatographic conditions were as follows: an anion exchanger-type separation column (4.6mm i.d.×250mm); phthalate-N-2-hydroxyethylpiperazine-N′-2-ethanesulfonic acid e uent (pH 6.5); an oven of temperature 40°C; a flow rate of 1.0ml/min; 280-nm UV detection; and an injection volume of 20μl. Calibration curves for ethyl esters of acetate, propionate, butyrate and isova erate were linear with the range 5×10-10mol to 1×10-7mol according to the peak-height method; their detection limits were 10-10 mol levels. The present method was applied for the determination of carboxylesters in practical samples.
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| 48.
論文 |
論文
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Yamamoto, Atsushi ; Matsunaga, Akinobu ; Mizukami, Eiichi ; Hayakawa, Kazuichi ; Miyazaki, Motoichi
概要:
A simultaneous determination method for five organic acids in vinegar has been established by photometric ion chromatogr
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aphy. Both trace components (lactic, gluconic, succinic and pyroglutamic acids) and the major component (acetic acid) in vinegar were separated on a TSK gel IC-Anion-PW column with 0.45 mM o-aminobenzenesulfonic acid aqueous solution as an eluent. Their elutions were detected as positive peaks before the system peak, and a negative peak after that by a UV monitor. The sensitivities of trace components were enhanced by adjusting their elutions close to the system peak. The lowest detection limits were 10μM lactic acid, 5μM gluconic and succinic acids and 3μM pyroglutamic acid, respectively. The only pretreatment necessary was dilution of vinegar 100-fold with the eluent. The results obtained by the proposed method were in good agreement with those by the enzymatic one.
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| 49.
論文 |
論文
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Nishimura, Masayuki ; Hayashi, Morimasa ; Yamamoto, Atsushi ; Hayakawa, Kazuichi ; Miyazaki, Motoichi
概要:
The effect of a mobile phase polyvalent counter ion on the retention behavior and peak intensity of sulfate in non- suppressed ion chromatography was quantitatively studied using a chromatogram simulation method. In this study,
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both indirect photometric detection (IPD) method and conductometric detection (CD) method were evaluated. With the IPD method, the retention of sulfate was observed to decrease in the presence of the polyvalent counter ion (Trien) without any change in peak intensity. With the CD method, however, peak intensity of sulfate decreased and, under some conditions, gave a negative peak in simulation as was also observed in actual experiments. The present work demonstrates the possibility of predicting the effect of a polyvalent counter ion on sulfate retention without resorting to physical experiments.
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| 50.
論文 |
論文
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Utsumi, Akiko ; Nakashima, Atsuko ; Ando, Kyoko ; Kizu, Ryoichi ; Hayakawa, Kazuichi
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| 51.
論文 |
論文
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Hayakawa, Kazuichi ; Kitamura, Ryuichi ; Butoh, Mizuka ; Imaizumi, Noriko ; Miyazaki, Motoichi
概要:
A high performance liquid chromatographic (HPLC) method with chemiluminescence (CL) detection was developed for the sens
…
itive determination of 1, 3-diaminopyrene (1, 3-DAP), 1, 6-DAP, 1, 8-DAP and 1-aminopyrene (1-AP). The HPLC conditions were as follows: column, Cosmosil 5C18 (4.6mm i.d.×250mm); mobile phase, 10mM imidazole- perchloric acid buffer(pH 7.6)-acetonitrile (1:1, v/v); CL reagent, 0.02mM bis(2, 4, 6-trichlorophenyl)oxalate (TCPO) and 15mM hydrogen peroxide in acetonitrile. The oxidative degradation of DAPS and AP in the presence of metals was prevented by adding ascorbic acid to sample solutions. The calibration curves were straight over 2 orders of magnitude for all analytes, and their detection limits (as S/N was 3) were in the sub-fmol range. Dinitro- and nitropyrenes in sooty emissions of diesel- and gasoline-engine cars could be determined by this HPLC after reductive conversion into DAPs and AP, respectively, by refluxing the samples in the presence of sodium hydrosulfide.
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| 52.
論文 |
論文
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Hayakawa, Kazuichi ; Nomura, Kyoko ; Miyazaki, Motoichi
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| 53.
論文 |
論文
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Yamamoto, Atsushi ; Matsunaga, Akinobu ; Hayakawa, Kazuichi ; Mizukami, Eiichi ; Miyazaki, Motoichi
概要:
A photometric detector for an optically active compound is described in which two polarizers are set on both sides of the flow cell. When a nonchromophoric, optically active compound passes through the cell, the intensity of natural
…
light transmitted through the polarizers and flow cell is changed. The detection of such a sample is possible photometrically. A large inclination angle between the polarizers increases the absorbance change and allows dextrorotatory and levorotatory to be differentiated. The direct HPLC/photometric detection of sugars is presented as an axample of this device.
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| 54.
論文 |
論文
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Kizu, Ryoichi ; Ikeda, Tomoko ; Hayakawa, Kazuichi ; Miyazaki, Motoichi
概要:
Metal-catalyzed hydrolyses of clioquinol-glucuronide (CG) and clioquinol-sulfate (CS) in the rabbit body were studied following intravenous injection of Cu (II)- or Fe (III)-gluconic acid complex system 6h after the oral administration of
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clioquinol (C). Molar fractions of C, CG and CS remained nearly constant through 24 h after administration of C at doses of 90-300mg/kg weight in rabbits which were not injected with Cu (II) or Fe (III). Therefore, molar fractions of C, CG and CS after the injection of Cu (II) or Fe (III) were monitored to clarify the metabolic changes of C. In rabbits injected with 2.5mg of Cu (II)/kg weight, C rapidly increased and CG and CS decreased after the injection of Cu (II). In rabbits injected with 20 mg of Fe (III)/kg weight, C and CS slowly increased and CG decreased until 18h after the injection of Fe (III). The patterns of the changes in molar fractions of C, CG and CS are consistent with the catalytic features of Cu (II) and Fe (III) seen in previous studies, and therefore, the changes in molar fractions of C, CG and CS observed in this study were considered to have been brought about as a result of metalcatalyzed hydrolyses of CG and CS or metal-catalyzed hydrolysis of CG in the rabbit body.
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| 55.
論文 |
論文
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Hayakawa, Kazuichi ; Chen, Chingtan ; Imanari, Toshio ; Tamura, Zenzo
概要:
Glucuronide (CF-G) and sulfate (CF-S) of 5-chloro-7-iodo-8-quinolinol were hydrolyzed in water in the presence of metal ions at pH 7. In this condition, CF-G was hydrolyzed more easily than CF-S. The rate of the hydrolysis,
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pseudo-first order reaction, was in parallel with the stability constants of 8-quinolinol-metal complexes. The rate of hydrolysis increased with reduction of concentration of H+ and tris buffer suppressed the hydrolysis of CF-G. These results suggest that metal catalyzed hydrolysis of CF-G and CF-S was derived from the formation of complexes between the conjugates and metal ions.
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| 56.
論文 |
論文
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Yamada, Maromu ; Nakamura, Kaya ; Kameda, Takayuki ; Kobayashi, Fumihisa ; Matsuki, Atsushi ; Tsuiki, Hisanaga ; Higaki, Seigo ; Iwasaka, Yasunobu ; Hayakawa, Kazuichi
概要:
Polycyclic aromatic hydrocarbons (PAHs) are known as carcinogenic and/or mutagenic substances, and are present at high c
…
oncentration in polluted environments. It has recently been reported that spore-forming bacteria (e.g., Bacillus spp.) can be transported long distances alive in the atmosphere, which raises the possibility that some of the transported bacteria could have adverse effects on human health. There is thus a need for filters that can remove gaseous PAHs from the air that people breathe and that can inhibit bacterial growth on the filters. We focused on metallophthalocyanine derivatives (M-Pc) which are known to adsorb PAHs as well as to inhibit the growth of bacteria as a potential filtering agent. In this study, we developed different types of M-Pc-supported rayon fibers by changing central metals, functional groups, concentrations of M-Pc and rayon types, and evaluated their removal effects by measuring adsorption rates of 3- and 4-ring PAHs with a HPLC and growth curves of Bacillus sp. with a spectrophotometer. The results showed that both the effects depended on functional groups and concentrations of M-Pc, and rayon types. The most effective combination was observed in Fe-Pc with sulfo group supported on cationized rayon fiber at the concentration of 2 to 3.3 wt%. Central metal species of M-Pc were influenced only on the antibacterial properties. This fiber would be applicable to filtering agents and textiles.
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| 57.
論文 |
論文
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Chen, Chingtan ; Hayakawa, Kazuichi ; Imanari, Toshio ; Tamura, Zenzo
概要:
An analytical method of 5-chloro-7-iodo-8-quinolinol (Clioquinol or Chinoform) (CF) conjugates was established by high p
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erformance liquid chromatography. The chromatographic conditions were as follows : column, SAX (50 cm×2 mm i.d.) ; mobile phase, I (0.02M borate buffer-0.1M KCl, pH9.5), II (0.02M borate buffer-0.5M NaClO4, pH 9.5) ; gradient, 0→25% (II/I+II) at 3%/min ; column pressure, 500 psi ; flow rate, 1 ml/min ; detector, ultraviolet-detector at 254 mμ. Urine samples of a man administered CF were injected directly to the column, and the major metabolite, CF glucuronide was determined, while very small amounts of CF sulfate was detected.
