Structural Effects of Amines in Enhancing Methanesulfonic Acid-Driven New Particle Formation

Jiewen Shen; Jonas Elm; Hong Bin Xie; Jingwen Chen; Junfeng Niu; Hanna Vehkamäki

doi:10.1021/acs.est.0c05358

Structural Effects of Amines in Enhancing Methanesulfonic Acid-Driven New Particle Formation

Jiewen Shen, Jonas Elm, Hong Bin Xie^*, Jingwen Chen, Junfeng Niu, Hanna Vehkamäki

^*Corresponding author for this work

iCLIMATE Aarhus University Interdisciplinary Centre for Climate Change - iCLIMATE Aarhus University Interdisciplinary Centre for Climate Change, Langelandsgade
Department of Chemistry

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

39 Citations (Scopus)

Abstract

Atmospheric amines can enhance methanesulfonic acid (MSA)-driven new particle formation (NPF), but the mechanism is fundamentally different compared to that of the extensively studied sulfuric acid (SA)-driven process. Generally, the enhancing potentials of amines in SA-driven NPF follow the basicity, while this is not the case for MSA-driven NPF, where structural effects dominate, making MSA-driven NPF more prominent for methylamine (MA) compared to dimethylamine (DMA). Therefore, probing structural factors determining the enhancing potentials of amines on MSA-driven NPF is key to fully understanding the contribution of MSA to NPF. Here, we performed a comparative study on DMA and MA enhancing MSA-driven NPF by examining cluster formation using computational methods. The results indicate that DMA-MSA clusters are more stable than the corresponding MA-MSA clusters for cluster sizes up to (DMA)2(MSA)2, indicating that the basicity of amines dominates the initial cluster formation. The methyl groups of DMA were found to present significant steric hindrance beyond the (DMA)2(MSA)2 cluster and this adds to the lower hydrogen bonding capacity of DMA, making the cluster growth less favorable compared to MA. This study implies that several amines could synergistically enhance MSA-driven NPF by maximizing the advantage of different amines in different amine-MSA cluster growth stages.

Original language	English
Journal	Environmental Science & Technology
Volume	54
Issue	21
Pages (from-to)	13498-13508
Number of pages	11
ISSN	0013-936X
DOIs	https://doi.org/10.1021/acs.est.0c05358
Publication status	Published - Nov 2020

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title = "Structural Effects of Amines in Enhancing Methanesulfonic Acid-Driven New Particle Formation",

abstract = "Atmospheric amines can enhance methanesulfonic acid (MSA)-driven new particle formation (NPF), but the mechanism is fundamentally different compared to that of the extensively studied sulfuric acid (SA)-driven process. Generally, the enhancing potentials of amines in SA-driven NPF follow the basicity, while this is not the case for MSA-driven NPF, where structural effects dominate, making MSA-driven NPF more prominent for methylamine (MA) compared to dimethylamine (DMA). Therefore, probing structural factors determining the enhancing potentials of amines on MSA-driven NPF is key to fully understanding the contribution of MSA to NPF. Here, we performed a comparative study on DMA and MA enhancing MSA-driven NPF by examining cluster formation using computational methods. The results indicate that DMA-MSA clusters are more stable than the corresponding MA-MSA clusters for cluster sizes up to (DMA)2(MSA)2, indicating that the basicity of amines dominates the initial cluster formation. The methyl groups of DMA were found to present significant steric hindrance beyond the (DMA)2(MSA)2 cluster and this adds to the lower hydrogen bonding capacity of DMA, making the cluster growth less favorable compared to MA. This study implies that several amines could synergistically enhance MSA-driven NPF by maximizing the advantage of different amines in different amine-MSA cluster growth stages.",

author = "Jiewen Shen and Jonas Elm and Xie, {Hong Bin} and Jingwen Chen and Junfeng Niu and Hanna Vehkam{\"a}ki",

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Structural Effects of Amines in Enhancing Methanesulfonic Acid-Driven New Particle Formation. / Shen, Jiewen; Elm, Jonas; Xie, Hong Bin et al.
In: Environmental Science & Technology, Vol. 54, No. 21, 11.2020, p. 13498-13508.

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

TY - JOUR

T1 - Structural Effects of Amines in Enhancing Methanesulfonic Acid-Driven New Particle Formation

AU - Shen, Jiewen

AU - Elm, Jonas

AU - Xie, Hong Bin

AU - Chen, Jingwen

AU - Niu, Junfeng

AU - Vehkamäki, Hanna

PY - 2020/11

Y1 - 2020/11

N2 - Atmospheric amines can enhance methanesulfonic acid (MSA)-driven new particle formation (NPF), but the mechanism is fundamentally different compared to that of the extensively studied sulfuric acid (SA)-driven process. Generally, the enhancing potentials of amines in SA-driven NPF follow the basicity, while this is not the case for MSA-driven NPF, where structural effects dominate, making MSA-driven NPF more prominent for methylamine (MA) compared to dimethylamine (DMA). Therefore, probing structural factors determining the enhancing potentials of amines on MSA-driven NPF is key to fully understanding the contribution of MSA to NPF. Here, we performed a comparative study on DMA and MA enhancing MSA-driven NPF by examining cluster formation using computational methods. The results indicate that DMA-MSA clusters are more stable than the corresponding MA-MSA clusters for cluster sizes up to (DMA)2(MSA)2, indicating that the basicity of amines dominates the initial cluster formation. The methyl groups of DMA were found to present significant steric hindrance beyond the (DMA)2(MSA)2 cluster and this adds to the lower hydrogen bonding capacity of DMA, making the cluster growth less favorable compared to MA. This study implies that several amines could synergistically enhance MSA-driven NPF by maximizing the advantage of different amines in different amine-MSA cluster growth stages.

AB - Atmospheric amines can enhance methanesulfonic acid (MSA)-driven new particle formation (NPF), but the mechanism is fundamentally different compared to that of the extensively studied sulfuric acid (SA)-driven process. Generally, the enhancing potentials of amines in SA-driven NPF follow the basicity, while this is not the case for MSA-driven NPF, where structural effects dominate, making MSA-driven NPF more prominent for methylamine (MA) compared to dimethylamine (DMA). Therefore, probing structural factors determining the enhancing potentials of amines on MSA-driven NPF is key to fully understanding the contribution of MSA to NPF. Here, we performed a comparative study on DMA and MA enhancing MSA-driven NPF by examining cluster formation using computational methods. The results indicate that DMA-MSA clusters are more stable than the corresponding MA-MSA clusters for cluster sizes up to (DMA)2(MSA)2, indicating that the basicity of amines dominates the initial cluster formation. The methyl groups of DMA were found to present significant steric hindrance beyond the (DMA)2(MSA)2 cluster and this adds to the lower hydrogen bonding capacity of DMA, making the cluster growth less favorable compared to MA. This study implies that several amines could synergistically enhance MSA-driven NPF by maximizing the advantage of different amines in different amine-MSA cluster growth stages.

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Structural Effects of Amines in Enhancing Methanesulfonic Acid-Driven New Particle Formation

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