Chemical Kinetic Study of the Reaction of CH2OO with CH3O2

被引：3

作者：

Chao, Wen ^{[1
]}

Markus, Charles R. ^{[2
]}

Okumura, Mitchio ^{[1
]}

Winiberg, Frank A. F. ^{[2
]}

Percival, Carl J. ^{[2
]}

机构：

[1] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA

[2] CALTECH, NASA, Jet Prop Lab, Pasadena, CA 91109 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2024年 / 15卷 / 13期

基金：

美国国家航空航天局;

关键词：

CRIEGEE INTERMEDIATE CH2OO; PEROXY-RADICALS; SELF-REACTION; CHEMISTRY; FORMALDEHYDE; ATOMS; OXIDE; IO;

D O I：

10.1021/acs.jpclett.4c00159

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Criegee intermediates play an important role in the oxidizing capacity of the Earth's troposphere. Although extensive studies have been conducted on Criegee intermediates in the past decade, their kinetics with radical species remain underexplored. We investigated the kinetics of the simplest Criegee intermediate, CH<INF>2</INF>OO, with the methyl peroxy radical, CH<INF>3</INF>O<INF>2</INF>, as a model system to explore the reactivities of Criegee intermediates with peroxy radicals. Using a multipass UV-Vis spectrometer coupled to a pulsed-laser photolysis flow reactor, CH<INF>2</INF>OO and CH<INF>3</INF>O<INF>2</INF> were generated simultaneously from the photolysis of CH<INF>2</INF>I<INF>2</INF>/CH<INF>3</INF>I/O<INF>2</INF>/N<INF>2</INF> mixtures with CH<INF>2</INF>OO measured directly near 340 nm. We determined a reaction rate coefficient k<INF>CH<INF>2</INF>OO+CH<INF>3</INF>O<INF>2</INF></INF> = (1.7 +/- 0.5) x 10-11 cm3 s-1 at 294 K and 10 Torr, where the influence of iodine adducts is reduced. This rate coefficient is faster than previous theoretical predictions, highlighting the challenges in accurately describing the interaction between zwitterionic and biradical characteristics of Criegee intermediates.

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页码：3690 / 3697

页数：8

相关论文

共 46 条

[1] The reaction of formaldehyde carbonyl oxide with the methyl peroxy radical and its relevance in the chemistry of the atmosphere [J].

Anglada, Josep M. ;

Olivella, Santiago ;

Sole, Albert .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2013, 15 (43) :18921-18933

[2] The reaction of fluorine atoms with methanol: yield of CH3O/CH2OH and rate constant of the reactions CH3O + CH3O and CH3O + HO2 [J].

Assaf, Emmanuel ;

Schoemaecker, Coralie ;

Vereecken, Luc ;

Fittschen, Christa .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2018, 20 (16) :10660-10670

[3] Evaluated kinetic and photochemical data for atmospheric chemistry: Volume III - gas phase reactions of inorganic halogens [J].

Atkinson, R. ;

Baulch, D. L. ;

Cox, R. A. ;

Crowley, J. N. ;

Hampson, R. F. ;

Hynes, R. G. ;

Jenkin, M. E. ;

Rossi, M. J. ;

Troe, J. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2007, 7 :981-1191

[4] Direct Determination of the Simplest Criegee Intermediate (CH2OO) Self Reaction Rate [J].

Buras, Zachary J. ;

Elsamra, Rehab M. I. ;

Green, William H. .

JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2014, 5 (13) :2224-2228

[5]

Burkholder J. B., 2020, JPL Publ, V195, P2

[6] Direct kinetic measurements and theoretical predictions of an isoprene-derived Criegee intermediate [J].

Caravan, Rebecca L. ;

Vansco, Michael F. ;

Au, Kendrew ;

Khan, M. Anwar H. ;

Li, Yu-Lin ;

Winiberg, Frank A. F. ;

Zuraski, Kristen ;

Lin, Yen-Hsiu ;

Chao, Wen ;

Trongsiriwat, Nisalak ;

Walsh, Patrick J. ;

Osborn, David L. ;

Percival, Carl J. ;

Lin, Jim Jr-Min ;

Shallcross, Dudley E. ;

Sheps, Leonid ;

Klippenstein, Stephen J. ;

Taatjes, Craig A. ;

Lester, Marsha, I .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2020, 117 (18) :9733-9740

[7] Products of Criegee intermediate reactions with NO2: experimental measurements and tropospheric implications [J].

Caravan, Rebecca L. ;

Khan, M. Anwar H. ;

Rotavera, Brandon ;

Papajak, Ewa ;

Antonov, Ivan O. ;

Chen, Ming-Wei ;

Au, Kendrew ;

Chao, Wen ;

Osborn, David L. ;

Lin, Jim Jr-Min ;

Percival, Carl J. ;

Shallcrossb, Dudley E. ;

Taatjes, Craig A. .

FARADAY DISCUSSIONS, 2017, 200 :313-330

[8] Hydrogen-Bonding Mediated Reactions of Criegee Intermediates in the Gas Phase: Competition between Bimolecular and Termolecular Reactions and the Catalytic Role of Water [J].

Chao, Wen ;

Yin, Cangtao ;

Takahashi, Kaito ;

Lin, Jim Jr-Min .

JOURNAL OF PHYSICAL CHEMISTRY A, 2019, 123 (39) :8336-8348

[9] Impact of Criegee Intermediate Reactions with Peroxy Radicals on Tropospheric Organic Aerosol [J].

Chhantyal-Pun, Rabi ;

Khan, M. Anwar H. ;

Zachhuber, Nicholas ;

Percival, Carl J. ;

Shallcross, Dudley E. ;

Orr-Ewing, Andrew J. .

ACS EARTH AND SPACE CHEMISTRY, 2020, 4 (10) :1743-1755

[10] Criegee intermediates: production, detection and reactivity [J].

Chhantyal-Pun, Rabi ;

Khan, M. Anwar H. ;

Taatjes, Craig A. ;

Percival, Carl J. ;

Orr-Ewing, Andrew J. ;

Shallcross, Dudley E. .

INTERNATIONAL REVIEWS IN PHYSICAL CHEMISTRY, 2020, 39 (03) :383-422

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