Heterogeneous Reactions of Methane with Cl Radicals on Large ArN Clusters

Result code in IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F22%3A00552510" target="_blank" >RIV/61388955:_____/22:00552510 - isvavai.cz</a>

Result on the web

<a href="http://hdl.handle.net/11104/0327621" target="_blank" >http://hdl.handle.net/11104/0327621</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acs.jpca.1c08476" target="_blank" >10.1021/acs.jpca.1c08476</a>

Result language

angličtina

Original language name

Heterogeneous Reactions of Methane with Cl Radicals on Large ArN Clusters

Original language description

Heterogeneous chemistry on the surfaces of atmospheric particles has a wide impact on the properties and composition of the Earth’s atmosphere. In laboratory studies, clusters can represent proxies to atmospheric aerosols and help to discern the individual steps in reactions on or in aerosols. We investigate the reactivity of Cl and CCl3 radicals with methane on argon clusters using the pickup method. For radical generation, we built a new pyrolysis source partially adapting the design of radical sources that utilize the supersonic expansion into a heated silicon carbide tube. Large ArN, N̅ ≈ 110, clusters were generated in a supersonic expansion, and CH4 molecules were embedded in the clusters via a pickup process followed by the uptake of the radicals produced in the pyrolysis source. The analysis of the mass spectra recorded under different experimental conditions (i.e., with the pyrolysis ON and OFF and with only one or both reactants) allowed us to identify various products of the radical reactions on ArN. We propose a sequence of reactions based on the reaction energetics. It starts with the hydrogen abstraction from CH4 by a Cl radical resulting in HCl and CH3 followed by a halogenation step where CCl4 molecules react with the available CH3 radicals, yielding CH3Cl. By analogy, the CH3Cl enters another hydrogen abstraction by Cl, producing HCl and the CH2Cl radical, which again undergoes a halogenation step with CCl4, generating CH2Cl2. Further reaction of CH2Cl2 with Cl terminates the sequence by the production of HCl and CHCl2.

Czech name

—

Czech description

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Type

J_imp - Article in a specialist periodical, which is included in the Web of Science database

CEP classification

—

OECD FORD branch

10403 - Physical chemistry

Project

<a href="/en/project/GA19-14105S" target="_blank" >GA19-14105S: Heterogeneous reactions of the atmospheric radicals on clusters.</a><br>

Continuities

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Publication year

2022

Confidentiality

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Name of the periodical

Journal of Physical Chemistry A

ISSN

1089-5639

e-ISSN

1520-5215

Volume of the periodical

126

Issue of the periodical within the volume

2

Country of publishing house

US - UNITED STATES

Number of pages

10

Pages from-to

249-258

UT code for WoS article

000742736000001

EID of the result in the Scopus database

2-s2.0-85123357615