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| 1.
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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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| 2.
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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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| 3.
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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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| 4.
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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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| 5.
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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
概要:
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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| 6.
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Kakimoto, Kensaku ; Toriba, Akira ; Ohno, Takanori ; Ueno, Mariko ; Kameda, Takayuki ; Tang, Ning ; Hayakawa, Kazuichi
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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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| 7.
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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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| 8.
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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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| 9.
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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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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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| 11.
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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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| 12.
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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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| 13.
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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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| 14.
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Tamura, Masayoshi ; Mochizuki, Naoki ; Nagatomi, Yasushi ; Harayama, Koichi ; Toriba, Akira
概要:
Fumonisin A-series (FAs) in a reference material of corn sample that was naturally contaminated with fumonisins was char
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acterized using high-resolution liquid chromatography-Orbitrap mass spectrometry (LC-Orbitap MS). Peaks for fumonisin B1 (FB1), fumonisin B2 (FB2), and fumonisin B3 (FB3), in addition to three peaks corresponding to unknown compounds I, II, and III, were detected in the chromatogram for the corn sample. Fragment ion analysis for FB1, FB2, and FB3 showed that while the ions formed at m/z values of 200-800 were similar to those formed by the cleavage of the tricarballylic acids and the hydroxyl groups, the fragmentation patterns at m/z values of 50-200 varied depending on the hydroxyl group locations in the compounds. Fragment ion analysis of compounds I-III revealed structural similarities to FBs, only differing by an additional C<inf>2</inf>H<inf>2</inf>O in the unknown compounds. Using these results and by comparing the product ion mass spectra of compound I with fumonisin A1 (FA1) synthesized from FB1 standards, compounds I-III were hypothesized to be N-acetyl analogs of FBs: fumonisins A1 (FA1), A2 (FA2), and A3 (FA3). The method for determining concentrations was validated with FA1, FB1, FB2, and FB3 standards and applied to analyze the reference material. The FB1, FB2, and FB3 analytical levels were within acceptance limits and the amount of FA1 in the material was ~15% of FB1 amount at 4.2 mg/kg. © 2014 by the authors; licensee MDPI, Basel, Switzerland.
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| 15.
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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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| 16.
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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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| 17.
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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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| 18.
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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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| 19.
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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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| 20.
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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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| 21.
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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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| 22.
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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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| 23.
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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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| 24.
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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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| 25.
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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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| 26.
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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
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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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| 27.
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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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| 28.
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論文
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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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| 29.
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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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| 30.
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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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| 31.
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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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| 32.
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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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| 33.
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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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| 34.
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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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| 35.
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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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| 36.
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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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| 37.
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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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| 38.
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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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| 39.
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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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| 40.
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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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| 41.
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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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| 42.
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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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| 43.
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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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| 44.
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Suzuki, Nobuo ; Hayakawa, Kazuichi ; Kameda, Takayuki ; Toriba, Akira ; Tang, Ning ; Tabata, Makoto J. ; Takada, Koji ; Wada, Shigehito ; Omori, Katsunori K. ; Srivastav, Ajai ; 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 />Aims: 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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| 45.
