Articles | Volume 22, issue 22
https://doi.org/10.5194/acp-22-14529-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-22-14529-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
16 Nov 2022
Research article |
| 16 Nov 2022
| 16 Nov 2022
Oligomer formation from the gas-phase reactions of Criegee intermediates with hydroperoxide esters: mechanism and kinetics
Long Chen
State Key Lab of Loess and Quaternary Geology (SKLLQG), Institute of Earth Environment, Chinese Academy of Sciences (CAS), Xi'an 710061, China
CAS Center for Excellence in Quaternary Science and Global Change, Xi'an 710061, China
Yu Huang
CORRESPONDING AUTHOR
State Key Lab of Loess and Quaternary Geology (SKLLQG), Institute of Earth Environment, Chinese Academy of Sciences (CAS), Xi'an 710061, China
CAS Center for Excellence in Quaternary Science and Global Change, Xi'an 710061, China
Yonggang Xue
State Key Lab of Loess and Quaternary Geology (SKLLQG), Institute of Earth Environment, Chinese Academy of Sciences (CAS), Xi'an 710061, China
CAS Center for Excellence in Quaternary Science and Global Change, Xi'an 710061, China
Zhihui Jia
School of Materials Science and Engineering, Shaanxi Normal University, Xi'an, Shaanxi 710119, China
Wenliang Wang
School of Chemistry and Chemical Engineering, Key Laboratory for Macromolecular Science of Shaanxi Province, Shaanxi Normal University, Xi'an, Shaanxi 710119, China
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The mechanisms and kinetics of the formation of highly oxidized products from the multi-generation ·OH oxidation of styrene in the absence and presence of NOx are studied using the quantum chemistry methods. The calculations show that the volatility of the multi-generation ·OH oxidation products significantly decreases with increasing the number of ·OH oxidation steps.
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Quantum chemical methods are applied to gain insight into the detailed mechanisms of OH-initiated oxidation of distinct HHPs. The dominant pathway is H-abstraction from the -OOH group in the initiation reactions of the OH radical with HOCH2OOH and HOC(CH3)2OOH. H-abstraction from -CH group is competitive with that from the -OOH group in the reaction of the OH radical with HOCH(CH3)OOH. The barrier of H-abstraction from the -OOH group is slightly increased as the methyl group number increases.
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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The mechanisms and kinetics of the formation of highly oxidized products from the multi-generation ·OH oxidation of styrene in the absence and presence of NOx are studied using the quantum chemistry methods. The calculations show that the volatility of the multi-generation ·OH oxidation products significantly decreases with increasing the number of ·OH oxidation steps.
Meng Wang, Yusen Duan, Wei Xu, Qiyuan Wang, Zhuozhi Zhang, Qi Yuan, Xinwei Li, Shuwen Han, Haijie Tong, Juntao Huo, Jia Chen, Shan Gao, Zhongbiao Wu, Long Cui, Yu Huang, Guangli Xiu, Junji Cao, Qingyan Fu, and Shun-cheng Lee
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In this study, we report the long-term measurement of organic carbon (OC) and elementary carbon (EC) in PM2.5 with hourly time resolution conducted at a regional site in Shanghai from 2016 to 2020. The results from this study provide critical information about the long-term trend of carbonaceous aerosol, in particular secondary OC, in one of the largest megacities in the world and are helpful for developing pollution control measures from a long-term planning perspective.
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Quantum chemical methods are applied to gain insight into the detailed mechanisms of OH-initiated oxidation of distinct HHPs. The dominant pathway is H-abstraction from the -OOH group in the initiation reactions of the OH radical with HOCH2OOH and HOC(CH3)2OOH. H-abstraction from -CH group is competitive with that from the -OOH group in the reaction of the OH radical with HOCH(CH3)OOH. The barrier of H-abstraction from the -OOH group is slightly increased as the methyl group number increases.
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Short summary
Quantum chemical methods are applied to gain insight into the oligomerization reaction mechanisms and kinetics of distinct stabilized Criegee intermediate (SCI) reactions with hydroperoxide esters, where calculations show that SCI addition reactions with hydroperoxide esters proceed through the successive insertion of SCIs to form oligomers that involve SCIs as the repeating unit. The saturated vapor pressure of the formed oligomers decreases monotonically with the increasing number of SCIs.
Quantum chemical methods are applied to gain insight into the oligomerization reaction...
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