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| 1.
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小村, 和久 ; 稲垣, 美幸 ; 西川, 方敏 ; 中西, 孝 ; 早川, 和一 ; 唐, 寧 ; 楊, 小陽 ; 飯田, 孝夫 ; 森泉, 純 ; Komura, Kazuhisa ; Inagaki, Miyuki ; Nishikawa, Katatoshi ; Hayakawa, Kazuichi ; Tang, Ning ; Yang, Xiaoyang ; Iida, Takao ; Moriizumi, Jyun
概要:
金沢大学環日本海域環境研究センター<br />Variations of radiation levels before and after the Noto Hanto Earthquake in 2007 have been analy
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zed from the point of view of environmental radioactivity. The 210Pb activities in the airborne particles are collected from Nishi-Futamata in Wajima, are analyzed. The Radon activity at Hegura Island located 50km North of Wajima, and the spatial gamma rays at Nishi-Futamata are measured since April 21, 2007. Abnormal increase of 210Pb activity started 3 weeks before the earthquake are found, suggesting the maximum value just before the earthquake, because it decrease to normal level after 2 weeks. Increase of radon level was not observed at Hegura Island, however, increase of radiation level at Nishi-Futamata area continued for 6 weeks after the earthquake, and settled to normal level in middle of May 2007.<br />環境放射能の観点から能登半島地震発生前後の放射能関連のデータの解析を試みた.解析したのは,輪島市西二又地区で採取した大気浮遊塵中の210Pb,輪島沖50kmに位置する舳倉島のラドン濃度,地震発生後の4月21日から西二又地区で連続測定を実施した空間γ線レベルの3項目である.その結果,地震発生約3週間前から大気浮遊塵試料のラドンの娘核種210Pbの濃度が増加し,地震直前にピークに達した後に低下に転じ,約2週間後にほぼ平常値に回復していたことが分かった.舳倉島のラドンには地震の影響は見られなかったが,西二又における空間γ線レベルはラドンに由来すると考えれる高い値が約6週間後も続き5月中頃に平常値に戻ったことが明らかになった.
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| 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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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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| 8.
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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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鳥羽, 陽 ; 本間, 千春 ; 宇於崎, 和香 ; Chuesaard, Thanyarat ; 唐, 寧 ; 早川, 和一
概要:
A high-performance liquid chromatographic (HPLC) method with fluorescence detection was developed for the quantification
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of polycyclic aromatic hydrocarbons (PAHs) in cigarette mainstream and sidestream smoke particulates. Fifteen kinds of PAHs classified as priority pollutants by the US EPA were quantified with six perdeuterated PAHs as internal standards. The smoke filter samples obtained from 3 brands of cigarettes using standardized smoking conditions were extracted with dichloromethane, and then treated with tandem solid phase extraction cartridges (Silica and Neutral Alumina). The limits of detection ranged from 0.24 to 2.2 pg, and were more sensitive than those by GC-MS. The analytes were quantified by using the internal standards, and the developed method achieved sufficient reproducibility and accuracy. The PAH levels in mainstream and sidestream smoke from 3 cigarette brands were in the range of 0.2 – 305 ng cigarette−1 and 26.4 – 6160 ng cigarette−1, respectively. The total PAH content in sidestream smoke was more than 10 times higher compared with that of mainstream smoke. This method should be useful as an optional analytical method to quantify PAHs in cigarette smoke particulates.
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| 12.