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論文
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鳥羽, 陽 ; Toriba, Akira
概要:
金沢大学医薬保健研究域薬学系<br />多環芳香族炭化水素(PAH)のなかで特に強い発がん作用を有するBenzo[a]pyrene(BaP)に着目し、BaPが代謝活性化されて生成する発がん作用の本体であるBaP-DNA付加体を生体指標(バイ
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オマーカー)として用いるために、BaP-DNA付加体の高速液体クロマトグラフ-タンデム質量分析計(LC-MS/MS)を用いた新しい高感度分析法の開発を試みた。DNA付加体関連物質としてdG-BPDE、及びdG-BPDEを加水分解して得られるBaP tetrolをBaP-DNA付加体の分析対象化合物としてLC-MS/MSの条件検討を行った。分子量関連イオンをプリカーサーイオンとしてdG-BPDEのMS/MSスペクトルを得たところ、グアニン残基が脱離したイオンが観察され、このイオンを効率よく生成させるように、移動相条件、電圧等を最適化した。これに順じてBaP tetrolのLC-MS/MS条件を最適化するとともに、蛍光検出HPLCによる分析法も確立した。確立した分析法を培養細胞にBaPを暴露して得られたDNAに適用したところ、発がん作用の本体として知られる代謝生成物のanti-BPDEに由来するBaP-DNA付加体をBaP tetrolとして検出することができた。細胞のBaP処理24時間後からBPDE-DNA付加体が観察され、処理時間に依存して付加体量の増加が見られた。続いてDNA付加体を利用したヒトの曝露評価を行うためのバイオマーカーの開発を行った。被験者への負担(侵襲性)の観点から尿中のBaP-DNA付加体関連物質をバイオマーカー候補として、DNA付加体を加水分解して得られる尿中tetrolの検出を試みたが、前処理法の回収率の低さなどの改善の余地が残った。<br />研究課題/領域番号:17659036, 研究期間(年度):2005 – 2006<br />出典：「多環芳香族炭化水素類(PAH)-DNA付加体を指標とするPAH曝露評価法の開発」研究成果報告書 課題番号17659036（KAKEN：科学研究費助成事業データベース（国立情報学研究所））（https://kaken.nii.ac.jp/ja/grant/KAKENHI-PROJECT-17659036/)を加工して作成
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| 46.
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鳥羽, 陽 ; Toriba, Akira
概要:
金沢大学医薬保健研究域薬学系<br />多環芳香族炭化水素類(PAHs)は、化石燃料に含まれ、また燃焼過程で生成する非意図的生成物であり、自動車やタバコなどを排出源として環境中に放出されるため、ヒトや動物の曝露量は高い。PAHsは、内分泌撹
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乱物質の一つとして疑いが持たれているものの、ヒトに対するリスク評価は十分ではない。昨年度の研究により、PAH関連化合物のエストロゲン様/抗エストロゲン作用を酵母two-hybrid法を用いて測定した結果、モノヒドロキシ体が特に強い活性を有することを見出した。そこで本年度は、様々な骨格を有するPAHモノヒドロキシ体のERに対するアゴニスト及びアンタゴニスト作用と構造との関係を考察し、活性発現に影響する因子の推定を行った。まずエストロゲン様/抗エストロゲン活性を示すPAHモノヒドロキシ体の多くは4環構造を有し、同じ環数を有していても母核構造や水酸基の位置が異なることによって発現する活性の種類やその強さが異なることが分かった。また、母核構造の違いを表すL/B比と水酸基の位置の違いを表すO-H distanceを用いて活性を有する化合物の分子構造を評価し、各パラメータ値がそれぞれ特定の範囲を満たす化合物が強いエストロゲン様/抗エストロゲン活性を示す傾向にあることを明らかとした。さらにCACheを用いたコンピューターシミュレーション解析によって算出されたフェノール性水酸基の酸素原子の部分電荷が活性発現に寄与することを確認した。環境試料のヒトに対する内分泌撹乱作用のリスク評価を行う上でエストロゲン様/抗エストロゲン活性を活性等価係数として表すことは必要不可欠であると考えられ、本研究で得られた活性値を基にPAHモノヒドロキシ体の活性等価係数を算出することが可能となった。また一方で、タバコ煙や大気粉塵抽出物などの環境試料中にPAHモノヒドロキシ体が存在することも確認できた。<br />研究課題/領域番号:14042219, 研究期間(年度):2002 – 2003<br />出典：「多環芳香族炭化水素類(PAHs)のホルモン活性等価係数(HAEF)の確立」研究成果報告書 課題番号14042219（KAKEN：科学研究費助成事業データベース（国立情報学研究所））（https://kaken.nii.ac.jp/ja/grant/KAKENHI-PROJECT-14042219/)を加工して作成
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| 47.
