Impact of Criegee Intermediate Reactions with Peroxy Radicals on Tropospheric Organic Aerosol

被引：26

作者：

Chhantyal-Pun, Rabi ^{[1
]}

Khan, M. Anwar H. ^{[1
]}

Zachhuber, Nicholas ^{[1
]}

Percival, Carl J. ^{[2
]}

Shallcross, Dudley E. ^{[1
]}

Orr-Ewing, Andrew J. ^{[1
]}

机构：

[1] Univ Bristol, Sch Chem, Bristol BS8 1TS, Avon, England

[2] CALTECH, Jet Prop Lab, Pasadena, CA USA

来源：

ACS EARTH AND SPACE CHEMISTRY | 2020年 / 4卷 / 10期

基金：

英国自然环境研究理事会; 美国国家航空航天局;

关键词：

atmospheric chemistry; Criegee intermediates; peroxy radicals; radical reactions; secondary organic aerosol; cavity ring-down spectroscopy; chemical transport modeling; GAS-PHASE OZONOLYSIS; DIRECT KINETIC MEASUREMENTS; PURE COMPONENT PROPERTIES; CRI MECHANISM; MONOTERPENE OZONOLYSIS; TEMPERATURE-DEPENDENCE; ATMOSPHERIC CHEMISTRY; PHOTOCHEMICAL DATA; GLOBAL CHEMISTRY; POTENTIAL SOURCE;

D O I：

10.1021/acsearthspacechem.0c00147

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Peroxy radicals and carbonyl oxides (Criegee intermediates) are produced in the troposphere during OH and ozone-initiated oxidation of hydrocarbons. Reactions between these species have previously been shown to form highly oxidized molecules which can condense to form secondary organic aerosols. Here, cavity ring-down spectroscopy coupled with laser flash photolysis was used to measure directly rate coefficients for reactions of CH2OO with CH3O2 and CH3C(O)O-2. The rate coefficients were found to be similar within the measurement uncertainties and only weakly dependent on temperature (in the range 243-310 K) and pressure (20-100 Torr, N-2). A combined rate coefficient of k (CH2OO + RO2, RO2 = CH3O2/CH3C(O)O-2) = (2.4 +/- 1.2) x 10(-11) cm(3) molecule(-1) s(-1) was obtained under these conditions. Global modeling using STOCHEM-CRI, updated with monoterpene chemistry generating Criegee intermediates and supplemented by regional box modeling, shows that this class of Criegee intermediate + peroxy radical reactions can contribute up to similar to 1.3% of secondary organic aerosol production in forested regions of the world.

引用

页码：1743 / 1755

页数：13

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