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| 1.
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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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| 2.
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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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| 3.
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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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| 4.
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岸田, 真男 ; 今村, 清 ; 亀田, 貴之 ; 早川, 和一 ; 坂東, 博
概要:
A determination method of atmospheric oxygenated polycyclic aromatic hydrocarbons (Oxy-PAHs) in particulate matter and t
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he gaseous phase using gas chromatograph (GC)-mass spectrometer (MS) was studied in the present study. First, we obtained fundamental data of GC-MS analyses (mass spectra and calibration curves) of twelve Oxy-PAHs as follows: acenaphthenequinone (AceQ), 1,4-naphtoquinone (1,4-NQ), 9-fluorenone (9-F-one), 1,4-phenanthrenequinone (1,4-PQ), 1,4-, 9,10-anthaquinone (1,4-, 9,10-AQ), 1-hydroxyanthrquinone (1-OHAQ), 1,2-benzanthraquinone (1,2-BAQ), benz[c]phenanthrene[1,4]quinine (BcP-1,4Q), 3,4-dihydrobenzo[a]anthracene-1(2H)-one (BaA-one), 1,4-chrysenequinone (1,4-CQ) and 9,10-dihydrobenzo[a]pyrene-7(8H)-one (BaP-one). Subsequently, to evaluate collection efficiency of Oxy-PAHs, air was passed through a quartz-fiber filter (QFF) spiked with authentic Oxy-PAHs and then through cleaned polyurethane form (PUF) plugs using a mini-pump or a low-volume air sampler for 24 h in the dark at a constant room temperature (20 or 35 °C). Oxy-PAHs retained on the QFF and those trapped within PUF plugs were simultaneously Soxhlet extracted, purified with silica by gel column chromatography and determined using GC-MS. The calibration curves for the determination of the twelve Oxy-PAHs were proportional in the concentration range between 0.02 and 1.0 μg/mL with r2 values of 0.960-0.999. Among the twelve Oxy-PAH compounds examined, recoveries of six compounds (1,4-NQ, 9-F-one, 9,10-AQ, 1,2-BAQ, BaA-one and BaP-one) during sampling, Soxhlet-extraction and clean-up procedures sufficiently yielded 79-127% at a room temperature of 20 °C and 57-127% at 35 °C . The method detection limits (MDLs) of the six compounds ranged between 0.61-1.07 ng/m3. The proposed method was applied to the determination of the six Oxy-PAH compounds in the atmosphere. Air sample was collected at an urban location of Osaka, Japan for 12-13 February 2007. 1,4-NQ, 9-F-one and 9-F-one were detected in the sample at concentration level of approximately 0.7-3 ng/m3.
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| 5.
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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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| 6.
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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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| 7.
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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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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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| 9.
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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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| 10.
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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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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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