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論文
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鳥羽, 陽 ; Toriba, Akira
概要:
金沢大学医薬保健研究域薬学系<br />近年発展著しいアジアの国々では，大気環境が年々悪化し，今後様々な疾患の増加が懸念される。大気汚染物質の曝露量や発生源などの環境要因を解明することは，健康影響のリスク評価に重要である。そこで尿中に排泄さ
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れる汚染物質由来の生体指標（バイオマーカー）を開発し，大気汚染の特徴の異なるアジア地域の住民を対象に曝露量や発生源について解析してバイオマーカーの有用性を評価した。タイ山間部の農村における被験者集団の多環芳香族炭化水素類への高濃度曝露がバイオマーカーの測定により明確になり，家屋内での調理による木材燃焼煙への曝露が原因であることが判明したことから，確立したバイオマーカーの有用性が証明された。<br />The rapid development of Asian countries has caused serious air pollution problems, and there are fears of increased risk of various diseases. The elucidation of the environmental factors such as exposure and sources of air pollutants is important for risk assessment of health effects. In this study, we developed biological markers (biomarkers) from pollutants that are excreted in the urine and evaluated the usefulness of the biomarkers by analyzing the exposure amounts and sources with residents of Asian region having different characteristic of air pollution. High-exposure to polycyclic aromatic hydrocarbons of the subject group in the rural villages of Thailand mountainous areas was clarified by the measurement of the biomarkers. It was caused by exposure to wood burning smoke from cooking inside the houses. In conclusion, the usefulness of the developed biomarkers was demonstrated.<br />研究課題/領域番号:23406004, 研究期間(年度):2011-04-01 – 2015-03-31
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| 48.
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論文
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鳥羽, 陽 ; Toriba, Akira
概要:
金沢大学医薬保健研究域薬学系<br />中国において大気汚染の主要な発生源となっている石炭燃焼由来の有機汚染物質で，黄砂を含め日本へ長距離輸送されている可能性が高いと推定される石炭燃焼マーカーとして含硫黄多環芳香族化合物(PASHs)を提案
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し，尿中代謝物を生体指標（バイオマーカー）とする石炭燃焼煙の人体曝露評価法を開発することを目的とした。代表的なPASHsの中からヒトへの曝露量が高いと予測できたdibenzothiophene (DBT)をマーカー候補とし，DBT投与ラット尿中から代謝物を同定し，代謝経路を明らかにすることに成功した。同定された主代謝物をバイオマーカー候補とし，実際にヒト尿試料から検出できる可能性が示唆された。<br />Polycyclic aromatic sulfur heterocyclic compounds (PASHs) are organic pollutants from coal combustion, which has become a major source of air pollution in China and are estimated to be a cross-boundary pollutant such as Asian dust. Urinary metabolites of PASHs as a biomarker for coal burning exposure were examined in this study. Dibenzothiophene (DBT) was predicted to have high exposures to humans in the tested PASH candidates. DBT metabolites from DBT administered rat urine were successfully identified and its metabolic pathway was elucidated. The analysis of human urine samples suggested the possibility of the metabolite excretion. It is concluded that the identified major metabolite is a convincing biomarker candidate for the biomarker of exposure to coal-burning smoke.<br />研究課題/領域番号:24590160, 研究期間(年度):2012-04-01 – 2015-03-31
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| 49.
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論文
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鳥羽, 陽 ; Toriba, Akira
概要:
ベンゾ[a]ピレン(BaP)をはじめとする多環芳香族炭化水素類(PAH)の内分泌撹乱作用は,抗エストロゲン作用などの一部の作用のみが報告されるにとどまっていることから,PAH及び類縁化合物の内泌撹乱作用を評価した。BaPを含むいくつかのPA
