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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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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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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 ; 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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戸次, 加奈江 ; 滝上, 英孝 ; 鈴木, 剛 ; 唐, 寧 ; 鳥羽, 陽 ; 亀田, 貴之 ; 早川, 和一
概要:
Polycyclic aromatic hydrocarbons (PAHs) and dioxins have several toxic properties, including mutagenicity, carcinogenici
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ty and reproductive toxicity. PAHs mainly originate from the burning of petroleum and coal, while dioxins originate mainly from waste incineration and agrochemicals. Both PAHs and dioxins have aryl hydrocarbon receptor (AhR) binding activity which is related to toxicity of PAHs and dioxins. In this study, we evaluated AhR binding activity of airborne particles collected in Beijing, China and Kanazawa, Japan by DR-CALUX and the contribution of PAHs and dioxins to this activity. AhR binding activity of airborne particles in Beijing (1,200 ng • m-3) was four hundred times higher than in Kanazawa (2.7 ng • m-3). The composition of PAHs didn′t show large difference in Beijing and Kanazawa. The contribution of the PAHs to CALUX-TEQ was higher than dioxins and especially high in Kanazawa (10.4 %). These results suggest that PAHs show large contribution to the toxicity of airborne particles, and other kinds of PAH and PAH related compounds will also contribute to that toxicity. The difference of concentration and composition of these compounds result in the different level of toxicity of airborne particles in each city.
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| 7.
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戸次, 加奈江 ; 唐, 寧 ; 鳥羽, 陽 ; 早川, 和一
概要:
大気中には様々な有機汚染物質が含まれている.そのうち多環芳香族炭化水素(PAH)およびニトロ多環芳香族炭化水素(NPAH)は,化石燃料などの燃焼に伴って発生し,ヒトの健康に影響をおよぼす物質である.環日本海域の4ヶ国,中国,ロシア,韓国,日
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本は,主要エネルギーの種類や生活様式,産業構造や事業所の設備などが異なり,その結果大気汚染のレベルと中身も大きく異なると推定される.そこで,本報では中国と日本の製鉄業を中心とする都市である鉄嶺と北九州を選び大気粉塵を捕集後PAH,NPAH,変異原性,活性酸素種(ROS)生成能を測定し化学物質と毒性の点から比較評価を行った.PAH,NPAH濃度は中国で高濃度を示し,冬高夏低の傾向が見られた.また変異原性は冬に高いが,ROS生成能は夏に高くなる傾向が見られ,変異原性とROS生成能には異なる原因物質が関与すると考えられた.PAH,NPAHとは異なる化合物の寄与も大きいことが考えられた. Airborne participate matters contain many kinds of organic pollutants. Among them, polycyclic aromatic hydrocarbons (PAH), nitropolycyclic aromatic hydrocarbons (NPAH) and quinoid PAHs were reported to have several human health effects. We collected airborne particulates in Kitakyushu, Japan and Tieling, China in summer and winter, and analyzed the PAH and NPAH to evaluate the direct- and indirect-acting mutagenicities and generating activities of reactive oxygen species (ROS). The concentrations of PAHs and NPAHs in Tieling were much higher than in Kitakyushu, with seasonal variations. The mutagenicity level was higher in winter while the ROS generation activity was higher in summer. These results suggest that concentrations of PAH and NPAH didn' t correlate with mutagenicity and ROS generation activity. More studies are needed on the environmental behaviors of compounds other than PAHs and NPAHs, such as quinoid PAHs, and their biological activities.
