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DOI | 10.1002/2017JD026950 |
Temperature dependence of stable carbon kinetic isotope effect for the oxidation reaction of ethane by OH radicals: Experimental and theoretical studies | |
Piansawan, T.1; Saccon, M.2; Vereecken, L.1; Gensch, I.1; Kiendler-Scharr, A.1 | |
2017-08-16 | |
发表期刊 | JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES |
ISSN | 2169-897X |
EISSN | 2169-8996 |
出版年 | 2017 |
卷号 | 122期号:15 |
文章类型 | Article |
语种 | 英语 |
国家 | Germany; Canada |
英文摘要 | The stable carbon kinetic isotope effect (KIE) of ethane photooxidation by OH radicals was deduced by employing both laboratory measurements and theoretical calculations. The investigations were designed to elucidate the temperature dependence of KIE within atmospherically relevant temperature range. The experimental KIE was derived from laboratory compound-specific isotope analyses of ethane with natural isotopic abundance exposed to OH at constant temperature, showing epsilon values of 7.160.54 (303K), 7.450.48 (288K), 7.36 +/- 0.28 parts per thousand (273K), 7.61 +/- 0.28 parts per thousand (263K), 8.89 +/- 0.90 parts per thousand (253K), and 9.42 +/- 2.19 parts per thousand (243K). Compared to previous studies, a significant improvement of the measurement precision was reached at the high end of the investigated temperature range. The KIE was theoretically determined as well, in the temperature range of 150K to 400K, by calculating the reaction rate coefficients of C-12 and singly C-13 substituted ethane isotopologues applying chemical quantum mechanics together with transition state theory. Tunneling effect and internal rotations were also considered. The agreement between experimental and theoretical results for rate coefficients and KIE in an atmospherically relevant temperature range is discussed. However, both laboratory observations and computational predictions show no significant temperature dependence of the KIE for the ethane oxidation by OH radicals. |
英文关键词 | kinetic isotope effects isotope fractionation stable carbon isotope ratio ethane oxidation quantum chemistry transition state theory |
领域 | 气候变化 |
收录类别 | SCI-E |
WOS记录号 | WOS:000408349500036 |
WOS关键词 | TRANSITION-STATE THEORY ; VOLATILE ORGANIC-COMPOUNDS ; WESTERN NORTH PACIFIC ; REACTION-RATE CONSTANTS ; GAS-PHASE REACTIONS ; AB-INITIO ; TUNNELING CALCULATIONS ; ATMOSPHERIC CHEMISTRY ; NONSEPARABLE SYSTEMS ; LIGHT-HYDROCARBONS |
WOS类目 | Meteorology & Atmospheric Sciences |
WOS研究方向 | Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/33048 |
专题 | 气候变化 |
作者单位 | 1.Forschungszentrum Julich, Inst Energy & Climate Res IEK 8, Julich, Germany; 2.York Univ, Ctr Atmospher Chem, Toronto, ON, Canada |
推荐引用方式 GB/T 7714 | Piansawan, T.,Saccon, M.,Vereecken, L.,et al. Temperature dependence of stable carbon kinetic isotope effect for the oxidation reaction of ethane by OH radicals: Experimental and theoretical studies[J]. JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES,2017,122(15). |
APA | Piansawan, T.,Saccon, M.,Vereecken, L.,Gensch, I.,&Kiendler-Scharr, A..(2017).Temperature dependence of stable carbon kinetic isotope effect for the oxidation reaction of ethane by OH radicals: Experimental and theoretical studies.JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES,122(15). |
MLA | Piansawan, T.,et al."Temperature dependence of stable carbon kinetic isotope effect for the oxidation reaction of ethane by OH radicals: Experimental and theoretical studies".JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES 122.15(2017). |
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