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| 58.
論文 |
論文
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Hayakawa, Kazuichi ; Ogai, Toshihiko ; Irikura, Yoshiaki ; Miyazaki, Motoichi ; Tamura, Zenzo
概要:
Changes in the distributions and chemical forms of biological metals, copper, iron, zinc, calcium and magnesium, produced by the administration of clioquinol in rabbits were investigated. Single administration caused a decrease in plasma
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zinc and excretion into urine of a large amount of iron (this may have originated from iron-binding proteins such as hemoglobin). Multiple administrations increased plasma copper, which was mainly bound to ceruloplasmin. Decrease in copper in the kidney, increase in copper in the cerebrum and increase in zinc in both the kidney and liver were also observed after multiple administrations.
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| 59.
論文 |
論文
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Imaizumi, Noriko ; Hayakawa, Kazuichi ; Okubo, Noboru ; Miyazaki, Motoichi
概要:
A selective, sensitive and accurate determination of sulfite was proposed by high performance liquid chromatography (HPL
…
C). The sulfite was converted quantitatively to an adduct by reacting with a triphenylmethane dye, malachite green (MG). The formation of adduct was complete, and the adduct was stable at the experimental conditions. Then, the adduct was submitted to HPLC. The working curve for sulfite was linear in the range from 2.0×10-12 mol upto 1.2×10-9 mol.
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| 60.
論文 |
論文
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Hayakawa, Kazuichi ; Kato, Akio ; Yamamoto, Atsushi ; Miyazaki, Motoichi
概要:
In non-suppressed conductometric ion chromatography, when a carboxylic acid eluent of low pH is used, the signal intensi
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ty (ΔHc) is proportional to the sum of the conductivity change caused by changes in the sample concentration (ΔCs) as well as conductivity changes caused by changes in the eluent concentration (ΔCe). This can be expressed as ΔHC=B(ΔCs)+B(ΔCe), where B is a constant. In this equation, ΔCs is constant for any sample species. However, ΔCe varies with changes in the sample capacity factors. This value is positive when the sample elutes before the system peak (k′s<k′e), and is negative when it elutes after the system peak (k′s>k′e). Therefore, the sample peak intensity (ΔHC) is enhanced prior to the system peak and is suppressed after it. These effects increase the closer the sample and the system peaks. The effect of this theory was proved by a determination of orthophosphate using a TSK gel IC-Anion-PW column and a 0.75mM phthalic acid eluent. The detection limit of this method for orthophosphate (1×10-11mol, with an S/N of three) was smaller (by a factor of 10-30) than those by previous conventional ion chromatographic methods. Also, the interference of chloride or nitrate, often observed in the previous methods, was removed by suppressing their peak intensities. When this method was applied for the determination of orthophosphate in environmental samples, other interfering compounds were effectively removed by a column-switching system attached to the ion chromatograph, and a trace level of the orthophosphate was determined.
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| 61.
論文 |
論文
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Hayakawa, Kazuichi ; Imanari, Toshio ; Asazuma, Shuko ; Kizu, Ryoichi ; Miyazaki, Motoichi
概要:
An effective method for fractional analysis of zinc in rabbit plasma was established, using polyethylene glycol. Rabbit plasma zinc was separated into two fractions ; the zinc profile in the precipitate showed two peaks, which were
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not albumin-bound zinc, on gel filtration, while the zinc in the supernatant proved to be albumin-bound zinc. The proposed method was used to investigate the effect of feeding on plasma zinc in rabbits. The decrease of total plasma zinc on feeding was significant, and was mainly due to that of albumin-bound zinc.
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| 62.
論文 |
論文
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Murahashi, Tsuyoshi ; Kizu, Ryoichi ; Kakimoto, Hitoshi ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Diesel-engine exhaust and airborne particulates were collected in downtown and suburban areas and five mutagenic nitroarenes (2-nitrofluoranthene (NF), 1-, 2- and 4-nitropyrenes (NPs) and 6-nitrochrysene (NC) in benzene-ethanol extracts
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were determined by high-performance liquid chromatography with chemiluminescence detection. 1- and 4-NPs and 6-NC were found in diesel-engine exhaust particulates, however, 2-NF and 2-NP were not detected. On the other hand, all five nitroarenes were found in airborne particulates. Diurnal concentration patterns of 4-NP and 6-NC in the downtown area were similar to the pattern of 1-NP, but the patterns of 2-NF and 2-NP were different from the pattern of 1-NP. These results strongly suggested that 2-NF and 2-NP are formed in the atmosphere. Of the five nitroarenes, 2-NF had the largest suburban / downtown concentration ratio. 2- and 4-NPs and 6-NC all showed larger ratios than did 1-NP. These results showed that 2-NF and 2-NP were formed in the atmosphere, but that the secondary formation of 4-NP and 6-NC were not known. Taking mutagenic activity and the atmospheric concentration into consideration, the mutagenic contribution of 2-NF was estimated to be comparable with that of 1-NP in the downtown area, and more than that of 1-NP in the suburban area. This result suggested that the mutagenic contribution of the minor nitroarenes formed in urban air might not be negligible.
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| 63.
論文 |
論文
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Hayakawa, Kazuichi ; Bekki, Kanae ; Yoshita, Morio ; Tachikawa, Chihiro ; Kameda, Takayuki ; Tang, Ning ; Toriba, Akira ; Hosoi, Shinzo
概要:
Estrogenic and antiestrogenic activities of 19 quinoid polycyclic aromatic hydrocarbons (PAHQs) and 9 ketone PAHs were e
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valuated by the yeast two-hybrid assay using yeast cells expressing estrogen receptor-α (ERα). Binding affinity of PAHQs to ERα was assayed by the polarized fluorescence method using FluormoneTM ES2. Ten PAHQs having 3-5 rings showed antiestrogenic activities. The most strongly antiestrogenic PAHQs were 1,4-chrysenequinone and 5,6-chrysenequinone. On the other hand, benzo[a]pyrene-3,6-quinone showed the strongest estrogenic activity. However, the other compounds tested did not show so strong estrogenic/antiestrogenic activities. Binding affinity to ER was required but not sufficient for estrogenic/antiestrogenic activities of PAHQs. The length-to-breadth ratios of the rectangular planes surrounding the ring molecules and the distances between the oxygen atom of the carbonyl group and farthest hydrogen atom of estrogenic/antiestrogenic PAHQs were in narrow ranges, suggesting a structure-activity relationship. As interactions between active PAHQ and ER, hydrogen bonding between carbonyl groups and amino acid residues and van der Waals forces were considered.
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| 64.
論文 |
論文
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Hayakawa, Kazuichi
概要:
Airborne particulate matter (PM) has been collected at four cities in Japan starting in the late 1990s, at five or more
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major cities in China, Korea and Russia starting in 2001 and at the Noto Peninsula starting in 2004. Nine polycyclic aromatic hydrocarbons (PAHs) and eleven nitropolycyclic aromatic hydrocarbons (NPAHs) were determined by HPLC with fluorescence and chemiluminescence detections, respectively. Annual concentrations of PAHs and NPAHs were in the order, China>Russia≫Korea=Japan, with seasonal change (winter>summer). During the observation period, concentrations of PAHs and NPAHs in Japanese cities significantly decreased but the increases in the PAH concentration were observed in Chinese and Russian cities. Concentrations of PAHs and NPAHs were higher in the Northern China than those in the Southern China. At the Noto peninsula, which is in the main path of winter northwest winds and a year-round jet stream that blow from the Asian continent to Japan, the concentrations were high in winter and low in summer every year. A cluster analysis and back trajectory analysis indicated that PAHs and NPAHs were long-range transported from Northeastern China, where coal burning systems such as coal-heating boilers are considered to be the major contributors of PAHs and NPAHs. A dramatic change in atmospheric concentrations of PAHs and NPAHs in East Asia suggests the rapid and large change of PM2.5 pollution in East Asia. Considering the adverse health effects of PM2.5, continuous monitoring of atmospheric PAHs and NPAHs is necessary in this area.
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| 65.
論文 |
論文
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Hayakawa, Kazuichi ; Wakatsuki, Misuzu ; Yamada, Eiko ; Shimizu, Kyoko ; Kizu, Ryoichi ; Miyazaki, Motoichi
概要:
Metals-catalyzed hydrolysis of clioquinol (C) conjugates, namely C-glucuronide (CG) and C-sulfate (CS), was examined to investigate the effects of pH and ligands on the activities. The initial rates of hydrolysis (Vo) of CG and CS
…
were measured as a function of pH in systems containing various metals. The profiles of Vo of CG varied from metal to metal, but the order of Vo in the acidic pH region was Cu (II) > Fe (III) > Ni (II) > Zn (II) > Mn (II), Mg (II), Ca (II). Acid hydrolysis of CG in the absence of metals was negligible down to pH 1. The profiles of Vo of CS were similar to that of acid hydrolysis in the absence of metals, except for the Cu (II) system, which gave a higher Vo. Under the condition [substrate] : [Cu (II)] : [ligand]=1 : 10 : 10, the hydrolysis in the presence of various ligands was a pseudo-first order reaction (rate constant=k'). All ligands which coordinate to Cu (II) reduced the value of k'. Such metals-catalyzed hydrolysis may be one of the mechanism of hydrolysis of C conjugates to produce C-metal chelates in vivo.