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戸次, 加奈江 ; 鳥羽, 陽 ; 唐, 寧 ; 亀田, 貴之 ; 滝上, 英孝 ; 鈴木, 剛 ; 早川, 和一
概要:
Polycyclic aromatic hydrocarbons (PAHs), some of which are carcinogenic/mutagenic, are generated by combustion of fossil fuels and also released through tanker or oilfield accident to cause a large scale
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environmental pollution. PAHs concentration in China is especially high in East Asia because of many kinds of generation sources such as coal heating systems, vehicles and factories without exhaust gas/particulate treatment systems. So, the atmospheric pollution caused by PAHs in China has been seriously concerned from the view point of health effects. Like yellow sand and sulfur oxide, PAHs exhausted in China are also transported to Japan. Additionally, strongly mutagenic nitrated PAHs (NPAHs), estrogenic/antiestrogenic PAH hydroxides (PAHOHs) and reactive oxygen species-producing PAH quinones (PAHQs) are formed from PAHs by the chemical reaction during the transport. Furthermore these PAHOHs and PAHQs are produced by the metabolism in animal body. In the biological activities caused by the above PAH derivatives, the structure-activity relationship was observed. In this review, our recent results on the generation of PAH derivatives by atmospheric transport and metabolism are reported. Also, the existing condition of PAHs as atmospheric pollutants is considered.
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| 13.
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柿本, 健作 ; 東條, 俊樹 ; 先山, 孝則 ; 永吉, 晴奈 ; 小西, 良昌 ; 梶村, 計志 ; 中野, 武 ; 畑, 光彦 ; 古内, 正美 ; 唐, 寧 ; 早川, 和一 ; 鳥羽, 陽
概要:
The particle size distributions of dechloranes were determined. For collecting PM, an Andersen air sampler equipped with
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five-stage quartz fiber filters and a PM0.1 air sampler equipped with six-stage Teflon and inertial SUS fiber filters were used. Particulate matter (PM) was collected in April 2014 by Andersen air sampler and October 2014 and January 2015 by PM0.1 air sampler. The samples were analyzed for Dechlorane Plus (DP), Dechlorane602, Dechlorane603, and Dechlorane604 Component A using gas chromatography high-resolution mass spectrometry. The almost all nanoparticles smaller than 100 nm are reported to reach and deposit in lung periphery, so it is important to reveal the concentration of these dechloranes in nanoparticles. In our study, only DP was detected in PM. DP was detected from all the filter samples. In this study, the particle size distribution of DP was revealed for the first time and the approximately 70 ％ of DP exist in ＜2.5 µm fractions and 10 ％ of DP exist in ＜0.1 µm fractions of PM samples.
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| 14.
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玉村, 修司 ; 佐藤, 努 ; 大田, 由貴恵 ; 唐, 寧 ; 早川, 和一 ; 米田, 哲朗
概要:
金沢大学大学院自然科学研究科環境動態<br />金沢大学薬学部
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| 15.
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早川, 和一 ; 鳥羽, 陽 ; 亀田, 貴之 ; 唐, 寧
概要:
金沢大学医薬保健研究域薬学系<br />化石燃料の消費量の増加は,大気中に大量の汚染物質を排出し,深刻な健康影響を招いている。有害大気汚染物質の一つに多環芳香族炭化水素(PAH)とニトロ多環芳香族炭化水素(NPAH)がある.このうち,NPA
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Hは極めて強い変異原性を有するものがあるにもかかわらず,環境中の濃度はPAHよりはるかに低く,しかもNPAHを追跡できる高感度な分析法もなかったため,PAHに比較するとNPAHの環境動態や健康影響に関する研究は大きく立ち遅れていた.本総説では,1980年代の後半から始まった高感度なNPAH分析法の開発研究を解説し,更にそれを用いて急速に展開しているNPAHの発生と大気内動態の解析,並びにヒト暴露測定について最近の動向までを解説する. With an increase in the consumption of fossil fuels, large amounts of pollutants released into the atmosphere cause serious health problems. Polycyclic aromatic hydrocarbons (PAHs) and nitropolycyclic aromatic hydrocarbons (NPAHs) are among the atmospheric hazardous pollutants. The mutagenicities of several NPAHs are much stronger than those of PAHs, but the concentrations of NPAHs are much lower than those of PAHs in the environment. However, the progress of studies on the environmental behaviors and health effects of NPAHs has been much slower than that of PAHs, because of the lack of a sensitive analytical method available for trace NPAHs. This review deals with the development of sensitive determination methods for NPAHs starting the in late 1980s and recent studies on the contributors and atmospheric behaviors of NPAHs and human exposure to them.