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Hに抗エストロゲンあるいは抗アンドロゲン作用が観察され,その作用はアリル炭化水素受容体を介して発現することが推定された。また,BaPの代謝物として知られるBaPモノヒドロキシ体(OHBaPs)がエストロゲン様/抗エストロゲン活性を示したが,ジオール体及びキノン体は活性を示さなかった。このことから,フェノール性水酸基の存在が活性発現に必須であるだけでなく,水酸基の位置も重要な要因であることが明らかとなり,BaPが生体内で代謝されることで新たな内分泌撹乱作用を獲得することが示唆された。 次に,BaPをはじめとするPAHの内分泌撹乱作用のヒトに対するリスク評価を行うにあたり,PAH曝露量を評価するための2つの手法を検討した。まず地域別の大気粉じん中PAH濃度を測定し,呼吸を介したPAH曝露の推定を試みた。その結果,PAH曝露量は都市域で高く,さらに地域のエネルギー事情を強く反映することが分かった。しかしながら,個人のPAH曝露量はPAHの摂取源の一つである喫煙などの生活習慣によっても異なってくることから,尿中代謝物量を指標とするPAH曝露量の推定を試みた。まず,BaPをシトクロムP450によりin vitroで代謝させたときに生成するBaP代謝物としての1-OH,3-OH,及び9-OHBaPを同定した。さらに尿中OHBaPs、及びPAH曝露の指標としての1-ヒドロキシピレン(1-OHP)と2-ヒドロキシフルオレン(2-OHF)についてのHPLC-蛍光検出法による分析法を開発し,ヒトの尿中代謝物を測定した結果,OHBaPsの異性体の中でエストロゲン様活性を有する3-OHBaPを検出した。また1-OHP及び2-OHFについては,PAH摂取源の一つである喫煙の影響を検討したところ,喫煙者でそれらの尿中濃度が有意に高く,PAHの曝露指標になることが分かった。以上の結果から、内分泌撹乱作用を有するPAH代謝物が生体内で生成することを確認するとともに,尿中PAH代謝物量が個人のPAH曝露量を反映した,優れた指標となることが明らかとなった。<br />Polycyclic aromatic hydrocarbons (PAHs) such as benzo[a]pyrene (BaP) have been reported for their endocrine-disrupting activities, primarily their antiestrogenic characteristics. In this study, the endocrine-disrupting activities of PAHs and their analogues (metabolites) were investigated. Several PAHs containing BaP exhibited the antiestrogenic and antiandrogenic effects and it was suggested that the PAHs act as antiestrogens and antiandrogens by activating the aryl hydrocarbon receptor (AhR). On the other hand, the estrogenic and antiestrogenic effects of the BaP metabolites were also examined. Monohydroxy derivatives of BaP (OHBaPs) exhibited the estrogenic or antiestrogenic effects, diol and quinone derivatives of BaP did not. Therefore, the presence and position of phenolic hydroxy group in the BaP metabolites play an important role in the induction of the endocrine-disrupting activities.Two methods for the evaluation of PAH exposure were developed to assess a human risk of the en docrine-disrupting effects for PAHs and their metabolites. To evaluate the exposure to PAHs from ambient air by inhalation, the atmospheric concentrations of PAHs were measured with the airborne particulates collected in three cities. The concentrations of PAHs, that is, the exposure dose were much higher in urban area than in suburban area, and the main contributors of PAHs in urban area were considered to be automobiles, domestic heating systems such as furnaces and kerosene heaters, power plants and incinerators. However, the intake of PAHs depends on individual lifestyle such as diet and tobacco smoke, therefore, biomonitoring is an especially valuable method to provide exposure data of PAHs. Urinary metabolites of PAHs including BaP were used as PAH biomarkers. 1-, 3-, 9-OHBaPs were identified as major metabolites of BaP in vitro by human recombinant cytochrome P450. The methods for determining OHBaPs, 1-hydroxypyrene (1-OHP) and 2-hydroxyfluorene (2-OHF) using high-performance liquid chromatography with fluorescence detection were developed. 3-OHBaP, which has a particularly high estrogenic activity, was detected in the urine of a subject. Further, the effect of smoking on the exposure to PAHs was investigated using the concentrations of urinary 1-OHP and 2-OHF. The urinary 1-OHP and 2-OHF levels in smokers were significantly higher than those in non-smokers. Thus, urinary metabolites of PAHs may be sensitive and specific biomarkers for the assessment of the exposure to PAHs.<br />研究課題/領域番号:13558066, 研究期間(年度):2001–2002<br />出典：「ベンゾ[a]ピレン及びその代謝物の内分泌撹乱作用の評価法に関する研究」研究成果報告書 課題番号13558066 (KAKEN：科学研究費助成事業データベース（国立情報学研究所）) 本文データは著者版報告書より作成
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Chung, Sang Woon ; Chung, Hae Young ; Toriba, Akira ; Hayakawa, Kazuichi
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金沢大学大学院自然科学研究科<br />場所：金沢大学自然科学研究科図書館棟1階，講演会場：図書館棟1階 大会議室，ポスター会場：図書館棟1階12会議室,主催・共催：文部科学省２１世紀COE「環日本海域の環境計測と長期・短期変動予測」， 大
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気環境学会， 金沢大学工学部
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| 51.
