The missing base molecules in atmospheric acid–base nucleation

Cai, Runlong; Yin, Rujing; Yan, Chao; Yang, Dongsen; Deng, Chenjuan; Dada, Lubna; Kangasluoma, Juha; Kontkanen, Jenni; Halonen, Roope; Ma, Yan; Zhang, Xiuhui; Paasonen, Pauli; Petäjä, Tuukka; Kerminen, Veli-Matti; Liu, Yongchun; Bianchi, Federico; Zheng, Jun; Wang, Lin; Hao, Jiming; Smith, James N.; Donahue, Neil M.; Kulmala, Markku; Worsnop, Douglas R.; Jiang, Jingkun

doi:10.1093/nsr/nwac137

The missing base molecules in atmospheric acid–base nucleation

Journal Article · Mon Jul 25 00:00:00 EDT 2022 · National Science Review

DOI:https://doi.org/10.1093/nsr/nwac137· OSTI ID:1890019

Cai, Runlong; Yin, Rujing; Yan, Chao; Yang, Dongsen; Deng, Chenjuan; ; Kangasluoma, Juha; Kontkanen, Jenni; Halonen, Roope; Ma, Yan; Zhang, Xiuhui; Paasonen, Pauli; Petäjä, Tuukka; Kerminen, Veli-Matti; Liu, Yongchun; Bianchi, Federico; Zheng, Jun; ; Hao, Jiming; Smith, James N. more »

Abstract

Transformation of low-volatility gaseous precursors to new particles affects aerosol number concentration, cloud formation and hence the climate. The clustering of acid and base molecules is a major mechanism driving fast nucleation and initial growth of new particles in the atmosphere. However, the acid–base cluster composition, measured using state-of-the-art mass spectrometers, cannot explain the measured high formation rate of new particles. Here we present strong evidence for the existence of base molecules such as amines in the smallest atmospheric sulfuric acid clusters prior to their detection by mass spectrometers. We demonstrate that forming (H2SO4)1(amine)1 is the rate-limiting step in atmospheric H2SO4-amine nucleation and the uptake of (H2SO4)1(amine)1 is a major pathway for the initial growth of H2SO4 clusters. The proposed mechanism is very consistent with measured new particle formation in urban Beijing, in which dimethylamine is the key base for H2SO4 nucleation while other bases such as ammonia may contribute to the growth of larger clusters. Our findings further underline the fact that strong amines, even at low concentrations and when undetected in the smallest clusters, can be crucial to particle formation in the planetary boundary layer.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center

Sponsoring Organization:: Academy of Finland; National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); Samsung PM2.5 SRP; USDOE; USDOE Office of Science (SC), Biological and Environmental Research (BER)

Contributing Organization:: Argonne National Laboratory (ANL); Brookhaven National Laboratory (BNL); Oak Ridge National Laboratory (ORNL); Pacific Northwest National Laboratory (PNNL)

Grant/Contract Number:: SC0019000

OSTI ID:: 1890019

Alternate ID(s):: OSTI ID: 1888594
OSTI ID: 1891461

Journal Information:: National Science Review, Journal Name: National Science Review Journal Issue: 10 Vol. 9; ISSN 2095-5138

Publisher:: Oxford University PressCopyright Statement

Country of Publication:: China

Language:: English

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