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| 1.
論文 |
論文
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早川, 和一 ; Hayakawa, Kazuichi
概要:
(1)大気粉じんから変異原物質を抽出するために使用されている様々な有機溶媒の中から,ニトロアレーン分析法とAmes法の併用に最適な抽出溶媒の検索をおこなった.1,3-, 1,6-, 1,8-ジニトロピレン(DNP),1-ニトロピレン(NP)
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及び直接変異原性物質の抽出効率はベンゼン-エタノール(3:1),アセトニトリル,エタノール,メタノールの順で高く,毒性を考慮するとこれらの中ではエタノールが最も適していると考えられた. (2)基本ニトロアレーン分析計では試料の前処理として必要な還元操作を,分析システムに亜鉛を充填した還元用カラムを導入することにより省略した.また,分離度を向上させるため,試料を還元後,最も還元成績体の濃度が高い部分をスイッチングバルブでハードカッティングして,分析カラムに導入した.これによって簡単な前処理のみで大気粉じん中の1,3-, 1,6-, 1,8-DNP及び1-NPが定量可能となった. (3)ニトロアレーン分析法の前処理操作では直接変異原性ニトロアレーンと同時に間接変異原性多環芳香族炭化水素(PAH)も定量化に抽出される.この試料をニトロアレーン分析計とPAH分析のための蛍光検出HPLCシステムをスイッチングバルブで併合したシステムに適用することで,両者の同時分析が可能となった.その結果,上記の4種ニトロアレーンに加えて8種PAHも1時間以内に定量可能となった. (4)大気中で2次生成することが知られている2-, 4-NP,2-ニトロフルオランテン,6-ニトロクリセンと1-NPを同時に分析するため,基本ニトロアレーン分析システムに妨害物質を除去するための精製用ODSカラム,還元を自動化する亜鉛充填カラムと分離・検出を改善する濃縮用ODSカラムを導入した.本法によって測定した金沢市市街地大気中の上記化合物濃度は10^<-12>-10^<-16>molm^<-3>の範囲にあった.<br />(1) Both the nitroarene analyzer and the Ames test are necessary in the study on mutagenic nitroarenes. For the simultaneous use of these two methods, several solvent systems were tested to extract 1,3-dinitropyrene (1,3-DNP), 1,6-DNP,1,8-DNP and 1-nitropyrene (1-NP) as well as directacting mutagenic activity from airborne particulates. Benzene-ethanol, acetonitrile, ethanol and methanol gave the high efficiencies. Considering toxicities, ethanol seemed to be the best solvent.(2) Although the nitroarene analyzer determined trace levels of 1,3-, 1,6-and 1,8-DNPs and 1-NP in extracts from a few mg of airborne particulates, the reduction of nitroarenes to corresponding aminoarenes was required before injection. To remove this tedious treatment, a reducer column packed with zinc/glass beads was on-line introduced into the system. Considering the better resolution of aminoarenes, both the reducer column and a switching valve equipped with a heart-cutting loop were introduced just before the ODS separation column. This system could determine the above four compounds in extracts from airborne particulatates without pre-column reduction.(3) In the method, not only nitroarenes but also polycyclic aromatic hydrocarbons (PAHs) were quantitatively extracted from airborne partculates. To determine them simultaneously, both the nitroarene analyzer and a conventional high-performance liquid chromatograph with a fluorescence detector were combined using a switching valve. After the reduced sample solution was injected, four nitroarenes and eight PAHs were separately determined in the two different lines in 1h with high sensitivities.(4) Several mutagenic nitroarenes such as 2-, 4-NPs, 2-nitrofluoranthene and 6-nitrochrycene were formed in air in the presence of NOx. To determine these compounds, a reducer column packed with zinc/glass beads and two ODS columns, one for the clean-up and the other for the concentration, were introduced into the nitroarene analyzer. By the system, the above four compounds were detected in air. The fact that their ratios to 1,3-, 1,6-, 1,8-DNPs and 1-NP in rural air were larger than those in urban air suggested the formation of those compounds during the transportation. However, their mutagenic contributions were not large.<br />研究課題/領域番号:06557121, 研究期間(年度):1994–1995<br />出典：「ニトロアレーン分析計の試作」研究成果報告書 課題番号06557121(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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| 2.