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Chung, Sang Woon ; Chung, Hae Young ; Toriba, Akira ; Hayakawa, Kazuichi
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金沢大学大学院自然科学研究科<br />場所：金沢大学自然科学研究科図書館棟1階，講演会場：図書館棟1階 大会議室，ポスター会場：図書館棟1階12会議室,主催・共催：文部科学省２１世紀COE「環日本海域の環境計測と長期・短期変動予測」， 大
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気環境学会， 金沢大学工学部
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| 52.
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Yang, Xiaoyang ; Tang, Ning ; Okada, Yumi ; Kameda, Takayuki ; Toriba, Akira ; Utanohara, Yoichi ; Yamaji, Kazuyo ; Kawanishi, Takuya ; Tamura, Kenji ; Uno, Itsushi ; Hayakawa, Kazuichi
概要:
金沢大学大学院自然科学研究科<br />場所：金沢大学自然科学研究科図書館棟1階，講演会場：図書館棟1階 大会議室，ポスター会場：図書館棟1階12会議室,主催・共催：文部科学省２１世紀COE「環日本海域の環境計測と長期・短期変動予測」， 大
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気環境学会， 金沢大学工学部
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| 53.
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Chung, Sang Woon ; Chung, Hae Young ; Toriba, Akira ; Hayakawa, Kazuichi
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金沢大学大学院自然科学研究科<br />場所：東京大学弥生講堂，共催：文部科学省２１世紀COE「環日本海域の環境計測と長期・短期変動予測」，大気環境学会
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| 54.
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Yang, Xiaoyang ; Tang, Ning ; Okada, Yumi ; Kameda, Takayuki ; Toriba, Akira ; Utanohara, Yoichi ; Yamaji, Kazuyo ; Kawanishi, Takuya ; Tamura, Kenji ; Ohara, Toshimasa ; Uno, Itsushi ; Hayakawa, Kazuichi
概要:
金沢大学大学院自然科学研究科<br />場所：東京大学弥生講堂，共催：文部科学省２１世紀COE「環日本海域の環境計測と長期・短期変動予測」，大気環境学会
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| 55.
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Yang, Xiaoyang ; Okada, Yumi ; Tang, Ning ; Kameda, Takayuki ; Toriba, Akira ; Hayakawa, Kazuichi
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金沢大学大学院自然科学研究科<br />Promoting Environmental Pesearch in Pan-Japan Sea Area : Young Researchers' Network, Schedule: March
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8-10,2006,Kanazawa Excel Hotel Tokyu, Japan, Organized by: Kanazawa University 21st-Century COE Program, Environmental Monitoring and Prediction of Long- & Short- Term Dynamics of Pan-Japan Sea Area ; IICRC(Ishikawa International Cooperation Research Centre), Sponsors : Japan Sea Research ; UNU-IAS(United Nations University Institute of Advanced Studies)+Ishikawa Prefecture Government ; City of Kanazawa
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| 56.
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Chung, Sang Woon ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
金沢大学大学院自然科学研究科<br />Promoting Environmental Pesearch in Pan-Japan Sea Area : Young Researchers' Network, Schedule: March
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8-10,2006,Kanazawa Excel Hotel Tokyu, Japan, Organized by: Kanazawa University 21st-Century COE Program, Environmental Monitoring and Prediction of Long- & Short- Term Dynamics of Pan-Japan Sea Area ; IICRC(Ishikawa International Cooperation Research Centre), Sponsors : Japan Sea Research ; UNU-IAS(United Nations University Institute of Advanced Studies)+Ishikawa Prefecture Government ; City of Kanazawa
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| 57.
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Chetiyanukornkul, Thaneeya ; Prapamontol, Tippwan ; Toriba, Akira ; Ning, Tang ; Kameda, Takayuki ; Hayakawa, Kazuichi
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Chiang Mai University<br />金沢大学大学院自然科学研究科<br />Promoting Environmental Pesearch in Pan-Japan Sea Area : Young Researcher
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s' Network, Schedule: March 8-10,2006,Kanazawa Excel Hotel Tokyu, Japan, Organized by: Kanazawa University 21st-Century COE Program, Environmental Monitoring and Prediction of Long- & Short- Term Dynamics of Pan-Japan Sea Area ; IICRC(Ishikawa International Cooperation Research Centre), Sponsors : Japan Sea Research ; UNU-IAS(United Nations University Institute of Advanced Studies)+Ishikawa Prefecture Government ; City of Kanazawa
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| 58.