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| 66.
論文 |
論文
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Kameda, Takayuki ; Akiyama, Ayuko ; Yoshita, Morio ; Tachikawa, Chihiro ; Toriba, Akira ; Tang, Ning ; Hayakawa, Kazuichi
概要:
The mutagenicities and endocrine-disrupting activities of two isomers of mononitrated 1-hydroxypyrene [1-hydroxy-x-nitro
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pyrenes (1-OH-x-NPs); x = 2 and 5], which are not only photoreaction products of 1-nitropyrene (1-NP) but also constituent of ambient airborne particles, were evaluated for the first time using the Ames plate incorporation assay and the yeast two-hybrid assay, respectively. The mutagenicity of 1-OH-5-NP was weakly positive in the absence of rat liver S9, but was enhanced up to 3-fold with the metabolic activation by S9. On the contrary, 1-OH-2-NPdid not exhibit significant mutagenicity in the presence or absence of S9. 1-OH-5-NP showed weak estrogenic activity, but 1-OH-2-NP did not show any estrogenic activity. The concentration of 1-OH-5-NP that gave 10% of activity of 1.0 × 10-6M 17ß- estradiol (E2) was 5.4 × 10-7M. 1-OH-5-NP exhibited stronger antiestrogenic and antiandrogenic activities than 1-OH-2-NP. 1-OH-5-NP at a concentration of 1.0 × 10-6M inhibited 71 and 90%of ß-galactosidase activity induced by 1.0 × 10-9Mof E2 and 1.0 × 10-8M of 5a-dihydrotestosterone (DHT), respectively. On the other hand, 1.0 × 10-6M of 1-OH-2-NP inhibited 16 and 43% of ß-galactosidase activity induced by 1.0 × 10-9M of E2 and 1.0 × 10-8M of DHT, respectively. These findings point out the need for determining the environmental sources and distribution of 1-OH-2-NP and 1-OH-5-NP as well as the other hydroxynitropyrene isomers. © 2011 The Pharmaceutical Society of Japan.
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| 67.
論文 |
論文
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Araki, Yuki ; Tang, Ning ; Ohno, Michihiro ; Kameda, Takayuki ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
We developed a sampler for collecting atmospheric polycyclic aromatic hydrocarbons (PAHs) and nitropolycyclic aromatic hydrocarbons (NPAHs) by attaching a glass column packed with XAD-4 resin to the gas sampling port of a
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high-volume air sampler equipped with a filter. When the upper and bottom layers of the column were packed with 64 g and 32 g of XAD-4 resin, respectively, all PAHs and NPAHs in the gas phase were quantitatively collected in the XAD-4 resin column without any break through, while PAHs and NPAHs in the particle phase were collected on the filter. We collected air samples at suburban and downtown Kanazawa by using the proposed sampler. It was found that about 95% of 2-3 ring PAHs and more than 99% of 2-ring NPAHs existed chiefly in the gas phase, that 4-ring PAHs such as fluoranthene (FR) and pyrene (Pyr) and 3-ring NPAHs were in both the gas and particle phases and that the other PAHs and NPAHs having 4-rings or more except for FR and Pyr were almost completely in the particle phase. Our data also indicated that the adsorption of NPAHs to the particle phase in the atmosphere is controlled by the same mechanism as that of PAHs.
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| 68.
論文 |
論文
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Toriba, Akira ; Hayakawa, Kazuichi
概要:
Polycyclic aromatic hydrocarbons (PAHs) and itropolycyclic aromatic hydrocarbons (NPAHs) are widespread carcinogenic compounds that arise from occupational, environmental and dietary sources. The metabolites of PAHs and NPAHs in
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biological fluids have been investigated as potential biomarkers for assessing human exposure to them, and, particularly, urinary metabolites are the excellent candidates due to the non-invasiveness and convenience of collecting the sample. Here we describe HPLC methods for accurately determining one type of these metabolites, monohydroxy PAHs (OHPAHs). The developed method was applied to the urine samples of non-smoker taxi drivers, traffic police officers and rural villagers of Chiang Mai, Thailand. The results showed higher urinary concentrations of OHPAHs in rural villagers, suggesting the higher respiratory exposure to PAHs contained in smoke from biomass burning. On the other hand, 1-nitropyrene (1-NP) is one of the most abundant NPAHs in diesel exhaust particulate matter (DEP). We also developed a liquid chromatography-tandem mass spectrometry (LC-MS/MS) method for determining urinary 1-NP metabolites. 1-NP metabolites were quantified in urine from healthy subjects. 6- and 8-Hydroxy-N-acetyl-1-aminopyrenes (OHNAAPs) and 6- and 8-hydroxy-1-nitropyrenes (OHNPs) were the most abundant 1-NP metabolites in human urine. The presence of OHNAAPs and OHNPs in human urine was demonstrated for the first time.
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| 69.
論文 |
論文
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Oka, Hideo ; Kakimoto, Hitoshi ; Miyata, Yoshiaki ; Yonezawa, Yumiko ; Niikawa, Akiko ; Kyudoh, Hirohisa ; Tang, Ning ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi
概要:
Air samples were collected at suburban Kanazawa and concentrations of dioxins in both gaseous and particulate phases were determined separately. The concentrations of the gaseous phase of dioxins increased with increasing
…
temperature. Co-planar polychlorinated biphenyls (co-PCBs), whose vapor pressures are higher than those of polychlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs), were mainly in the gaseous phase samples in all the seasons. The gaseous phase ratios [gaseous phase/(gaseous phase + particulate phase)] of tetrachloro dibenzop-dioxins and dibenzofurans (TeCDD/DFs) were high regardless of the temperature. However, the gaseous phase ratios of penta-hepta CDD/DFs varied widely depending on the temperature. Gas/particle partitioning of atmospheric dioxins depended on not only the number of chlorine-substitutions but also the positions of the chlorine-substitutions. The position of chlorine-substitution in an isomer affects the isomer's molecular polarity. Dioxin isomers with higher molecular polarity, which have shorter retention times on the selected ion monitoring (SIM) chromatograms of their homologues, tended to be distributed unevenly in the gaseous phase. In addition, the differences in the gaseous phase ratios between the isomers with higher molecular polarity and those with lower molecular polarity increased with decreasing temperature.
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| 70.
論文 |
論文
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Hirose, Toshiharu ; Morito, Keiko ; Kizu, Ryoichi ; Toriba, Akira ; Hayakawa, Kazuichi ; Ogawa, Sumito ; Inoue, Satoshi ; Muramatsu, Masami ; Masamune, Yukito
概要:
Benzo[a]pyrene (BaP), a major environmental pollutant, is metabolized in vivo and produces many hydroxy derivatives. The
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estrogenic/antiestrogenic activities of twelve monohydroxy derivatives of BaP (1- through 12-OH species) were investigated using competition binding to human estrogen receptor (hER)α and hERβ, and the gene expression assay of the yeast two-hybrid system. BaP and 5-OH BaP did not bind to either hER. The other monohydroxy derivatives bound to both hERs. These compounds bound more strongly to hERβ than to hERα. Using the yeast two-hybrid assay system, 1-, 2-, 3-, and 9-OH BaP induced β-galactosidase with hERβ but not with hERα. This suggested that these compounds were estrogenic. In the presence of 10-9 M 17 β-estradiol, 8-OH BaP inhibited the induction of β-galactosidase. Because 8-OH BaP did not affect cell growth, it appeared to be an antiestrogen. The present study shows that most of the monohydroxy derivatives of BaP bind to estrogen receptors (ERs), and several of them have estrogenic or antiestrogenic activity.
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| 71.
論文 |
論文
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Hayakawa, Kazuichi
概要:
The East Asia countries including Japan, China, Korea and Russia have been undergoing a rapid increase of economic and i
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ndustrial development. However, large amounts of pollutants are released into the air and water. The main energy source, economic stage and lifestale are different in the above four countries and these differences cause the current diverse situation of atmospheric and water pollution in East Asia. This view describes the present stage of atmospheric pollution and countermeasures in East Asia including the author's recent research results concerning polycyclic aromatic hydrocarbons and nitropolycyclic aromatic hydrocarbons. ©2009 The Pharmaceutical Society of Japan.
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| 72.
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Tozuka, Yoshiko ; Watanabe, Nobue ; Osawa, Masanobu ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi
概要:
Polycyclic aromatic hydrocarbons (PAHs) were analyzed in maternal blood and fetuses from Fischer 344 rats exposed to diesel exhaust (DE) during pregnancy, and in breast milk from rats exposed to DE during pregnancy and lactation using
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high performance liquid chromatography with fluorescence detection. Concentrations of phenanthrene (Phe), anthracene (Ant) and benz[a]anthracene (BaA) were significantly higher in maternal blood of the DE group than those of the control group. Concentration of Phe in fetuses of the DE group was significantly higher than those of the control group. Concentrations of fluorene, Ant, fluoranthene (Flu), pyrene (Pyr), BaA and chrysene (Chr) tended to be higher in fetuses of the DE group. The levels of Ant, Flu, Pyr and Chr in breast milk from the DE group were significantly higher than those of the control group. These results indicate that PAHs taken into mother rat by the inhalation of DE are transferred into fetuses via placenta and into breast milk. This is the first report to clarify the transportation of inhaled PAHs into fetuses and breast milk from mother rats.