論文 |
論文
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早川, 和一 ; Hayakawa, Kazuichi
概要:
(1)金沢市市街地の大気中1,3-,1,6-,1,8-ジニトロピレン(DNP)及び1-ニトロピレン(1-NP)の平均濃度は,それぞれfmol m^<-3>,サブpmol m^<-3>〜pmol m^<-3>レベルであった.これらの化合物濃度
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は,日中に高く夜間から早朝に低い日内変動を示し,交通量と高い相関が認められたことより,主要発生源は自動車と推定された.また,これらの化合物濃度は春から夏に低く,秋から冬に高い季節変動を示し,その要因の一つとして,前者には太陽光による光分解が,後者には逆転層による大気の安定が考えられた. (2)ガソリン車とディーゼル車の排ガス中DNP,1-NP濃度及び粉じん量を比較すると,DNP濃度は大差ないが,後者は前者に比べて1-NP濃度が遙かに高く,粉じん量も多い.これらに基づいて金沢市市街地の大気中DNP,1-NPについて発生源としてのディーゼル車の寄与率を求めると,それぞれ約90%,99%以上と試算された. (3)金沢市,東京都,札幌市の大気中DNP及び1-NP濃度には,都市の特徴によって多少の違いがあるものの,類似した日内及び季節変動が認められた.3都市の中では,札幌市がDNP濃度に対する1-NP濃度の比が最も大きく,その理由として,ガソリン車に対するディーゼル車の保有台数の割合が高いことが考えられた. (4)大気中1,3-,1,6-,1,8-DNP及び1-NP濃度推移と,Ames試験による大気直接変異原活性推移との相関は高く,上記化合物の大気直接変異原活性における寄与率は,YG1024株では約30%,TA98株では約10%と試算された.粒径別では,肺胞に沈積する割合の高い1.1μm以下の最微細粉じんに,化合物と変異原活性のいずれも最も多く分布していることが明らかとなった.大気変異原性に寄与するDNP,1-NP以外の化合物は,シリカゲルカラムクロマトグラフィーにより,DNPよりも低極性であると推定された.<br />(1) Each mean concentration of 1,3-dinitropyrene (1,3-DNP), 1,6-DNP,1,8-DNP and 1-nitropyrene (1-NP) in air in downtown Kanazawa were in the levels of fmol m^<-3> and sub pmol m^<33>-pmol m^<-3>, respectively. The concentrations were high in the daytime and low in the midnight and early in the morning. This diurnal variation gave a good correlation to the traffic volume, suggesting automobiles were the main contributors. The concentrations were high in spring and summer and low in autumn and winter. As reasons for this, degradation by sunlight in the former seasons and low atmospheric mixing dephts in the latter seasons were considered.(2) Concentrations of 1,3-, 1,6-and 1,8-DNPs and 1-NP in air in winter and summer in downtown Kanazawa, Sapporo and Tokyo were determined. Although the mean concentrations in Kanazawa were lower than those in Tokyo and Sapporo, there were similar tendencies as described above. The 1-NP to DNPs ratio in Sapporo was the largest in the three cities, suggest ing the largest diesel-engine vehicles to gasoline-engine vehicles ratio.(3) Concentrations of 1,3-, 1,6-and 1,8-DNPs in diesel Particulate were at the same levels as those in gasoline particulate. However, the concentration of 1-NP in diesel particulate was much higher than that in gasoline particulate. Considering the amount of particulates emitted from diesel-engine much larger than that of gasoline-engine, the contribution of diesel-engine vehicles to the amount of the above compounds in urban air was much larger than that of gasoline-engine vehicles.(4) In both diurnal and seasonal variation studies, good correlation coefficients were observed between the four concentrations and direct-acting mutagenic activities by the Ames test using three stains, TA98, YG1021 and YG1024. In the three, the YG1024 gave the largest coefficient. The contributions of the four compounds to the activities of air in YG1024 and TA98 strains were about 30% and 10%, respectively. The silica gel column chromatography suggested that the other contributors were less polar. When particulates were separately collected into five fractions of different particulate sizes, both the compounds and the activity were mainly contained in the finest particulate fraction (less than 1.1um) which was most adsorbed in alveoli of the lung.<br />研究課題/領域番号:06672138, 研究期間(年度):1994–1995<br />出典：「ニトロアレーンの環境動態解析とその軽減に関する基礎研究」研究成果報告書 課題番号06672138(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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