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DOI | 10.5194/acp-17-15137-2017 |
Temperature-dependent rate coefficients for the reactions of the hydroxyl radical with the atmospheric biogenics isoprene, alpha-pinene and delta-3-carene | |
Dillon, Terry J.1,2; Dulitz, Katrin1,3; Gross, Christoph B. M.1; Crowley, John N.1 | |
2017-12-21 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2017 |
卷号 | 17期号:24 |
文章类型 | Article |
语种 | 英语 |
国家 | Germany; England |
英文摘要 | Pulsed laser methods for OH generation and detection were used to study atmospheric degradation reactions for three important biogenic gases: OH + isoprene (Reaction R1), OH + alpha-pinene (Reaction R2) and OH+Delta-3-carene (Reaction R3). Gas-phase rate coefficients were characterized by non-Arrhenius kinetics for all three reactions. For (R1), k(1) (241-356 K) = (1.93 +/- 0.08) 10(-11) exp{(466 +/- 12)/T} cm(3) molecule(-1)s(-1) was determined, with a room temperature value of k(1) (297 K) = 9.3 +/- 0.4) x 10(-11) cm(3) molecule(-1) s(-1), independent of bath-gas pressure (5-200 Torr) and composition (M = N-2 or air). Accuracy and precision were enhanced by online optical monitoring of isoprene, with absolute concentrations obtained via an absorption cross section, sigma(isoprene) = (1.28 +/- 0.06) x 10(-17) cm(2) molecule(-1) at lambda = 184.95 nm, determined in this work. These results indicate that significant discrepancies between previous absolute and relative-rate determinations of k(1) result in part from sigma values used to derive the isoprene concentration in high-precision absolute determinations. Similar methods were used to determine rate coefficients (in 10(-11) cm(3) molecule(-1) s(-1)) for (R2)-(R3): k(2) (238-357 K) = 1.83 +/- 0.04) x exp{(330 +/- 6)/T} and k(3) (235-357 K) = 2.48 +/- 0.14) x exp{(357 +/- 17)/T}. This is the first temperature-dependent dataset for (R3) and enables the calculation of reliable atmospheric lifetimes with respect to OH removal for e.g. boreal forest springtime conditions. Room temperature values of k(2) (296 K) = 5.4 +/- 0.2) x 10(11) cm(3) molecule(-1) s(-1) and k(3) (297 K) = 8.1 +/- 0.3) x 10(-11) cm(3) molecule(-1) s(-1) were independent of bath-gas pressure (7-200 Torr, N2 or air) and in good agreement with previously reported values. In the course of this work, 184.95 nm absorption cross sections were determined: sigma = 1.54 +/- 0.08) x 10(-17) cm(2) molecule(-1) for sigma-pinene and (2.40 +/- 0.12) x 10(-17) cm(2) molecule(-1) for Delta-3-carene. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000418423900003 |
WOS关键词 | VOLATILE ORGANIC-COMPOUNDS ; GAS-PHASE REACTIONS ; RATE CONSTANTS ; RAIN-FOREST ; TROPICAL TROPOSPHERE ; INITIATED OXIDATION ; BOREAL FOREST ; OH ; KINETICS ; CHEMISTRY |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; 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/30705 |
专题 | 地球科学 |
作者单位 | 1.Max Planck Inst Chem, Dept Air Chem, D-55128 Mainz, Germany; 2.Univ York, Dept Chem, Wolfson Atmospher Chem Labs, York YO10 5DD, N Yorkshire, England; 3.Univ Freiburg, Phys Inst, Hermann Herder Str 3, D-79104 Freiburg, Germany |
推荐引用方式 GB/T 7714 | Dillon, Terry J.,Dulitz, Katrin,Gross, Christoph B. M.,et al. Temperature-dependent rate coefficients for the reactions of the hydroxyl radical with the atmospheric biogenics isoprene, alpha-pinene and delta-3-carene[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2017,17(24). |
APA | Dillon, Terry J.,Dulitz, Katrin,Gross, Christoph B. M.,&Crowley, John N..(2017).Temperature-dependent rate coefficients for the reactions of the hydroxyl radical with the atmospheric biogenics isoprene, alpha-pinene and delta-3-carene.ATMOSPHERIC CHEMISTRY AND PHYSICS,17(24). |
MLA | Dillon, Terry J.,et al."Temperature-dependent rate coefficients for the reactions of the hydroxyl radical with the atmospheric biogenics isoprene, alpha-pinene and delta-3-carene".ATMOSPHERIC CHEMISTRY AND PHYSICS 17.24(2017). |
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