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| 73.
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Motoyama, Yumi ; Bekki, Kanae ; Chung, Sang Woon ; Tang, Ning ; Kameda, Takayuki ; Toriba, Akira ; Taguchi, Keiko ; Hayakawa, Kazuichi
概要:
The effect of four ortho-quinoid polycyclic aromatic hydrocarbons (PAHs) and seven para-quinoid PAHs on the viability of
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A549 cells were examined. The ortho-quinoid PAHs [1,2-naphthoquinone (1,2-NQ), 9,10-phenanthrenquinone (9,10-PQ), 5,6-chrysenequinone (5,6-CQ), and benzo[c]phenanthrene-5,6-quinone (B[c]P-5,6-Q)] overproduced hydrogen peroxide (H2O2) without being consumed themselves. These ortho-quinoid had strong cytotoxic effects except for 1,2-NQ, since of its tendency to covalently bind to thiol groups. The cytotoxicity appears to be due to the overproduction of H 2O2 by ortho-quinoid PAHs in a redox cycle coupled with the consumption of thiol group. In contrast, the para-quinoid PAHs were not as strong cytotoxic and did not produce H2O2. ©2009 The Pharmaceutical Society of Japan.
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| 74.
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Honoki, Hideharu ; Tsushima, Katsutoshi ; Hayakawa, Kazuichi
概要:
The ion constituents contained in fresh snow immediately after snowfall were examined at 5-10 km intervals over 50 km from the coast of Hakui city in Ishikawa Prefecture leeward of the northwestern seasonal wind to the plain in
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Toyama city in Toyama Prefecture. The concentrations of sodium ions and sea-salt-sulfate ions that originated from the Sea of Japan decreased exponentially from Hakui city in Ishikawa Prefecture to Toyama city. The concentration of non sea-salt sulfate ions, which probably originate from human activities, also decreased exponentially, but it was lower than the concentration of sea-salt sulfate ions until 25 km from Hakui city and higher in the farther regions. We considered that this was due to additive effects of non sea-salt sulfate ions transported from a distance and local sulfate ions. The concentration of non sea-salt sulfate ions transported from the Asian Continent was estimated in each sampling station. Its contribution was 0.98 of the total at the coast of Hakui city and 0.65 at Toyama city, respectively, and showed a pattern similar to those of sodium ions and sea-salt sulfate ions. The concentrations of ammonium ions and non sea-salt calcium ions were slightly higher in the plain in Toyama than on the coast of Hakui city, suggesting that they mostly originated from the sampling regions in this study. The concentration of nitrate ions was almost constant in the regions from the coast to the inland areas, suggesting also that they mostly originated from the sampling regions.
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| 75.
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Bekki, Kanae ; Takigami, Hidetaka ; Suzuki, Go ; Tang, Ning ; Hayakawa, Kazuichi
概要:
金沢大学医薬保健研究域薬学系<br />金沢大学自然科学研究科<br />Several polycyclic aromatic hydrocarbons and nitrated polycyclic aromatic hydrocarb
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ons (PAHs/NPAHs) such as benzo[a]pyrene and 1-nitropyrene are mutagens and/or carcinogens. These compounds secondarily generate PAH hydroxides, ketones, and quinones through atmospheric and metabolic reactions. The health effects of these compounds is now an important social concern. For example, lung cancer, bronchitis, whistling and so on. In this work, we evaluated toxicities of 25 PAH derivatives (hydroxides, ketones and quinones) in terms of aryl hydrocarbon receptor (AhR) binding and thyroid hormone-related endpoints using three in vitro bioassays: dioxinresponsive chemical-activated luciferase gene expression (DR-CALUX), thyroid receptor β chemical-activated luciferase gene expression (TRβ-CALUX), and competitive human transthyretin-binding (TTR-binding) assays. Eleven of the 25 PAH derivatives had AhR agonist activity, six had AhR antagonist activity and seven had TRpotentiation activity in the TR-CALUX. Furthermore, PAH quinones and hydroxides had strong TTR-binding activity. 3,4-Dihydrobenz[a]anthracen-1(2 H)-one had the strongest agonist activity (EC20: 0.4μM) as determined by DR-CALUX. PAH ketones showed stronger activity than the control and significant difference by statistical analysis. Benzo[c]phenanthrene-[1,4]-quinone was the most TTR-active compound (IC50: 2.5μM). Both PAH ketones and quinones, which have functional groups with low polarity, had significant activities in all tested assays. These in vitro results suggest that PAH derivatives might have various toxic activities in animals. For estimating the health effects and accessing the environmental risks of PAHs, further studies on the toxicity mechanisms are necessary. ©2009 The Pharmaceutical Society of Japan.
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| 76.
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Ohno, Takanori ; Toriba, Akira ; Kameda, Takayuki ; Tang, Ning ; Hayakawa, Kazuichi
概要:
金沢大学医薬保健研究域薬学系<br />To measure the actual exposure of a person to 1-nitropyrene (1-NP) in airborne particulate matter, i
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t is considered more accurate to collect air samples with a portable air sampler than to sample at a fixed location. However, because the portable samplers can sample only small volumes, a sensitive method is needed to analyze the compounds that are collected on a filter. Here we describe a high-performance liquid chromatographic (HPLC) method with fluorescence detection that is sensitive and precise enough for use with portable air samplers. The developed column-switching system successfully removed the interfering substances in the samples with only a simple pretreatment. To improve the precision of the measurement, deuterated 1-NP was used as an internal standard, and it eluted immediately prior to 1-NP with sufficient resolution (Rs, 1.50). The detection limit was 0.32 fmol/injection, and the calibration range was from 2 to 100 fmol. The proposed method was applied to determining 1-NP in fine airborne particulate matter (PM2.5) at two sites with low pollution levels. 1-NP was detected in all samples at concentrations in the low fmol/m3 range. The proposed method has enough sensitivity and precision to determine 1-NP in the limited air volume of the portable sampler. © 2009 Elsevier B.V. All rights reserved.
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| 77.
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Maeda, Osamu ; Oikawa, Chie ; Shiomi, Nobuo ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
金沢大学医薬保健学域薬学類 金沢大大学自然科学研究科 ㈱ハウス食品分析テクノサービス<br />Titanium dioxide was used as a photocatalyst to decompose interfering su
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bstances for a quantitative analysis of a fungicide (iprodione) in dry basil by HPLC. A quartz vial containing basil extract and titanium dioxide was irradiated with black light. The interfering substances were almost completely decomposed by 180 min of irradiation, whereas 88.3% of iprodione remained. The recovery of iprodione was 102.6% by the proposed method in basil extracts. This may have been due to different decomposition rates of the analyte and interfering substances. 2008 © The Japan Society for Analytical Chemistry.
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| 78.
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Tanaka, Hiroki ; Sugita-Kounishi, Yuka ; Takino, Masahiko ; Tanaka, Toshitsugu ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
金沢大学医薬保健研究域薬学系<br />By adopting a rapid and sensitive method for simultaneous detection of nivalenol (NIV), deoxynivalen
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ol (DON), fusarenon-X (FX), 3-acetyl deoxinivalenol (3ADON), HT-2 toxin (HT-2), T-2 toxin (T-2) and zearalenone (ZEN), the natural occurrence of these mycotoxins in biscuits made of wheat (201 samples) in Japan was surveyed. Samples were analyzed by LC/MS with atmospheric pressure photo ionization (APPI). Further confirmation was performed by liquid chromatography/time of flight mass spectrometry (LC/TOFMS). The average contamination of each Fusarium mycotoxin was 3.1, 23, 0.7, 0.1 and 4.2 ng/g for NIV, DON, HT-2, T-2 and ZEN, respectively. Multiple toxins were observed in 120 samples while FX and 3ADON were not detected. The incidence of these toxins was 41% for NIV, 98% for DON, 19% for HT-2, 11% for T-2 and 2% for ZEN. There were no significant differences in the concentration and incidence between conventional biscuits made of wheat and biscuits made of wheat for infants. This is the first report concerning the presence of NIV, DON, HT-2, T-2 and ZEN in biscuits in Japan. © 2010 The Pharmaceutical Society of Japan.
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| 79.
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Hayakawa, Kazuichi ; Miyazaki, Motoichi
概要:
A HPLC method with peroxyoxalate-chemiluminescence (CL) detection has been developed for the determination of dinitropyr
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enes (DNPs) and nitropyrene (NP). Both DNPs and NP, which are CL-insensitive, were initially reduced to the corresponding amino-derivatives with sodium hydrosulfide. They were separated on a reversed-phase column and chemilumigenically determined with detection limits in the subfmol range. Utilizing this method, DNPs and NP were determined in gasoline and diesel particulate samples. © 1991, The Japan Society for Analytical Chemistry. All rights reserved.
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| 80.