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| 16.
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鈴木, 元気 ; 森川, 多津子 ; 柏倉, 桐子 ; 唐, 寧 ; 鳥羽, 陽 ; 早川, 和一
概要:
首都圏3地点(野毛、九段、つくば)において、野毛および九段では2006～2013年まで、つくばでは2010～2013年までの夏と冬の大気粉塵を捕集し、多環芳香族炭化水素 (PAH) 9種類およびニトロ多環芳香族炭化水素 (NPAH) 3種類
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をそれぞれHPLC-蛍光検出法、HPLC-化学発光検出法で測定し、その濃度の変遷を明らかにした。PAH濃度は野毛、九段で2006年から2008年の間の冬に低下傾向が認められた。NPAH濃度は、野毛では2006年から2011年の間の夏と冬、九段では2007年から2009年の間の夏および2006年から2011年の間の冬に低下傾向が認められた。つくばでは観測期間が2010年から2013年と短く、PAHとNPAHのいずれについても明確な変動傾向は認められなかった。また野毛および九段で[1-NP]/[Pyr]値の低下が確認され、PAH、NPAH濃度低下の要因の一つとして自動車排ガス規制による粉塵およびNOx排出量の減少が考えられた。 Airborne particulates were collected in Noge and Kudan, Japan, in the summer and winter from 2006 to 2013 and in Tsukuba, Japan, in the summer and winter from 2010 to 2013. The polycyclic aromatic hydrocarbons (PAHs) and nitropolycyclic aromatic hydrocarbons (NPAHs) were determined by HPLC with fluorescence and chemiluminescence detections, respectively. The decreasing tendencies of the total concentrations of nine PAHs were observed at Noge and Kudan in the winter from 2006 to 2008. The decreasing tendencies of the total concentrations of three NPAHs were observed in both the summer and winter in Noge from 2006 to 2011. The decreasing tendencies of the NPAH concentrations were also observed in Kudan in the winter from 2006 to 2011 and in the summer from 2007 to 2009. The concentration ratio of 1-nitropyrene to pyrene also decreased in Noge and Kudan. As the main reason for the decrease in the urban atmospheric PAH and NPAH concentrations, the Japanese regulation of exhaust gas/particulates from automobiles was considered.
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| 17.
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浜, 寛貴 ; 徳田, 貴裕 ; 伊崎, 陽彦 ; 大野, 友子 ; 渡辺, 有梨 ; 神田, 哲雄 ; 唐, 寧 ; 亀田, 貴之 ; 鳥羽, 陽 ; 早川, 和一
概要:
石川県金沢市藤江の幹線道路脇において12年間（1999～2010年）の夏と冬の大気粉塵を捕集し、多環芳香族炭化水素（PAH）6種類（pyrene、benz[a]anthracene、chrysene、benzo[b]fluoranthene
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、benzo[k]fluoranthene、benzo[a]pyrene）およびニトロ多環芳香族炭化水素（NPAH）7種類（1,3-、1,6-、1,8-dinitropyrenes、1-nitropyrene、6-nitrochrysene、7-nitrobenz[a]anthracene、6-nitrobenzo[a]pyrene）をそれぞれHPLC-蛍光検出法、HPLC-化学発光検出法で測定し、その変遷を明らかにした。この間に、PAH濃度は冬63.9％、夏75.6％減少、NPAH濃度は冬88.0％、夏89.2％減少した。また[1-NP]/[Pyr]値は冬と夏ともに著しく減少した。自動車排ガス規制の強化によって排出源としての自動車の寄与率が低下したことが、大気中PAH、NPAH濃度および[1-NP]/[Pyr]値が顕著に減少した主要因と考えられた。 Airborne particulates were collected at a roadside site in Kanazawa, Japan, in the summer and winter, 1999, 2004/2005, 2007/2008 and 2010. The polycyclic aromatic hydrocarbons (PAHs) and nitropolycyclic aromatic hydrocarbons (NPAHs) were determined by HPLC with fluorescence and chemiluminescence detections, respectively. The total concentration of six PAHs (pyrene, benz[a]anthracene, chrysene, benzo[b]fluoranthene, benzo[k]fluoranthene and benzo[a]pyrene) decreased by the factor of 63.9% in the winter and 75.6% in the summer from 1999 to 2010. The total concentration of seven NPAHs (1,3-, 1,6-, 1,8-dinitropyrenes, 1-nitropyrene, 6-nitrochrysene, 7-nitrobenz[a]anthracene and 6-nitrobenzo[a]pyrene) significantly decreased by the factor of 88.0% in the winter and 89.2% in the summer during the same period. The concentration ratio of 1-nitropyrene to pyrene also significantly decreased in this period, suggesting a decrease in the emission amount. As the main reason for the significant decrease in the PAHs and NPAHs, the regulation of exhaust gas/particulates from automobiles was considered.