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Tang, Ning ; Tamura, Kenji ; Hattori, Tetsuyuki ; Yang, Xiao-Yang ; Kameda, Takayuki ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
金沢大学大学院自然科学研究科<br />National Institute for Environmental Studies<br />Promoting Environmental Pesearch in Pan-Japan Sea
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Area : Young Researchers' Network, Schedule: March 8-10,2006,Kanazawa Excel Hotel Tokyu, Japan, Organized by: Kanazawa University 21st-Century COE Program, Environmental Monitoring and Prediction of Long- & Short- Term Dynamics of Pan-Japan Sea Area ; IICRC(Ishikawa International Cooperation Research Centre), Sponsors : Japan Sea Research ; UNU-IAS(United Nations University Institute of Advanced Studies)+Ishikawa Prefecture Government ; City of Kanazawa
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| 59.
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Chetiyanukornkul, Thaneeya ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi
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金沢大学大学院自然科学研究科<br />Proceeding : International Symposium of Kanazawa University 21st-Century COE Program Vol.2(2004),Sch
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edule: February 29(SUN)-March 3(WED), Venue: 29 FEB, Ishikawa Life-Long Learning Center(Former Prefectural Government Building) / 1-3 MAR Kanazawa Art Hall, Organized by: Kanazawa University 21st-Century COE Program / Ishikawa International Cooperation Research Centre / United Nations University-Institute of Advanced Studies, Supported by: Ishikawa Prefectural Government / City of Kanazawa, Eds : Hayakawa, Kazuichi / Kizu, Ryoichi / Kamata, Naoki
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| 60.
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Okamura, Kazumasa ; Kizu, Ryoichi ; Hayakawa, Kazuichi ; Toriba, Akira
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金沢大学大学院自然科学研究科<br />Proceeding : International Symposium of Kanazawa University 21st-Century COE Program Vol.2(2004),Sch
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edule: February 29(SUN)-March 3(WED), Venue: 29 FEB, Ishikawa Life-Long Learning Center(Former Prefectural Government Building) / 1-3 MAR Kanazawa Art Hall, Organized by: Kanazawa University 21st-Century COE Program / Ishikawa International Cooperation Research Centre / United Nations University-Institute of Advanced Studies, Supported by: Ishikawa Prefectural Government / City of Kanazawa, Eds : Hayakawa, Kazuichi / Kizu, Ryoichi / Kamata, Naoki
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| 61.
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Tang, Ning ; Taga, Rina ; Hattori, Tetsuyuki ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi ; Tamura, Kenji ; Kakimoto, Hitoshi
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金沢大学大学院自然科学研究科<br />国立環境研究所<br />石川県保健環境センター<br />Proceeding : International Symposium of Kanazawa University 21st-Centu
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ry COE Program Vol.2(2004),Schedule: February 29(SUN)-March 3(WED), Venue: 29 FEB, Ishikawa Life-Long Learning Center(Former Prefectural Government Building) / 1-3 MAR Kanazawa Art Hall, Organized by: Kanazawa University 21st-Century COE Program / Ishikawa International Cooperation Research Centre / United Nations University-Institute of Advanced Studies, Supported by: Ishikawa Prefectural Government / City of Kanazawa, Eds : Hayakawa, Kazuichi / Kizu, Ryoichi / Kamata, Naoki
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| 62.
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Hayakawa, Kazuichi ; Nomura, Maki ; Nakagawa, Takuya ; Oguri, Seiji ; Toriba, Akira ; Kizu, Ryoichi ; Sakaguchi, Toshifumi ; Tamiya, Eiichi
概要:
金沢大学大学院自然科学研究科 環境科学<br />Editor : Tazaki, Kazue |田崎, 和江
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| 63.
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Kizu, Ryoichi ; Ishii, Katsuaki ; Noji, Kazushige ; Toriba, Akira ; Hayakawa, Kazuichi
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金沢大学大学院自然科学研究科 環境科学<br />Editor : Tazaki, Kazue |田崎, 和江
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| 64.
