Preprints
https://doi.org/10.5194/acp-2022-86
https://doi.org/10.5194/acp-2022-86
 
09 Feb 2022
09 Feb 2022
Status: a revised version of this preprint was accepted for the journal ACP and is expected to appear here in due course.

Reversible and irreversible gas-particle partitioning of dicarbonyl compounds observed in the real atmosphere

Jingcheng Hu, Zhongming Chen, Xuan Qin, and Ping Dong Jingcheng Hu et al.
  • State Key Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing, 100871, China

Abstract. Glyoxal and methylglyoxal are vital carbonyl compounds in the atmosphere and play substantial roles in radical cycling and ozone formation. The partitioning process of glyoxal and methylglyoxal between the gas and particle phase via reversible and irreversible pathways could efficiently contribute to secondary organic aerosol (SOA) formation. However, the relative importance of two partitioning pathways still remain elusive, especially in the real atmosphere. In this study, we launched five field observations in different seasons and simultaneously measured glyoxal and methylglyoxal in the gas and particle phase. The field-measured gas-particle partitioning coefficients were 5–7 magnitudes higher than the theoretical ones, indicating the significant roles of reversible and irreversible pathways in the partitioning process. The particulate concentration of dicarbonyls and product distribution via the two pathways were further investigated using a box model coupled with the corresponding kinetic mechanisms. We recommended the irreversible reactive uptake coefficient γ for glyoxal and methylglyoxal in different seasons in the real atmosphere, and the average value of 8.0 × 10−3 for glyoxal and 2.0 × 10−3 for methylglyoxal best represented the the loss of gaseous dicarbonyls by irreversible gas-particle partitioning processes. Compared to the reversible pathways, the irreversible pathways played a dominant role, with a proportion of more than 90 % in the gas-particle partitioning process in the real atmosphere and the proportion was significantly influenced by relative humidity and inorganic components in aerosols. However, the reversible pathways were also substantial, especially in winter, with a proportion of more than 10 %. These two pathways of dicarbonyls jointly contributed to more than 25 % of SOAs in the real atmosphere. To our knowledge, this study was the first to systemically examine both reversible and irreversible pathways in the ambient atmosphere, strove to narrow the gap between model simulations and field-measured gas-particle partitioning coefficients, and revealed the importance of gas-particle processes for dicarbonyls in SOA formation.

Jingcheng Hu et al.

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2022-86', Anonymous Referee #1, 14 Feb 2022
  • RC2: 'Comment on acp-2022-86', Anonymous Referee #2, 25 Mar 2022
  • RC3: 'Comment on acp-2022-86', Anonymous Referee #3, 30 Mar 2022
  • RC4: 'Comment on acp-2022-86', Anonymous Referee #4, 31 Mar 2022

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2022-86', Anonymous Referee #1, 14 Feb 2022
  • RC2: 'Comment on acp-2022-86', Anonymous Referee #2, 25 Mar 2022
  • RC3: 'Comment on acp-2022-86', Anonymous Referee #3, 30 Mar 2022
  • RC4: 'Comment on acp-2022-86', Anonymous Referee #4, 31 Mar 2022

Jingcheng Hu et al.

Jingcheng Hu et al.

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Short summary
In this study, glyoxal and methylglyoxal, two important carbonyl compounds in the atmosphere, in the gas and particle phase were simultaneously measured in five field observations. We find that irreversible pathways play a dominant role with a proportion of more than 90 % in the partitioning process and we recommend the uptake coefficient for dicarbonyls in the real atmosphere. We expect this study could make contribution to the model simulation of secondary organic aerosols formation.
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