26 Aug 2022
26 Aug 2022
Status: this preprint is currently under review for the journal ACP.

Aging impact on sources, volatility, and viscosity of organic aerosols in the Chinese outflows

Tingting Feng1,2,3,4,5,, Yingkun Wang1,2,3,4,5,, Weiwei Hu1,2,4,5,6, Ming Zhu1,2,3,4,5, Wei Song1,2,4,5, Wei Chen1,2,3,4,5, Yanyan Sang7, Zheng Fang1,2,3,4,5, Wei Deng1,2,3,4,5, Hua Fang1,2,3,4,5,a, Xu Yu1,2,3,4,5, Cheng Wu8, Bin Yuan9, Shan Huang9, Min Shao9, Xiaofeng Huang10, Lingyan He10, Young Ro Lee11, L. Gregory Huey11, Francesco Canonaco12,13, Andre S. H. Prevot12, and Xinming Wang1,2,3,4,5 Tingting Feng et al.
  • 1State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
  • 2CAS Center for Excellence in Deep Earth Science, Guangzhou 510640, China
  • 3Chinese Academy of Sciences University, Beijing 100049, China
  • 4Guangdong-Hong Kong-Macao, Joint Laboratory for Environmental Pollution and Control, Guangzhou Institute of Geochemistry, Chinese Academy of Science, Guangzhou 510640, China
  • 5Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Chinese Academy of Science, Guangzhou 510640, China
  • 6Shanghai Academy of Environmental Sciences, Shanghai 200233, China
  • 7Tai’an Environmental Protection Bureau, Tai’an, Shandong 271000, China
  • 8Institute of Mass Spectrometry and Atmospheric Environment, Jinan University, Guangzhou 510632, China
  • 9Institute for Environmental and Climate Research, Jinan University, Guangzhou 511443, China
  • 10Key Laboratory for Urban Habitat Environmental Science and Technology, School of Environment and Energy, Peking University Shenzhen Graduate School, Shenzhen, China
  • 11School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA 30332, USA
  • 12Paul Scherrer Institute, Laboratory of Atmospheric Chemistry, 5232 Villigen PSI, Switzerland
  • 13Datalystica Ltd., Park innovAARE, 5234 Villigen, Switzerland
  • anow at: School of Ecology and Environment, Anhui Normal University, Wuhu, Anhui 241000, China
  • These authors contributed equally to this work.

Abstract. To investigate the aging impact on sources, volatility, and viscosity of organic aerosols (OA) in the Chinese outflows, a high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) coupled with a thermodenuder (TD) was deployed in the spring of 2018 in Dongying, which is a regional receptor site of metropolitan emissions in North China Plain (NCP). The average mass concentration of PM1 was 31.5 ± 22.7 μg m–3, which was mainly composed of nitrate (33 %) and OA (25 %). The source apportionment results show the OA was mainly contributed by oxygenated OA (OOA) from secondary sources, including background-OOA (33 %) representing a background concentration of OA (2.6 μg m–3) in the NCP area, and transported-OOA (33 %) oxidizing from urban emissions. The other two factors include aged hydrocarbon-liked OA (aged-HOA, 28 %) from transported vehicle emissions and biomass burning OA (BBOA, 5 %) from local open burnings. The volatility of total OA (average C* = 3.2×10–4 µg m–3) in this study is generally lower than those in previous field studies, which is mainly due to the high OA oxidation level resulting from aging processes during transport. The volatilities of OA factors follow the order of background-OOA (average C* = 2.7×10–5 μg m–3) < transported-OOA (3.7×10–4 μg m–3) < aged-HOA (8.1×10–4 μg m–3) < BBOA (0.012 μg m–3), indicating the probable existence of oligomers. The viscosity estimation suggests that the majority of ambient OA in this study behaves as semi-solid (60 %), liquifies at higher RH (21 %), and solidifies (19 %) during noon time when the RH is low and the oxidation level is high. Finally, the estimated mixing time of OA varies dramatically from minutes at night to years in the afternoon, emphasizing the necessity to consider its dynamic kinetic limits when modeling OA. In general, the overall results of this study improve the understanding of the aging impact on OA volatility and viscosity.

Tingting Feng et al.

Status: open (until 07 Oct 2022)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2022-575', Anonymous Referee #2, 15 Sep 2022 reply
  • RC2: 'Comment on acp-2022-575', Anonymous Referee #1, 24 Sep 2022 reply

Tingting Feng et al.

Tingting Feng et al.


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Short summary
To investigate the impact of aging processes on the organic aerosols (OA), we conducted a comprehensive field study at a continental remote site using on-line mass spectrometers. The results show that OA in the Chinese outflows was strongly influenced by upwind anthropogenic emissions. The aging processes can significantly decrease the OA volatility and result in a varied viscosity of OA under different circumstances, signifying the complex physiochemistry properties of OA in the aged plumes.