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唐, 寧 ; 伊崎, 陽彦 ; 徳田, 貴裕 ; 季, 若男 ; 董, 麗君 ; 呉, 慶 ; 周, 志俊 ; 黄, 蓉 ; 林, 振宇 ; 亀田, 貴之 ; 鳥羽, 陽 ; 島, 正之 ; 早川, 和一
概要:
Urban air contains various kinds of organic pollutants. Among them, several polycyclic aromatic hydrocarbons (PAHs) and
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nitropolycyclic aromatic hydrocarbons (NPAHs) are carcinogenic and/or endocrine disrupting. PAHs and NPAHs in the atmosphere mainly originate from imperfect combustion of organic matter, such as petroleum and coal. In this study, total suspended particles (TSP) were collected in three different particulate size fractions by using Andersen low-volume air samplers in Shenyang, Shanghai and Fuzhou, China, in the winter and summer seasons in 2010. Nine PAHs and twelve NPAHs in the extracts from the TSP were analyzed by HPLC with fluorescence detection and chemiluminescence detection, respectively. The mean concentrations of the sums of the nine PAHs and twelve NPAHs were highest in Shenyang and lowest in Fuzhou. In each city, more than 80% of the total PAHs and total NPAHs were found in the fine particulate fraction (<2.1 μm). All PAHs and NPAHs were clearly higher in the winter than in the summer. Furthermore, the ratio of the molar concentrations of 1-nitropyrene to pyrene ([1-NP]/[Pyr]), which is a suitable indicator to estimate the contribution of diesel-engine vehicles and coal combustion to urban TSP, were smaller in Shenyang in the winter. However, in Shanghai, Fuzhou and Shenyang (summer), the [1-NP]/[Pyr] ratios were close to those of particulates released from diesel-engine automobiles. Our study showed that the major contributors of atmospheric PAHs and NPAHs were diesel-engine vehicles both in the winter and the summer in Shanghai and Fuzhou, and in the summer in Shenyang. However, in the winter in Shenyang, atmospheric PAHs and NPAHs seemed to be affected by the mixture of coal combustion systems, such as coal heating and diesel-engine vehicles. 2010年の冬季及び夏季に中国の東部に位置する瀋陽，上海及び福州で総浮遊粒子状物質をアンダーセン式ローボリウムエアサンプラーを用いて粒径別（＜2.1 μm，2.1～7 μm，＞7 μm）に捕集した．強い発がん性または内分泌かく乱性を有する9種の多環芳香族炭化水素（PAH）と12種のニトロ多環芳香族炭化水素（NPAH）をそれぞれ高速液体クロマトグラフ（HPLC）蛍光検出法，HPLC化学発光検出法で分析した．その結果，3都市の大気中PAH，NPAH濃度はいずれも冬高夏低の季節変動を呈し，また季節によらず瀋陽で最も高く，福州で最も低いことが分かった．また3都市の大気中PAH，NPAHの80％ 以上は呼吸器への沈着率の高い微小粒子画分（＜2.1 μm）に存在した．さらに，大気中PAH，NPAHの主要発生源の識別マーカーであるピレンに対する1-ニトロピレン濃度比を3都市で比較した結果，上海，福州及び夏季の瀋陽の大気中PAH，NPAHの主要発生源がディーゼル車であり，冬季の瀋陽はディーゼル車と石炭暖房施設の両方であることが明らかになった．
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| 9.
