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| 1.
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論文
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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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| 2.
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論文
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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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| 3.
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論文
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早川, 和一
概要:
Many hazardous chemicals are absorbed into human body through respiration and have effects on human health. The 21st Century COE (center of excellence) "Environmental Monitoring and Prediction of Long- and Short-term Dynamics of
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Pan-Japan Sea Area-Construction of Monitoring Network and Assessment of Human Effects" (Leader : Kazuichi Hayakawa, Graduate School of Natural Science and Technology, Kanazawa University) concentrates on atmospheric pollution caused by human activities occurred in countries, Japan, China, Korea and Russia, surrounding Pan-Japan Sea as one of major projects. My talk focuses on atmospheric pollution caused by polycyclic aromatic hydrocarbon (PAH) and nitropolycyclic aromatic hydrocarbon (NPAH), which clearly exists in this area, and demonstrates the following aspects concerning this issue : 1) The 21st Century "Environmental Monitoring and Prediction of Long- and Short-term Dynamics of Pan-Japan Sea Area-Construction of Monitoring Network and Assessment of Human Effects," 2) Importance of PAH and NPAH as hazardous pollutants emitted from combustion of fossil fuels such as coal and oil, 3) Current status of atmospheric pollution of PAH and NPAH of Pan-Japan Sea Area, focusing on coal combustion systems such as heating in China and diesel-engine automobiles in Japan, and 4) Health effects of PAH and NPAH such as lung cancer and endocrine disruption.
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| 4.
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村橋, 毅 ; 早川, 和一 ; 岩本, 侑子 ; 宮崎, 元一
概要:
金沢大学医薬保健研究域薬学系<br />A simultaneous determination method for polycyclic aromatic hydrocarbons (PAHs) and nitro-PAHs (NPAH
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s) in airborne particulates was developed. Airborne particulates were extracted with benzene/ethanol, cleaned up by liquid-liquid partition, refluxed in the presence of NaSH and then the resultant solution was injected into an HPLC system. The system was hybridized into two systems with different optimum conditions for PAHs and NPAHs by introducing a switching valve and a mini separation column. Mobile phases were acetonitrile/water (75 : 25) for PAHs, and acetonitrile/imidazole HClO_4 buffer (1 : 1) for NPAHs and the postcolumn reagent solution for NPAHs was an acetonitrile solution containing bis(2,4,6-trichlorophenyl)oxalate and H_2O_2. By this method, four NPAHs (1,3-, 1,6-, 1,8-dinitropyrenes and 1-nitropyrene) and eight PAHs (fluoranthene, pyrene, benz[a]anthracene, chrysene, benzo[b]fluoranthene, benzo[k]fluoranthene, benzo[a]pyrene and coronene) in sub-milligram quantities of airborne particulates were determined chemilumigenically and fluorogenically, respectively using 2-fluoro-7-nitrofluorene as an internal standard within sixty minutes.
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| 5.
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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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| 6.
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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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| 7.
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早川, 和一 ; Hayakawa, Kazuichi
概要:
環日本海域の7都市,瀋陽(中国),ウラジオストク(ロシア),ソウル(韓国),北九州,金沢,東京,札幌(日本)で,冬及び夏に大気粉塵を捕集した。更に,家庭石炭燃焼ストーブ排出粉塵及びディーゼル車排出粉塵も捕集した。粉塵抽出物について,多環芳香
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族炭化水素9種類(フルオランテン,ピレン,ベンツ[a]アントラセン,クリセン,ベンゾ[b]フルオランテン,ベンゾ[k]フルオランテン,ベンゾ[a]ピレン,ベンゾ[ghi]ペリレン,インデノ[1,2,3-cd]ピレン)とニトロ多環芳香族炭化水素4種類(1,3-,1,6-,1,8-ジニトロピレン,1-ニトロピレン)を,それぞれ蛍光,化学発光検出HPLCで測定した。瀋陽とウラジオストクの平均大気中多環芳香族炭化水素濃度はソウル,北九州,金沢,東京,札幌より著しく高かったが,平均大気中ニトロ多環芳香族炭化水素濃度は北九州以外を除くと同レベルであった。いずれの都市でも多環芳香族炭化水素とニトロ多環芳香族炭化水素濃度には明確な季節変動(冬>夏)が見られた。各都市の多環芳香族炭化水素とニトロ多環芳香族炭化水素の発生源を明らかにする為に,クラスター分析及び因子分析を行った結果,3つの主要クラスターが見出された。更に,瀋陽とウラジオストク,北九州のピレンに対する1-ニトロピレンの濃度比は石炭燃焼ストーブ排出粉塵のそれに近似し,ソウル,金沢,東京,札幌の値はディーゼル車排出粉塵のそれに近似していた。本研究は,ピレンに対する1-ニトロピレンの濃度比が,都市大気粉塵の発生源である石炭燃焼システムとディーゼル車の指標として有用なことを示している。<br />Airborne particulates were collected in seven cities in the Pan-Japan Sea countries, Shenyang (China), Vladivostok (Russia), Seoul (South Korea), Kitakyushu, Kanazawa, Tokyo and Sapporo (Japan), in winter and summer. In addition, particulates from domestic coal-burning stoves and particulates from diesel-engine automobiles were collected. Nine polycyclic aromatic hydrocarbons (PAHs), fluoranthene, pyrene (Pyx), benz[a]anthracene, chrysene, benzo[b]fluoranthene, benzo[k]fluoranthene, benzo[a]pyrene, benzo[ghi]perylene and indeno[1,2,3-cd]pyrene, and four nitropolycyclic aromatic hydrocarbons (NPAHs), 1,3-, 1,6-, 1,8-dinitropyrenes, and 1-nitropyrenes (1-Np) in the extracts from the particulates were analyzed by HPLC with fluorescence and chemiluminescence defections, respectively. The mean atmospheric concentrations of PAHs in Shenyang and Vladivostok were substantially higher than those in Seoul, Tokyo, Sapporo, Kitakyushu and Kanazawa. However, the mean atmospheric concentrations of NPAHs were at the same levels in every city except for Kitakyushu. Obvious seasonal variations (winter > summer) in the PAR and NPAH concentrations were observed in each city. In order to study the major contributors of atmospheric PAHs and NPAHs in these cities, cluster analysis and factor analysis were used and three large clusters were identified. Furthermore, the concentration ratios of 1-Np to Pyr were significantly smaller in Shenyang, Vladivostok and Kitakyushu and the values were close to those of particulates in the exhaust from coal stoves. However, the ratios were larger in Seoul, Kanazawa, Tokyo and Sapporo and the values were close to those of particulates in the exhaust from diesel-engine automobiles. Our results show that the concentration ratio of 1-Np to Pyr is an useful indicator of the contributions made by diesel-engine vehicles and coal combustion systems to particulates in urban air.<br />研究課題/領域番号:15406001, 研究期間(年度):2003–2004<br />出典：「環日本海都市の多環芳香族炭化水素/ニトロ多環芳香族炭化水素の発生と曝露の国際比較」研究成果報告書 課題番号15406001 (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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