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Chinaka, Satoshi ; Iio, Reiko ; Takayama, Nariaki ; Kodama, Shuji ; Hayakawa, Kazuichi
概要:
Amphetamine-type stimulants (ATS), having one or more asymmetric carbons, are important targets in forensic science field. For chiral analysis, capillary electrophoresis (CE) has advantages over other chromatographic methods,
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especially, in fastness, resolution, cost performance and simplicity. This review summarizes chiral separation techniques of ATS using CE with UV detection or CE/mass spectrometry mainly by the present authors' research group.
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| 81.
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論文
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Kameda, Takayuki ; Akiyama, Ayuko ; Toriba, Akira ; Tachikawa, Chihiro ; Yoshita, Morio ; Tang, Ning ; Hayakawa, Kazuichi
概要:
Endocrine disrupting activities of three isomers of monohydroxylated 1-nitropyrene (1-NP) [3-, 6-, and 8-hydroxy-1-nitro
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pyrenes (OHNPs)] were evaluated for the first time by yeast two-hybrid assay. OHNPs, which are not only metabolites of 1-NP but are also found in airborne particles, did not exhibit androgenic activity but exhibited estrogenic, antiestrogenic, and antiandrogenic activities. 6-OHNP showed the strongest estrogenic activity among the three OHNP isomers examined in this study. Concentrations of the OHNP isomers that gave 10% of activity of 1.0 × 10-6 M 17β-estradiol (E2) were as follows: 3-OHNP, 6.0 × 10 -7 M; 6-OHNP, 6.0 × 10-8 M; 8-OHNP, 9.0 × 10-7 M. On the contrary, 8-OHNP exhibited the strongest antiestrogenic and antiandrogenic activities of the three isomers. 1.0 × 10-6 M of 8-OHNP inhibited 32 and 90% of β-galactosidase activity induced by 1.0 × 10-9 M of E2 and 1.0 × 10-8 M of 5α-dihydrotestosterone (DHT), respectively. These findings point out the necessity for detailed investigation of environmental sources and distributions of OHNPs as well as the parent 1-NP.
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| 82.
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Hayakawa, Kazuichi ; Onoda, Yu ; Tachikawa, Chihiro ; Hosoi, Shinzo ; Yoshita, Morio ; Chung, Sang Woon ; Kizu, Ryoichi ; Toriba, Akira ; Kameda, Takayuki ; Tang, Ning
概要:
Estrogenic/antiestrogenic activities of 14 polycyclic aromatic hydrocarbons (PAHs) and 63 monohydroxylated PAHs (OHPAHs)
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having 2 to 6 rings were evaluated by yeast two-hybrid assay expressing human estrogen receptor α. Relative effective potencies of estrogenic and antiestrogenic activities were calculated as the inverse values of the relative concentration of the test compound that gave the same activities of E2 and 4-hydroxytamoxifen, respectively. PAHs did not show any estrogenic/antiestrogenic activity, but several OHPAHs having 3 to 5 rings showed activities. Especially, OHPAHs having 4 rings such as 3-, 4- and 10-hydroxybenz[a]anthracenes (3-, 4- and 10-OHBaAs) and 2-hydroxychrysene (2-OHCh) showed strongly estrogenic activity. Several other OHPAHs having 4 rings such as 2- and 3-hydroxybenzo[c]phenanthrenes (2-, 3- OHBcPhs), 2-OHBaA and 3-OHCh showed strongly antiestrogenic activity. The length-to-breadth (L/B) ratios of the rectangular van der Walls planes surrounding the ring molecules of estrogenic OHPAHs were in the narrow range from 1.599 to 1.734. The distances between the oxygen atom of the phenol group and farthest hydrogen atom (O-H distance) of the estrogenic OHPAHs ranged from 10.825 A° to 11.738 A°. The L/B ratios and O-H distances of antiestrogenic OHPAHs were in the wider ranges from 1.277 to 1.734 and from 8.47 A° to 11.681 A°, respectively. The partial charges (atomic unit) of the phenol group of both estrogenic and antiestrogenic OHPAHs were in the range from 0.250 atmic unit (au) to 0.253 au. The similarity of these values to those of E2 and diethylstilbestrol suggested that the compositions of estrogenic OHPAHs were similar to them and that the compositional conditions of estrogenic OHPAHs were much smaller than those of antiestrogenic OHPAHs. These results raise the possibility of predicting the estrogenic/antiestrogenic activities of OHPAHs from their structural characteristics, although using only the above three parameters might not be enough for accurate estimations.
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| 83.
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論文
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Kizu, Ryoichi ; Otsuki, Naoki ; Kishida, Yoshiko ; Toriba, Akira ; Mizokami, Atsushi ; Burnstein, Kerry L. ; Klinge, Carolyn M. ; Hayakawa, Kazuichi
概要:
We developed a new mammalian cell-based luciferase reporter gene assay for androgenic and antiandrogenic activities of c
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hemicals and environmental samples. Environmental samples usually have a complex matrix that may contain the constituents acting as androgen receptor (AR) agonists, AR antagonists or aryl hydrocarbon receptor (AhR) agonists. AhR agonists are known to elicit the antiandrogenic effect through cross-talk between AR and AhR signal transduction pathways. In this study, PC3/AR human prostate carcinoma cells were transiently transfected with a prostate-specific antigen (PSA) promoter-driven luciferase expression plasmid. The cells were treated with a test compound or an environmental sample for 24 h at 37°C and then measured for luciferase activity. The luciferase activity was induced by dihydrotestosterone (DHT) in a concentration-dependent manner in a concentration range from 10 fM to I nM. R1881, a synthetic androgen receptor agonist, induced luciferase activity and its inductive effects was additive to that of DHT. The luciferase activity was not induced by cortisol, a glucocorticoid, progesterone, a progestin, and 17β-estradiol, an estrogen in a concentration range of up to 1 μM. DHT-induced luciferase activity was reduced by bicalutamide and cyproterone acetate, AR antagonists, and also by benzo[a]pyrene, an aryl hydrocarbon receptor agonist, through AhR-mediated pathways. All of these findings indicate that the present assay system correctly responds to AR agonists, AR antagonists and AhR agonist and, therefore, it is a powerful tool for the sensitive and selective screening of chemicals and environmental samples for their androgenic and antiandrogenic activities. We developed the first assay system, in which the expression of luciferase was driven by the promoter of a prostate-specific antigen gene, a typical human androgen-regulated gene.
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| 84.
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論文
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Tang, Ning ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi
概要:
An automatic HPLC system for analyzing nitropolycyclic aromatic hydrocarbons (NPAHs, nitroarenes) in airborne particulates was previously described (Anal. Chim. Acta, 2001, 445, 20). Some problems with this system were that it
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generated a peak originating from an ascorbic acid solution that elutes at a retention time close to that of 1,6-dinitropyrene (DNP), and that it was able to analyze only 1,3-, 1,6-, 1,8-DNPs and 1-nitropyrene (1-NP). Here, we describe an improved system that effectively removes the interfering peak by introducing an ODS column just after the pump for the ascorbic acid solution, and which is capable of analyzing several additional compounds (2-, 4-NPs, 2-nitrofluorene, 6-nitrochrysene, 7-nitrobenz[a]anthracene, 3-nitroperylene and 6-nitrobenzo[a]pyrene etc.). The improved sensitivities were achieved by concentrating the compounds in a benzene-ethanol extract from airborne particulates, by increasing the loading time of the sample solution from 20 to 38 min, and by increasing the flow rate of an ascorbic acid solution from 1.3 to 1.8 mL/min.
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| 85.
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論文
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Tang, Ning ; Taga, Rina ; Hattori, Tetsuyuki ; Tamura, Kenji ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi
概要:
A method using high-performance liquid chromatography with chemiluminescence detection was developed for analyzing mutagenic nitrobenzanthrone (NBA) isomers in airborne particulates. The method was a modification of our previously
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described method for analyzing nitropolycyclic aromatic hydrocarbons (NPAHs). The pretreatment and reducing conditions for 1-, 2-, 3- and 10-NBAs were the same as those for NPAHs. In order to separate these NBA isomers, we used a polymeric-type ODS column (Cosmosil 5C-18MS); a mixture of 40% acetonitrile and 60% 10 mM imidazole-HClO4 buffer was employed as the mobile phase at a flow rate of 1 mL/min. The isomers of 1-, 2-, 3- and 10-NBA were determined in chemiluminescence with linear calibration graphs from 0.1 to 4 pmol, from 200 to 4000 pmol, from 1 to 50 pmol and from 10 to 400 pmol, respectively. The detection limits (S/N = 3) of 1-, 2-, 3- and 10-NBA isomers were 0.02 pmol, 35 pmol, 0.3 pmol and 3 pmol, respectively. The method was used to analyze airborne particulates at a heavy traffic site in Kanazawa. 2- and 3-NBAs were detected in the extracts of the particulates, while 1-NBA and 10-NBA were not detected. The atmospheric concentrations of 2- and 3-NBAs were 1.83 pmol/m3 and 24.7 fmol/m3, respectively.
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| 86.
