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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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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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| 4.
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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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| 5.
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論文
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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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| 6.
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論文
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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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| 7.
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早川, 和一 ; Hayakawa, Kazuichi
概要:
ディーゼル排出粉塵(DEPE)及びその構成成分の一つである多環芳香族炭化水素(PAH)類の内分泌攪乱作用について,昨年度はエストロゲン様/抗エストロゲン活性を明らかにした.今年度はDEPE及びPAHのアンドロゲン様活性/抗アンドロゲン活性に
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ついて検討した。DEPEをヒトPC3/AR培養細胞を用いたルシフェラーゼレポーターアッセイに適用した結果,アンドロゲン様活性は認められなかったが,抗アンドロゲン活性が観察された。DEPEに含まれるいくつかの4,5環PAHは,強い抗アンドロゲン活性を示した。また,DEPE及び4,5環PAHはいずれも,ヒトのアリルヒドロカーボンレセプター(AhR)のアゴニストであった。以上の結果から,DEPEは抗アンドロゲン活性を示し,その一部はDEPEに含まれるPAHに由来することがわかった。更に,酵母two-hybrid法を用いた結果,DEPE及びいくつかのニトロ多環芳香族炭化水素が抗アンドロゲン活性を示した。次に,分析対象のモノヒドロキシ多環芳香族炭化水素(OHPAH)の数を増加させるために,逆相HPLC/蛍光検出法の条件を改良した。また,ヒト尿試料に適用可能とするために,OHPAHの抱合体も加水分解してOHPAHと合わせて定量する前処理方法を開発した。その結果,喫煙者は非喫煙者に比較して尿中2-ヒドロキシフルオレン濃度が有為に高く,1-ヒドロキシピレンより有効な喫煙指標となることがわかった。また,2〜4環の複数のOHPAHを同時分析した結果,タイ人は日本人に比較して尿中の各種OHPAH濃度が高く,室内で使用する薪燃料由来の煙の影響が大きいと推定された。このように,開発したOHPAH分析法は,ガス状及び粒子状のいずれのPAHの代謝物も分析対象としており,異なる多様なPAH発生源にも対応できることから,ヒトのPAH個人曝露量評価法として有用なことがわかった。<br />Last year, both estrogenic and antiestrogenic actions of diesel exhaust particulate(DEPE) and polycyclic aromatic hydrocarbon(PAH), which was one of the constituent of DEPE, were clarified. This year, both androgenic and antiandrogenic activities of DEPE and PAH were examined. By applying DEPE to the luciferase reporter gene assay in human PC3/AR culture cells, DEPE did not show androgenic activity but antiestrogenic activity. Several PAHs having 4 or 5 rings, which are included in DEPE, showed strong antiandrogenic activity. Both DEPE and PAHs having 4 or 5 rings, were also agonists of human allyl hydrocarbon receptor(AhR). These results suggested that DEPE showed antiandrogenic activity and that a part of this activity was derived from PAHs which were included in DEPE. In addition, several nitropolycyclic aromatic hydrocarbons showed aniandorgenic activity in the yeast two-hybrid assay. Next, to increase the number of monohydroxy polycyelic aromatic hydrocarbons(OHPAH) as analytes, conditions of our HPLC/fluorimetric detection method were modified. And, to anayze both urinary OHPAHs and their conjugates, the pretreatment method including hydrolysis of the conjugates was developed. As the result, the urinary concentration of 2-hydroxyfluorene in smokers' urine samples was higher than that in nonsmokers', and it was proven that 2-hydroxyfluorene was a more effective biomarker for smoking than 1-hydroxypyrene. Urinary OHPAH concentrations of Thai subjects were higher than those of Japanese. As a possible reason for this, the smoke of the firewood fuel used in the indoor of Thai house was considered.<br />研究課題/領域番号:14370728, 研究期間(年度):2002–2003<br />出典：「多環芳香族炭化水素とその代謝物の内分泌撹乱作用とその測定法に関する研究」研究成果報告書 課題番号14370728 (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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