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鳥羽, 陽 ; Toriba, Akira
概要:
金沢大学医薬保健研究域薬学系<br />北海道東部の湿原に生息するタンチョウは、絶滅危惧種に選定されている。近年、その生息域は人間の生活圏に近づき，人為起源の化学物質への曝露量が増える可能性があることから，化学物質への曝露量の推定は保護活動
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を行う上で重要である。本研究では、タンチョウの筋肉組織中の残留性有機汚染物質（POPs）を初めて測定し、観察された濃度は他の鳥類より低く、毒性発現を考慮すべきレベルではないことが分かった。また、胆汁に排泄される多環芳香族炭化水素（PAH）の代謝物である水酸化PAHの分析法を開発し、タンチョウの胆汁中に排泄される代謝物を検出することに成功し、PAH曝露指標の候補になることを明らかにした。<br />Japanese Red-crowned crane inhabits the marsh in the eastern Hokkaido and it is classified as an endangered species. Nowadays, it lives near human beings and it is concerned that Red-crowned cranes are exposed to more anthropogenic chemical substances. Therefore, it is important to investigate the exposure levels of the chemicals for their protection. In this study, we determined the concentrations of persistent organic pollutants (POPs) in red-crowned crane muscle tissues and the concentrations were not high that their toxicities need to be considered. Furthermore, hydroxylated metabolites of polycyclic aromatic hydrocarbons (PAHs) excreted in the bile of the crane were successfully identified and quantified by using a developed analytical method. The biliary metabolites should be useful for the surveillance of exposure to PAHs.<br />研究課題/領域番号:15K08043, 研究期間(年度):2015-04-01 - 2018-03-31
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| 65.
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鳥羽, 陽 ; Toriba, Akira
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金沢大学医薬保健研究域薬学系<br />多環芳香族炭化水素(PAH)は、化石燃料の燃焼過程で生成する非意図的生成物であり、自動車やタバコなどを排出源として環境中に放出されるPAHは、燃焼時もしくは大気中で窒素酸化物と反応して極めて強い発ガン
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性・変異原性を有するニトロ多環芳香族炭化水素(NPAH)を生成するNPAHのヒトや動物への暴露量は高いと予測され、その大気内挙動や季節変動、都市のエネルギー・交通事情との関係等が明らかになりつつあるが、ヒトに対するリスク評価(健康影響評価)が急務となっている。そこで本研究では、NPAHのヒトに対する曝露量を評価するためのバイオマーカーの開発を行うにあたり、指標の候補となるNPAHの尿中代謝物を同定した。NPAHの中で大気粉塵やディーゼル排ガス粉塵に高濃度で存在する1-ニトロピレン(1-NP)に着目し、まず代謝物として考えられるヒドロキシ-1-ニトロピレン(OH-1-NP)を合成した。尿中代謝物として存在するOH-1-NPを定量するためには、より高感度な分析法の開発が要求された。そこでOH-1-NPを逆相カラムで分離した後、オンライン白金/ロジウムカラムにより効率よく蛍光性のアミノ体に還元してその蛍光を検出することによりOH-1-NPを高感度に測定するHPLC-蛍光検出法を開発した。次に尿試料の前処理法を検討し、抱合体として存在するOH-1-NPを酵素で加水分解した後、逆相系と順相系の固相抽出カラムを組み合わせること夾雑ピークを効率よく除去することに成功した。実際にヒトの尿試料を用いてOH-1-NPの同定を試みたところ、OH-1-NPのピークを確認することができ、さらにそのピークを分取してLC-MSで測定したところ、その分子量関連イオンピークを観察することができた。開発したヒト尿中OH-1-NPの分析法は、NPAHの曝露量の有用な指標(バイオマーカー)となる可能性が高い。<br />研究課題/領域番号:15790077, 研究期間(年度):2003 – 2004<br />出典：「変異原性環境化学物質、ニトロ多環芳香族炭化水素類の人体曝露評価法の開発」研究成果報告書 課題番号15790077（KAKEN：科学研究費助成事業データベース（国立情報学研究所））（https://kaken.nii.ac.jp/ja/grant/KAKENHI-PROJECT-15790077/)を加工して作成
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