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論文
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Sasaki, Hideki ; Yonekubo, Jun ; Hayakawa, Kazuichi
概要:
Current on-line solid-phase extraction methods combined with HPLC for shortening the clean-up operation are not suitable
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for simultaneously detecting compounds that have a wide variety of hydrophobicities. To solve these problems, we designed a new on-line sample preparation system. The system consists of an eluting pump, a mixing TEE connector, a 10-port 2-position valve and a solid-phase extraction precolumn. The eluate from the precolumn is diluted with a weak solvent from the HPLC at the TEE connection to load low hydrophobic compounds onto the analytical column. The proposed on-line sample preparation system was successfully applied to the simultaneous analysis of 21 pesticides in river water using LC/TOF-MS. In this method, the recoveries from river water samples were 67 to 126% (mean 83%), the reproducibility (CV%) was in the range from 1.1 to 11% (mean 5.6%), the calibration curve was linear in the range from 1 ppb to 500 ppb (r > 0.999) and the detection limits (S/N = 3) were in the range from 0.0034 ppb (daimuron) to 3.3 ppb (oxine-copper). 2006 © The Japan Society for Analytical Chemistry.
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| 87.
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論文
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Yamamoto, Atsushi ; Kawai, Mio ; Sakamoto, Mitsunori ; Kodama, Shuji ; Hayakawa, Kazuichi
概要:
A sensitive and variable-wavelength optical rotatory (OR) detector for high-performance liquid chromatography is present
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ed. This design is entirely different from that of conventional OR detectors consisting of a crossed polarizer pair. By placing a polarizing prism and a retardation plate into a commercial circular dichroism (CD) detector, the OR signal was obtained. The Mueller matrix approach was used to prove the principle of the OR signal appearance. Sugars and 4-androstene-3,17-dione were chosen as test compounds. The limit of detection was below 0.5 μg of injected sucrose at 260 nm, which was superior to that obtained with a conventional OR detector. For 4-androstene-3,17-dione, which is CD active, and shows a large anomalous OR dispersion curve, our detector gave a large OR signal with approximately half the intensity of the CD signal at 340 nm. 2008 © The Japan Society for Analytical Chemistry.
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| 88.
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論文
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Higashi, Tomomi ; Kambayashi, Yasuhiro ; Ohkura, Noriyuki ; Fujimura, Masaki ; Nakanishi, Sayaka ; Yoshizaki, Tomokazu ; Saijoh, Kiyofumi ; Hayakawa, Kazuichi ; Kobayashi, Fumihisa ; Michigami, Yoshimasa ; Hitomi, Yoshiaki ; Nakamura, Hiroyuki
概要:
The health effects associated with Asian dust have attracted attention due to the rapid increase in the number of Asian
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dust events in East Asia in recent years. The aim of this study was to investigate the associations between Asian dust and daily cough, as well as allergic symptoms, in adult patients who suffer from chronic cough. We enrolled 86 adult patients from Kanazawa University Hospital, Japan, who were diagnosed with asthma, cough variant asthma, atopic cough or a combination of these conditions. From January to June 2011, subjects recorded their symptoms in a diary every day. Asian dust and non-Asian dust periods were defined according to the dust extinction coefficient, measured using the light detection and ranging (LIDAR). The daily levels of total suspended particulates, polycyclic aromatic hydrocarbons (PAHs) and coexisting factors related to allergies, such as the Japanese cedar pollen count, were measured. McNemar's test showed that there were significantly more cough-positive patients during Asian dust periods than during the non-Asian dust period (p = 0.022). In addition, during Asian dust periods when the daily levels of Japanese cedar pollen, Japanese cypress pollen and PAHs were elevated, there were significantly more patients who experienced itchy eyes than during the non-Asian dust period (p < 0.05). On the other hand, there were no significant differences in the allergic symptoms, including sneezing or a runny nose and nasal congestion. This is the first report to show that Asian dust triggers cough and allergic symptoms in adult patients with chronic cough. © 2014 Elsevier Ltd. All rights reserved.
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| 89.
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論文
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Higashi, Tomomi ; Kambayashi, Yasuhiro ; Ohkura, Noriyuki ; Fujimura, Masaki ; Nakai, Satoshi ; Honda, Yasushi ; Saijoh, Kiyofumi ; Hayakawa, Kazuichi ; Kobayashi, Fumihisa ; Michigami, Yoshimasa ; Olando, Anyenda Enoch ; Hitomi, Yoshiaki ; Nakamura, Hiroyuki
概要:
Asian dust, known as kosa in Japanese, is a major public health concern. In this panel study, we evaluated the effects o
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f exposure to kosa on daily cough occurrence. The study subjects were 86 patients being treated for asthma, cough variant asthma, or atopic cough in Kanazawa University Hospital from January 2011 to June 2011. Daily mean concentrations of kosa and spherical particles were obtained from light detection and ranging (LIDAR) measurements, and were categorized from Grade 1 (0μg/m3) to 5 (over 100μg/m3). The association between kosa and cough was analyzed by logistic regression with a generalized estimating equation. Kosa effects on cough were seen for all Grades with potential time lag effect. Particularly at Lag 0 (the day of exposure), a dose-response relationship was observed: the odds ratios for Grades 2, 3, 4, and 5 above the referent (Grade 1) were 1.111 (95% confidence interval (CI): 0.995-1.239), 1.171 (95% CI: 1.006-1.363), 1.357 (95% CI: 1.029-1.788), and 1.414 (95% CI: 0.983-2.036), respectively. Among the patients without asthma, the association was higher: the odds ratios for Grades 2, 3, 4 and 5 were 1.223 (95% CI: 0.999-1.497), 1.309 (95% CI: 0.987-1.737), 1.738 (95% CI: 1.029-2.935) and 2.403 (95% CI: 1.158-4.985), respectively. These associations remained after adjusting for the concentration of spherical particles or particulate matter with an aerodynamic diameter of less than 2.5μm (PM2.5). Our findings demonstrate that kosa is an environmental factor which induces cough in a dose-response relationship. © 2014 Elsevier Ltd.
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| 90.
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論文
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Suzuki, Nobuo ; Danks, Janine A. ; Maruyama, Yusuke ; Ikegame, Mika ; Sasayama, Yuichi ; Hattori, Atsuhiko ; Nakamura, Masahisa ; Tabata, Makoto J. ; Yamamoto, Toshio ; Furuya, Ryo ; Saijoh, Kiyofumi ; Mishima, Hiroyuki ; Srivastav, Ajai K. ; Furusawa, Yukihiro ; Kondo, Takashi ; Tabuchi, Yoshiaki ; Takasaki, Ichiro ; Chowdhury, Vishwajit S. ; Hayakawa, Kazuichi ; Martin, T. John
概要:
金沢大学環日本海域環境研究センター<br />The effect of fugu parathyroid hormone 1 (fugu PTH1) on osteoblasts and osteoclasts in teleosts w
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as examined with an assay system using teleost scale and the following markers: alkaline phosphatase (ALP) for osteoblasts and tartrate-resistant acid phosphatase (TRAP) for osteoclasts. Synthetic fugu PTH1 (1-34) (100 pg/ml-10 ng/ml) significantly increased ALP activity at 6 h of incubation. High-dose (10 ng/ml) fugu PTH1 significantly increased ALP activity even after 18 h of incubation. In the case of TRAP activity, fugu PTH1 did not change at 6 h of incubation, but fugu PTH1 (100 pg/ml-10 ng/ml) significantly increased TRAP activity at 18 h. Similar results were obtained for human PTH (1-34), but there was an even greater response with fugu PTH1 than with human PTH. In vitro, we demonstrated that both the receptor activator of the NF-κB ligand in osteoblasts and the receptor activator NF-κB mRNA expression in osteoclasts increased significantly by fugu PTH1 treatment. In an in vivo experiment, fugu PTH1 induced hypercalcemia resulted from the increase of both osteoblastic and osteoclastic activities in the scale as well as the decrease of scale calcium contents after fugu PTH1 injection. In addition, an in vitro experiment with intramuscular autotransplanted scale indicated that the ratio of multinucleated osteoclasts/mononucleated osteoclasts in PTH-treated scales was significantly higher than that in the control scales. Thus, we concluded that PTH acts on osteoblasts and osteoclasts in the scales and regulates calcium metabolism in goldfish. © 2011 Elsevier Inc. All rights reserved.
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| 91.
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論文
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Yachiguchi, Koji ; Matsumoto, Noriko ; Haga, Yuki ; Suzuki, Motoharu ; Matsumura, Chisato ; Tsurukawa, Masahiro ; Okuno, Toshihiro ; Nakano, Takeshi ; Kawabe, Kimi ; Kitamura, Kei-ichiro ; Toriba, Akira ; Hayakawa, Kazuichi ; Chowdhury, Vishwajit S. ; Endo, Masato ; Chiba, Atsuhiko ; Sekiguchi, Toshio ; Nakano, Masaki ; Tabuchi, Yoshiaki ; Kondo, Takashi ; Wada, Shigehito ; Mishima, Hiroyuki ; Hattori, Atsuhiko ; Suzuki, Nobuo
概要:
To analyze the effect of polychlorinated biphenyl (PCB) 118 on fish bone metabolism, we examined osteoclastic and osteob
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lastic activities, as well as plasma calcium levels, in the scales of PCB (118)-injected goldfish. In addition, effect of PCB (118) on osteoclasts and osteoblasts was investigated in vitro. Immature goldfish, in which the endogenous effects of sex steroids are negligible, were used. PCB (118) was solubilized in dimethyl sulfoxide at a concentration of 10 ppm. At 1 and 2 days after PCB (118) injection (100 ng/g body weight), both osteoclastic and osteoblastic activities, and plasma calcium levels were measured. In an in vitro study, then, both osteoclastic and osteoblastic activities as well as each marker mRNA expression were examined. At 2 days, scale osteoclastic activity in PCB (118)-injected goldfish increased significantly, while osteoblastic activity did not change significantly. Corresponding to osteoclastic activity, plasma calcium levels increased significantly at 2 days after PCB (118) administration. Osteoclastic activation also occurred in the marker enzyme activities and mRNA expressions in vitro. Thus, we conclude that PCB (118) disrupts bone metabolism in goldfish both in vivo and in vitro experiments. © 2012 The Author(s).
