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Interaction between succinic acid and sulfuric acid–base clusters

Lin, Yun and Ji, Yuemeng and Li, Yixin and Secrest, Jeremiah and Xu, Wen and Xu, Fei and Wang, Yuan and An, Taicheng and Zhang, Renyi (2019) Interaction between succinic acid and sulfuric acid–base clusters. Atmospheric Chemistry and Physics, 19 (12). pp. 8003-8019. ISSN 1680-7324. https://resolver.caltech.edu/CaltechAUTHORS:20190709-084300424

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Abstract

Dicarboxylic acids likely participate in the formation of pre-nucleation clusters to facilitate new particle formation in the atmosphere, but the detailed mechanism leading to the formation of multicomponent critical nuclei involving organic acids, sulfuric acid (SA), base species, and water remains unclear. In this study, theoretical calculations are performed to elucidate the interactions between succinic acid (SUA) and clusters consisting of SA-ammonia (AM)∕dimethylamine (DMA) in the presence of hydration of up to six water molecules. Formation of the hydrated SUA•SA• base clusters is energetically favorable, triggering proton transfer from SA to the base molecule to form new covalent bonds or strengthening the preexisting covalent bonds. The presence of SUA promotes hydration of the SA•AM and SA•AM•DMA clusters but dehydration of the SA•DMA clusters. At equilibrium, SUA competes with the second SA molecule for addition to the SA• base clusters at atmospherically relevant concentrations. The clusters containing both the base and organic acid are capable of further binding with acid molecules to promote subsequent growth. Our results indicate that the multicomponent nucleation involving organic acids, sulfuric acid, and base species promotes new particle formation in the atmosphere, particularly under polluted conditions with a high concentration of diverse organic acids.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.5194/acp-19-8003-2019DOIArticle
ORCID:
AuthorORCID
Lin, Yun0000-0001-8222-0346
Xu, Wen0000-0002-2084-2630
Zhang, Renyi0000-0001-8708-3862
Additional Information:© Author(s) 2019. This work is distributed under the Creative Commons Attribution 4.0 License. Received: 13 September 2018 – Discussion started: 16 October 2018. Revised: 4 April 2019 – Accepted: 8 April 2019 – Published: 18 June 2019. Data availability. The data used in this study are available from the corresponding author upon request (renyi-zhang@tamu.edu). Supplementary material contains additional relief maps for the sulfuric acid–base clusters and lists of topological properties for the most stable conformers of each cluster category. The supplement related to this article is available online at: https://doi.org/10.5194/acp-19-8003-2019-supplement. Author contributions. YuL, YJ, and RZ designed the research. YuL, YJ, YiL, WX, and FX performed simulations. YuL, YW, YJ, YiL, TA, and JS analyzed data. YuL, YJ, YiL, and RZ wrote the paper. The authors declare that they have no conflict of interest. Special issue statement. This article is part of the special issue “Multiphase chemistry of secondary aerosol formation under severe haze”. It is not associated with a conference. The research was partially conducted with the advanced computing resources provided by Texas A&M High Performance Research Computing. The authors acknowledged the Laboratory for Molecular Simulations at Texas A&M University. This work was supported by the National Natural Science Foundation of China (41675122, 41425015, U1401245, and 41373102), Science and Technology Program of Guangzhou City (201707010188), Team Project from the Natural Science Foundation of Guangdong Province, China (S2012030006604), Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase), National Supercomputing Center in Guangzhou (NSCC-GZ), and Robert A. Welch Foundation (A-1417). Review statement. This paper was edited by Jingkun Jiang and reviewed by three anonymous referees.
Funders:
Funding AgencyGrant Number
National Natural Science Foundation of China41675122
National Natural Science Foundation of China41425015
National Natural Science Foundation of ChinaU1401245
National Natural Science Foundation of China41373102
Guangzhou City201707010188
Natural Science Foundation of Guangdong ProvinceS2012030006604
NSFC-Guangdong Joint FundUNSPECIFIED
National Supercomputing Center (NSCC-GZ)UNSPECIFIED
Robert A. Welch FoundationA-1417
Issue or Number:12
Record Number:CaltechAUTHORS:20190709-084300424
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20190709-084300424
Official Citation:Lin, Y., Ji, Y., Li, Y., Secrest, J., Xu, W., Xu, F., Wang, Y., An, T., and Zhang, R.: Interaction between succinic acid and sulfuric acid–base clusters, Atmos. Chem. Phys., 19, 8003-8019, https://doi.org/10.5194/acp-19-8003-2019, 2019
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:96941
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:09 Jul 2019 17:18
Last Modified:03 Oct 2019 21:26

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