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唐, 寧 ; 伊崎, 陽彦 ; 徳田, 貴裕 ; 季, 若男 ; 董, 麗君 ; 呉, 慶 ; 周, 志俊 ; 黄, 蓉 ; 林, 振宇 ; 亀田, 貴之 ; 鳥羽, 陽 ; 島, 正之 ; 早川, 和一
概要:
Urban air contains various kinds of organic pollutants. Among them, several polycyclic aromatic hydrocarbons (PAHs) and
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nitropolycyclic aromatic hydrocarbons (NPAHs) are carcinogenic and/or endocrine disrupting. PAHs and NPAHs in the atmosphere mainly originate from imperfect combustion of organic matter, such as petroleum and coal. In this study, total suspended particles (TSP) were collected in three different particulate size fractions by using Andersen low-volume air samplers in Shenyang, Shanghai and Fuzhou, China, in the winter and summer seasons in 2010. Nine PAHs and twelve NPAHs in the extracts from the TSP were analyzed by HPLC with fluorescence detection and chemiluminescence detection, respectively. The mean concentrations of the sums of the nine PAHs and twelve NPAHs were highest in Shenyang and lowest in Fuzhou. In each city, more than 80% of the total PAHs and total NPAHs were found in the fine particulate fraction (<2.1 μm). All PAHs and NPAHs were clearly higher in the winter than in the summer. Furthermore, the ratio of the molar concentrations of 1-nitropyrene to pyrene ([1-NP]/[Pyr]), which is a suitable indicator to estimate the contribution of diesel-engine vehicles and coal combustion to urban TSP, were smaller in Shenyang in the winter. However, in Shanghai, Fuzhou and Shenyang (summer), the [1-NP]/[Pyr] ratios were close to those of particulates released from diesel-engine automobiles. Our study showed that the major contributors of atmospheric PAHs and NPAHs were diesel-engine vehicles both in the winter and the summer in Shanghai and Fuzhou, and in the summer in Shenyang. However, in the winter in Shenyang, atmospheric PAHs and NPAHs seemed to be affected by the mixture of coal combustion systems, such as coal heating and diesel-engine vehicles. 2010年の冬季及び夏季に中国の東部に位置する瀋陽，上海及び福州で総浮遊粒子状物質をアンダーセン式ローボリウムエアサンプラーを用いて粒径別（＜2.1 μm，2.1～7 μm，＞7 μm）に捕集した．強い発がん性または内分泌かく乱性を有する9種の多環芳香族炭化水素（PAH）と12種のニトロ多環芳香族炭化水素（NPAH）をそれぞれ高速液体クロマトグラフ（HPLC）蛍光検出法，HPLC化学発光検出法で分析した．その結果，3都市の大気中PAH，NPAH濃度はいずれも冬高夏低の季節変動を呈し，また季節によらず瀋陽で最も高く，福州で最も低いことが分かった．また3都市の大気中PAH，NPAHの80％ 以上は呼吸器への沈着率の高い微小粒子画分（＜2.1 μm）に存在した．さらに，大気中PAH，NPAHの主要発生源の識別マーカーであるピレンに対する1-ニトロピレン濃度比を3都市で比較した結果，上海，福州及び夏季の瀋陽の大気中PAH，NPAHの主要発生源がディーゼル車であり，冬季の瀋陽はディーゼル車と石炭暖房施設の両方であることが明らかになった．
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| 10.
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亀田, 貴之 ; 片山, 裕規 ; 後藤, 知子 ; 鳥羽, 陽 ; 唐, 寧 ; 早川, 和一
概要:
A simple and sensitive method for measuring quinoid polycyclic aromatic hydrocarbons (PAHQs) in soluble organic fraction
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(SOF) of airborne particles based on two-dimensional high-performance liquid chromatography (HPLC) with fluorescence detection was established. The system involves a reversed phase column with naphtylethyl groups bonded silica packing material for sample clean-up, a 6-port switching valve, an ODS column for trapping the fraction containing PAHQs, a reversed phase column with cholesteryl groups bonded silica packing material for sample separation, and a Pt-Rh catalytic column for the reduction of PAHQs to a corresponding fluorescent compound. The accuracy of the assay, as applied to airborne particulate sample extracts spiked with known amounts of PAHQs were 91 – 107%. The detection limits were 19 to 2000 fmol per injection (signal-to-noise ratio = 3), and the calibration range was from 1 to 100 pmol with excellent proportionality (R2≥0.9992) for four kinds of PAHQs: benz[a]anthracene-7,12-dione, fluoranthene-2,3-dione, pyrene-1,6-dione, and pyrene-1,8-dione. PAHQs in SOF of airborne particles collected in Kyoto, Japan were successfully measured using the established analytical method with simple sample-preparation steps: ultrasonic extraction in organic solvent and concentration under reduced pressure and/or a nitrogen stream.
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