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| 92.
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Suzuki, Nobuo ; Sekiguchi, Toshio ; Satake, Honoo ; Kato, Kanoko ; Nishiyama, Yudai ; Takahashi, Hideya ; Dankse, Janine A. ; Martin, T. John ; Hattori, Atsuhiko ; Nakano, Masaki ; Kakikawa, Makiko ; Yamada, Sotoshi ; Ogoshi, Maho ; Hyodo, Susumu ; Yamaguchi, Yoko ; Chowdhur, Vishwajit S. ; Hayakawa, Kazuichi ; Funahashi, Hisayuki ; Sakamoto, Tatsuya ; Sasayama, Yuichi
概要:
In cartilaginous fish, two cDNAs encoding calcitonin-family receptors were isolated for the first time from the stingray
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brain. The open reading frame of one receptor cDNA coded a 525-amino acid protein. The amino acid identity of this receptor to human calcitonin-receptor-like receptor (CRLR) is 64.5%, frog CRLR is 64.7%, and flounder CRLR is 61.2% and this was higher than to human calcitonin receptor (CTR) (46.1%), frog CTR (54.7%), and flounder CTR (48.9%). We strongly suggested that this receptor is a ray CRLR based on phylogenetic analysis. In case of the second receptor, amino acid identity among CRLRs (human 50.5%, frog 50.7%, flounder 48.0%) and CTRs (human 43.2%, frog 49.1%, flounder 41.8%) was similar. From phylogenetic analysis of both CRLRs and CTRs, we believe that this receptor is ray CTR. The expression of ray CRLR mRNA was predominantly detected in the nervous system (brain) and vascular system (atrium, ventricle, and gill), which reflects the similar localization of CGRP in the nervous and vascular systems as mammals. It was observed that the second receptor was expressed in several tissues, namely cartilage, brain, pituitary gland, gill, atrium, ventricle, pancreas, spleen, liver, gall bladder, intestine, rectal gland, kidney, testis and ovary. This localization pattern was very similar to flounder CTR. Both receptor mRNAs were strongly expressed in the gill. This suggests that the calcitonin-family members are involved in the osmoregulation of stingray as this fish is known to be euryhaline. When a stingray was transferred to diluted seawater (20% seawater), the expression of both receptors significantly decreased in the gill. Similar results were obtained in the kidney of the stingray. Thus, our cloning and isolation of both receptors in the stingray will be helpful for elucidation of their physiological role(s) such as osmoregulation including calcium metabolism of cartilaginous fish. © 2012 Elsevier B.V.
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| 93.
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Yano, Sachiko ; Kitamura, Kei-ichiro ; Satoh, Yusuke ; Nakano, Masaki ; Hattori, Atsuhiko ; Sekiguchi, Toshio ; Ikegame, Mika ; Nakashima, Hiroshi ; Omori, Katsunori ; Hayakawa, Kazuichi ; Chiba, Atsuhiko ; Sasayama, Yuichi ; Ejiri, Sadakazu ; Mikuni-Takagaki, Yuko ; Mishima, Hiroyuki ; Funahashi, Hisayuki ; Sakamoto, Tatsuya ; Suzuki, Nobuo
概要:
Fish scales are a form of calcified tissue similar to that found in human bone. In medaka scales, we detected both osteo
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blasts and osteoclasts and subsequently developed a new scale assay system. Using this system, we analyzed the osteoblastic and osteoclastic responses under 2-, 3-, and 4-gravity (G) loading by both centrifugation and vibration. After loading for 10 min, the scales from centrifugal and vibration loading were incubated for 6 and 24 hrs, respectively, after which the osteoblastic and osteoclastic activities were measured. Osteoblastic activity significantly increased under 2- to 4-G loading by both centrifugation and vibration. In contrast, we found that osteoclastic activity significantly decreased under 2- and 3-G loading in response to both centrifugation and vibration. Under 4-G loading, osteoclastic activity also decreased on centrifugation, but significantly increased under 4-G loading by vibration, concomitant with markedly increased osteoblastic activity. Expression of the receptor activator of the NF-αB ligand (RANKL), an activation factor of osteoclasts expressed in osteoblasts, increased significantly under 4-G loading by vibration but was unchanged by centrifugal loading. A protein sequence similar to osteoprotegerin (OPG), which is known as an osteoclastogenesis inhibitory factor, was found in medaka using our sequence analysis. The ratio of RANKL/OPG-like mRNAs in the vibration-loaded scales was significantly higher than that in the control scales, although there was no difference between centrifugal loaded scales and the control scales. Accordingly, medaka scales provide a useful model by which to analyze bone metabolism in response to physical strain. © 2013 Zoological Society of Japan.
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| 94.
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論文
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Suzuki, Nobuo ; Maruyama, Yusuke ; Nakano, Masaki ; Hattori, Atsuhiko ; Honda, Masato ; Shimasaki, Yohei ; Sekiguchi, Toshio ; Mishima, Hiroyuki ; Wada, Shigehito ; Srivastav, Ajai K. ; Hayakawa, Kazuichi ; Oshima, Yuji
概要:
We recently demonstrated that prostaglandin E2 PG¿ increases osteoclastic activity and induces bone resorption in both i
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n vitro and in vivo experiments using goldfish. In the fish reproductive period, the plasma calcium (Ca) level in female teleosts increases remarkably to make vitellogenin, which is a major component of egg protein and a Ca-binding protein. In this period, however, there is no reported relationship between PGE2 and Ca metabolism in fish. To clarify the Ca metabolism in fish reproduction, we examined plasma PGE2 and Ca levels and measured tartrate-resistant acid phosphatase (TRAP) activities as an indicator of osteoclastic activity in goldfish. Plasma PGE2 levels in the reproductive stage significantly increased as compared with those in non-reproductive stages. Also, both plasma Ca and TRAP increased in the reproductive stage. Significant positive correlations were recognized between plasma Ca and the gonad somatic index (r=0.81, p<0.001), plasma Ca and plasma PGE2 levels (r=0.635, p<0.05), and plasma Ca and plasma TRAP activities (r=0.584, p<0.05) from the analysis using samples of both reproductive and nonreproductive stages. Taking these data into consideration, we suggested that PGE, acts on osteoclasts and increases plasma Ca as a result of osteoclastic bone resorption, and we concluded that PGE, is an important hormone in Ca metabolism during fish reproduction.
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| 95.
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論文
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Yachiguchi, Koji ; Sekiguchi, Toshio ; Nakano, Masaki ; Hattori, Atsuhiko ; Yamamoto, Megumi ; Kitamura, Kei-ichiro ; Maeda, Masahiro ; Tabuchi, Yoshiaki ; Kondo, Takashi ; Kamauchi, Hiromitsu ; Nakabayashi, Hajime ; Srivastav, Ajai K. ; Hayakawa, Kazuichi ; Sakamoto, Tatsuya ; Suzuki, Nobuo
概要:
To evaluate the effects of inorganic mercury (InHg) and methylmercury (MeHg) on bone metabolism in a marine teleost, the
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activity of tartrate-resistant acid phosphatase (TRAP) and alkaline phosphatase (ALP) as indicators of such activity in osteoclasts and osteoblasts, respectively, were examined in scales of nibbler fish (Girella punctata). We found several lines of scales with nearly the same TRAP and ALP activity levels. Using these scales, we evaluated the influence of InHg and MeHg. TRAP activity in the scales treated with InHg (10-5 and 10-4 M) and MeHg (10-6 to 10-4 M) during 6 hrs of incubation decreased significantly. In contrast, ALP activity decreased after exposure to InHg (10-5 and 10-4 M) and MeHg (10-6 to 10-4 M) for 18 and 36 hrs, although its activity did not change after 6 hrs of incubation. As in enzyme activity 6 hrs after incubation, mRNA expression of TRAP (osteoclastic marker) decreased significantly with InHg and MeHg treatment, while that of collagen (osteoblastic marker) did not change significantly. At 6 hrs after incubation, the mRNA expression of metallothionein, which is a metal-binding protein in osteoblasts, was significantly increased following treatment with InHg or MeHg, suggesting that it may be involved in the protection of osteoblasts against mercury exposure up to 6 hrs after incubation. To our knowledge, this is the first report of the effects of mercury on osteoclasts and osteoblasts using marine teleost scale as a model system of bone. © 2014 Zoological Society of Japan.
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| 96.
