Preprints
https://doi.org/10.5194/egusphere-2023-692
https://doi.org/10.5194/egusphere-2023-692
21 Apr 2023
 | 21 Apr 2023
Status: this preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).

Influence of acidity on liquid−liquid phase transitions of mixed SOA proxy–inorganic aerosol droplets

Yueling Chen, Xiangyu Pei, Huichao Liu, Yikan Meng, Zhengning Xu, Fei Zhang, Chun Xiong, Thomas C. Preston, and Zhibin Wang

Abstract. Phase state and morphology of aerosol particles play a critical role in determining their effect on climate. While aerosol acidity has been identified as a key factor affecting the multiphase chemistry and phase transitions, the impact of acidity on phase transition of multicomponent aerosol particles has not been extensively studied in situ. In this work, we employ an aerosol optical tweezer (AOT) to probe the impact of acidity on the phase transition behavior of levitated aerosol particles. Our results reveal that higher acidity decreases the separation relative humidity (SRH) of aerosol droplets mixed with ammonium sulfate (AS) and secondary organic aerosol (SOA) proxy, such as 3-methylglutaric acid (3-MGA), 1,2,6-hexanetriol (HEXT) and 2,5-hexanediol (HEXD) across aerosol pH in atmospheric condition. Phase separation of organic acids was more sensitive to acidity compared to organic alcohols. We found the mixing relative humidity (MRH) was consistently higher than the SRH in several systems. Phase-separating systems, including 3-MGA/AS, HEXT/AS, and HEXD/AS, exhibited oxygen-to-carbon ratios (O:C) of 0.67, 0.50, and 0.33, respectively. In contrast, liquid-liquid phase separation (LLPS) did not occur in the high O:C system of glycerol/AS, which had an O:C of 1.00. Additionally, the morphology of 38 out of the 40 aerosol particles that underwent LLPS was observed to be a core-shell. Our findings provide a comprehensive understanding of the pH-dependent LLPS in individual suspended aerosol droplets and pave the way for future research on phase separation of atmospheric aerosol particles.

Yueling Chen et al.

Status: open (until 02 Jun 2023)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2023-692', Anonymous Referee #1, 18 May 2023 reply
  • RC2: 'Comment on egusphere-2023-692', Anonymous Referee #2, 22 May 2023 reply

Yueling Chen et al.

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Short summary
The impact of acidity on the phase transition behavior of levitated aerosol particles was examined. Our results revealed that lower acidity decreases the separation relative humidity of aerosol droplets mixed with ammonium sulfate and secondary organic aerosol proxy. Our research suggests that in real atmospheric conditions where the high acidity found in many ambient aerosol particles, droplets encounter heightened impediments to phase separation and tend to display a homogeneous structure.