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| 18.
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片山, 裕規 ; 後藤, 知子 ; 亀田, 貴之 ; 唐, 寧 ; 松木, 篤 ; 鳥羽, 陽 ; 早川, 和一
概要:
本研究では，日本および近年大気汚染の著しい中国における大気中多環芳香族炭化水素（PAH）キノン濃度レベルを把握すること，さらに大気内動態を解明するための基礎的なデータを得ることを目的とし，PAHキノンの一種である1,2-benzanthra
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quinone（benz[a]anthracene-7,12-dione; BAQ）の実大気中観測，ならびに光やオゾンによるPAHの酸化反応によるBAQの生成を実験的に検討した。北京，大阪，輪島における実大気粒子中BAQ濃度を測定したところ，最も高かった北京・冬の濃度は，輪島・冬の濃度の約200倍高い値を示した。またBAQ/benzo[k]fluoranthene（BkF）濃度比を比較したところ，いずれの地点においても夏季のほうが冬季よりも低いという結果を得た。夏季には強い太陽光強度の影響により，BAQの光分解がBkFの光分解以上に促進され，BAQ/BkF比が小さくなったものと考えられた。北京で大規模な黄砂が観測された時期においては，黄砂のほとんど観測されなかった春季よりもBAQ/BkF比は高い値となった。室内反応実験により，中国砂漠土壌粒子表面に担持させたBaAからのBAQ生成を，光照射およびオゾンとの反応によって調べたところ，参照とするグラファイト粒子，およびテフロン粒子よりも土壌粒子表面において反応が促進される傾向があることがわかった。このことから，黄砂期にBAQ/BkF比が高くなる理由の一つとして，黄砂表面上におけるBAQの二次生成が示唆された。 Selected polycyclic aromatic hydrocarbons (PAH), nitrated PAH, and quinoid PAH (PAH-quinone) in airborne particles were simultaneously determined at Beijing, China, Osaka, Japan, and Wajima, Japan. The concentration of particle-associated 1,2-benzanthraquinone (benz[a]anthracene-7,12-dione; BAQ), a quinoid PAH, at Beijing was higher than that at Osaka and Wajima by factors of 35 and 200, respectively. Strong correlations between the BAQ and 2-nitropyrene concentrations in the summer and between the BAQ and 1-nitropyrene concentrations in the winter imply that atmospheric secondary reactions and primary emissions significantly contribute to the occurrence of atmospheric BAQ in the summer and winter, respectively. The concentration ratios of BAQ to benz[k]fluoranthene (BkF) in the summer were lower than those in the winter due to the instability of BAQ under sunlight. The BAQ/BkF ratio at Beijing in the Asian dust season was significantly higher than that in the regular spring season, suggesting that the secondary formation of BAQ is promoted by catalytic effects on the Asian dust surface.
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| 19.
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唐, 寧 ; 小操, 征司 ; 渡辺, 有梨 ; 田畑, 勝弘 ; 鳥羽, 陽 ; 木津, 良一 ; 早川, 和一
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| 20.
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早川, 和一 ; 唐, 寧 ; 木津, 良一
概要:
Kizu, Ryouichi<br />金沢大学自然科学研究科<br />金沢大学薬学部
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