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論文
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Yachiguchi, Koji ; Matsumoto, Noriko ; Haga, Yuki ; Suzuki, Motoharu ; Matsumura, Chisato ; Tsurukawa, Masahiro ; Okuno, Toshihiro ; Nakano, Takeshi ; Kawabe, Kimi ; Kitamura, Kei-ichiro ; Toriba, Akira ; Hayakawa, Kazuichi ; Chowdhury, Vishwajit S. ; Endo, Masato ; Chiba, Atsuhiko ; Sekiguchi, Toshio ; Nakano, Masaki ; Tabuchi, Yoshiaki ; Kondo, Takashi ; Wada, Shigehito ; Mishima, Hiroyuki ; Hattori, Atsuhiko ; Suzuki, Nobuo
概要:
To analyze the effect of polychlorinated biphenyl (PCB) 118 on fish bone metabolism, we examined osteoclastic and osteob
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lastic activities, as well as plasma calcium levels, in the scales of PCB (118)-injected goldfish. In addition, effect of PCB (118) on osteoclasts and osteoblasts was investigated in vitro. Immature goldfish, in which the endogenous effects of sex steroids are negligible, were used. PCB (118) was solubilized in dimethyl sulfoxide at a concentration of 10 ppm. At 1 and 2 days after PCB (118) injection (100 ng/g body weight), both osteoclastic and osteoblastic activities, and plasma calcium levels were measured. In an in vitro study, then, both osteoclastic and osteoblastic activities as well as each marker mRNA expression were examined. At 2 days, scale osteoclastic activity in PCB (118)-injected goldfish increased significantly, while osteoblastic activity did not change significantly. Corresponding to osteoclastic activity, plasma calcium levels increased significantly at 2 days after PCB (118) administration. Osteoclastic activation also occurred in the marker enzyme activities and mRNA expressions in vitro. Thus, we conclude that PCB (118) disrupts bone metabolism in goldfish both in vivo and in vitro experiments. © 2012 The Author(s).
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| 97.
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論文
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Tang, Ning ; Suzuki, Genki ; Morisaki, Hiroshi ; Tokuda, Takahiro ; Yang, Xiaoyang ; Zhao, Lixia ; Lin, Jinming ; Kameda, Takayuki ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Airborne particulates were collected at an urban site (site 1) from 2004 to 2010 and at a suburban site (site 2) in 2010
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in Beijing. Nine polycyclic aromatic hydrocarbons (PAHs) and five nitropolycyclic aromatic hydrocarbons (NPAHs) in the airborne particulates were determined by HPLC with fluorescence and chemiluminescence detection, respectively. The concentrations of PAHs and NPAHs were higher in heating season than in non-heating season at the two sites. Both the concentrations of PAHs and NPAHs decreased in the non-heating season but only the concentrations of NPAHs decreased in heating season at site 1, from 2004 to 2010. These findings suggest that source control measures implemented by the city of Beijing helped to reduce air pollution in Beijing. The concentrations of PAHs increased at site 1 in 2010, possibly because of the transport of emissions from windward other areas, such as Shanxi province. Several diagnostic ratios of PAHs and NPAHs showed that the different sources contributed to Beijing's air pollution, although coal combustion was the main source in the heating season and vehicle emission was the main source in the non-heating season. An analysis of physical parameters at Beijing showed that high wind speed can remove atmospheric PAHs and NPAHs in the heating season and that high relative humidity can remove them in the non-heating season. © 2017 Elsevier Ltd<br />Embargo Period 12 months
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| 98.
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論文
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Morisaki, Hiroshi ; Nakamura, Shiho ; Tang, Ning ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Benzo[c]fluorene (BcFE) concentrations in benzene/ethanol extracts of airborne particulates were determined by high-perf
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ormance liquid chromatography (HPLC) with fluorescence detection. HPLC conditions were as follows: columns, two ZORBAX Eclipse PAH (4.6 i.d. × 250 mm, 3.5 μm) and one Inertsil ODS-P (4.6 i.d. × 250 mm, 5 μm) in series; mobile phase, acetonitrile–water (98:2, v/v), 0.3 mL/min; detection wavelengths, excitation 309 nm, emission 354 nm. Particulate-phase BcFE concentrations in the atmosphere varied seasonally (winter > summer). The concentrations were 11000 ± 6100 pg m−3 (winter) and 40 ± 12 pg m−3 (summer) in Beijing, China, and 13 ± 5.0 pg m−3 (winter) and 2.7 ± 0.52 pg m−3 (summer), in Kanazawa, Japan. In both cities, the particulate-phase BcFE concentration in the atmosphere was lower than that of benzo[a]pyrene (BaP) by a factor of 0.03 – 0.43. However, the mutagenic contribution of particulate-phase BcFE in the atmosphere in winter calculated from the mutagenicity relative potency factor was greater than that of BaP.
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| 99.
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論文
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Suzuki, Nobuo ; Sato, Masayuki ; Nassar, Hossam F. ; Abdel-Gawad, Fagr Kh. ; Bassem, Samah M. ; Yachiguchi, Koji ; Tabuchi, Yoshiaki ; Endo, Masato ; Sekiguchi, Toshio ; Urata, Makoto ; Hattori, Atsuhiko ; Mishima, Hiroyuki ; Shimasaki, Youhei ; Oshima, Yuji ; Hong, Chun-Sang ; Makino, Fumiya ; Tang, Ning ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
We have developed an original in vitro bioassay using teleost scale, that has osteoclasts, osteoblasts, and bone matrix
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as each marker: alkaline phosphatase (ALP) for osteoblasts and tartrate-resistant acid phosphatase (TRAP) for osteoclasts. Using this scale in vitro bioassay, we examined the effects of seawater polluted with highly concentrated polycyclic aromatic hydrocarbons (PAHs) and nitro-polycyclic aromatic hydrocarbons (NPAHs) on osteoblastic and osteoclastic activities in the present study. Polluted seawater was collected from two sites (the Alexandria site on the Mediterranean Sea and the Suez Canal site on the Red Sea). Total levels of PAHs in the seawater from the Alexandria and Suez Canal sites were 1364.59 and 992.56 ng/l, respectively. We were able to detect NPAHs in both seawater samples. Total levels of NPAHs were detected in the seawater of the Alexandria site (12.749 ng/l) and the Suez Canal site (3.914 ng/l). Each sample of polluted seawater was added to culture medium at dilution rates of 50, 100, and 500, and incubated with the goldfish scales for 6 hrs. Thereafter, ALP and TRAP activities were measured. ALP activity was significantly suppressed by both polluted seawater samples diluted at least 500 times, but TRAP activity did not change. In addition, mRNA expressions of osteoblastic markers (ALP, osteocalcin, and the receptor activator of the NF-κB ligand) decreased significantly, as did the ALP enzyme activity. In fact, ALP activity decreased on treatment with PAHs and NPAHs. We conclude that seawater polluted with highly concentrated PAHs and NPAHs influences bone metabolism in teleosts. © 2016 Zoological Society of Japan.<br />Embargo Period 12 months
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| 100.
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論文
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Suzuki, Nobuo ; Hayakawa, Kazuichi ; Kameda, Takayuki ; Toriba, Akira ; Tang, Ning ; Tabata, Makoto J. ; Takada, Koji ; Wada, Shigehito ; Omori, Katsunori ; Srivastav, Ajai K. ; Mishima, Hiroyuki ; Hattori, Atsuhiko
概要:
金沢大学環日本海域環境研究センター生物多様性研究部門<br />AAims: We previously demonstrated that monohydroxylated polycyclic aromatic hydrocarbons
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(OHPAHs) bound to a human estrogen receptor (ER) by a yeast two-hybrid assay, but polycyclic aromatic hydrocarbons did not have a binding activity. Therefore, the direct effect of 3-hydroxybenz[a]anthracene (3-OHBaA) and 4-hydroxybenz[a]anthracene (4-OHBaA) on osteoclasts and osteoblasts in teleosts was examined. As a negative control, 1-hydroxypyrene (1-OHPy), which has no binding activity to human ER, was used. Main methods: The effect of OHPAHs on osteoclasts and osteoblasts was examined by an assay system using teleost scale as each marker: tartrate-resistant acid phosphatase for osteoclasts and alkaline phosphatase for osteoblasts. Changes in cathepsin K (an osteoclastic marker) and insulin-like growth factor-I (IGF-I) (an osteoblastic marker) mRNA expressions in 4-OHBaA-treated goldfish scales were examined by using a reverse transcription-polymerase chain reaction. Key findings: In both goldfish (a freshwater teleost) and wrasse (a marine teleost), the osteoclastic activity in the scales was significantly suppressed by 3-OHBaA and 4-OHBaA, although 1-OHPy did not affect the osteoclastic activity. In reference to osteoblasts, the osteoblastic activity decreased with both 3-OHBaA and 4-OHBaA and did not change with the 1-OHPy treatment. However, 17β-estradiol (E2) significantly increased both the osteoclastic and osteoblastic activities in the scales of both goldfish and wrasse. The mRNA expressions of both cathepsin K and IGF-I decreased in the 4-OHBaA-treated scales but increased in the E2-treated scales. Significance: The current data are the first to demonstrate that 3-OHBaA and 4-OHBaA inhibited both osteoclasts and osteoblasts and disrupted the bone metabolism in teleosts. © 2009 Elsevier Inc. All rights reserved.
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