Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels

Miao, Ruqian; Chen, Qi; Shrivastava, Manish; Chen, Youfan; Zhang, Lin; Hu, Jianlin; Zheng, Yan; Liao, Keren

doi:10.5194/acp-21-16183-2021

Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels

Journal Article · Thu Nov 04 00:00:00 EDT 2021 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-21-16183-2021· OSTI ID:1832987

Miao, Ruqian ^[1]; Chen, Qi ^[1]; ^[2]; Chen, Youfan ^[3]; Zhang, Lin ^[4]; Hu, Jianlin ^[5]; Zheng, Yan ^[1]; Liao, Keren ^[1]

Peking Univ., Beijing (China). State Key Joint Lab. of Environmental Simulation and Pollution Control, BIC-ESAT and IJRC
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sichuan Academy of Environmental Policy and Planning, Chengdu (China)
Peking Univ., Beijing (China). Lab. for Climate and Ocean–Atmosphere Studies
Nanjing Univ. of Information Science and Technology (China). Jiangsu Key Lab. of Atmospheric Environment Monitoring and Pollution Control, Jiangsu Engineering Technology Research Center of Environmental Cleaning Materials, Collaborative Innovation Center of Atmospheric Environment and Equipment Technology

Organic aerosol (OA) is a major component of tropospheric submicron aerosol that contributes to air pollution and causes adverse effects on human health. Chemical transport models have difficulties in reproducing the variability in OA concentrations in polluted areas, hindering understanding of the OA budget and sources. Herein, we apply both process-based and observation-constrained schemes to simulate OA in GEOS-Chem. Comprehensive data sets of surface OA, OA components, secondary organic aerosol (SOA) precursors, and oxidants were used for model–observation comparisons. The base models generally underestimate the SOA concentrations in China. In the revised schemes, updates were made on the emissions, volatility distributions, and SOA yields of semivolatile and intermediate-volatility organic compounds (SVOCs and IVOCs) and additional nitrous acid sources. With all the model improvements, both the process-based and observation-constrained SOA schemes can reproduce the observed mass concentrations of SOA and show spatial and seasonal consistency with each other. Our best model simulations suggest that anthropogenic SVOCs and IVOCs are the dominant source of SOA, with a contribution of over 50% in most of China, which should be considered for pollution mitigation in the future. The residential sector may be the predominant source of SVOCs and IVOCs in winter, despite large uncertainty remaining in the emissions of IVOCs from the residential sector in northern China. The industry sector is also an important source of IVOCs, especially in summer. More SVOC and IVOC measurements are needed to constrain their emissions. Besides, the results highlight the sensitivity of SOA to hydroxyl radical (OH) levels in winter in polluted environments. The addition of nitrous acid sources can lead to over 30% greater SOA mass concentrations in winter in northern China. It is important to have good OH simulations in air quality models.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1832987

Report Number(s):: PNNL-SA--164911

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 21 Vol. 21; ISSN 1680-7324

Publisher:: Copernicus Publications, EGUCopyright Statement

Country of Publication:: United States

Language:: English

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Submicron aerosol composition in the world's most polluted megacity: the Delhi Aerosol Supersite study Gani, Shahzad; Bhandari, Sahil; Seraj, Sarah Atmospheric Chemistry and Physics, Vol. 19, Issue 10 https://doi.org/10.5194/acp-19-6843-2019	journal	January 2019
Secondary organic aerosol enhanced by increasing atmospheric oxidizing capacity in Beijing–Tianjin–Hebei (BTH), China Feng, Tian; Zhao, Shuyu; Bei, Naifang Atmospheric Chemistry and Physics, Vol. 19, Issue 11 https://doi.org/10.5194/acp-19-7429-2019	journal	January 2019
Emission of trace gases and aerosols from biomass burning – an updated assessment Andreae, Meinrat O. Atmospheric Chemistry and Physics, Vol. 19, Issue 13 https://doi.org/10.5194/acp-19-8523-2019	journal	January 2019
Persistent growth of anthropogenic non-methane volatile organic compound (NMVOC) emissions in China during 1990–2017: drivers, speciation and ozone formation potential Li, Meng; Zhang, Qiang; Zheng, Bo Atmospheric Chemistry and Physics, Vol. 19, Issue 13 https://doi.org/10.5194/acp-19-8897-2019	journal	January 2019
Formation and sink of glyoxal and methylglyoxal in a polluted subtropical environment: observation-based photochemical analysis and impact evaluation Ling, Zhenhao; Xie, Qianqian; Shao, Min Atmospheric Chemistry and Physics, Vol. 20, Issue 19 https://doi.org/10.5194/acp-20-11451-2020	journal	January 2020
Observationally constrained modeling of atmospheric oxidation capacity and photochemical reactivity in Shanghai, China Zhu, Jian; Wang, Shanshan; Wang, Hongli Atmospheric Chemistry and Physics, Vol. 20, Issue 3 https://doi.org/10.5194/acp-20-1217-2020	journal	January 2020
Model bias in simulating major chemical components of PM_2.5 in China Miao, Ruqian; Chen, Qi; Zheng, Yan Atmospheric Chemistry and Physics, Vol. 20, Issue 20 https://doi.org/10.5194/acp-20-12265-2020	journal	January 2020
Correcting model biases of CO in East Asia: impact on oxidant distributions during KORUS-AQ Gaubert, Benjamin; Emmons, Louisa K.; Raeder, Kevin Atmospheric Chemistry and Physics, Vol. 20, Issue 23 https://doi.org/10.5194/acp-20-14617-2020	journal	January 2020
Elevated levels of OH observed in haze events during wintertime in central Beijing Slater, Eloise J.; Whalley, Lisa K.; Woodward-Massey, Robert Atmospheric Chemistry and Physics, Vol. 20, Issue 23 https://doi.org/10.5194/acp-20-14847-2020	journal	January 2020
Evaluation and uncertainty investigation of the NO₂, CO and NH₃ modeling over China under the framework of MICS-Asia III Kong, Lei; Tang, Xiao; Zhu, Jiang Atmospheric Chemistry and Physics, Vol. 20, Issue 1 https://doi.org/10.5194/acp-20-181-2020	journal	January 2020
An evaluation of global organic aerosol schemes using airborne observations Pai, Sidhant J.; Heald, Colette L.; Pierce, Jeffrey R. Atmospheric Chemistry and Physics, Vol. 20, Issue 5 https://doi.org/10.5194/acp-20-2637-2020	journal	January 2020
Summertime and wintertime atmospheric processes of secondary aerosol in Beijing Duan, Jing; Huang, Ru-Jin; Li, Yongjie Atmospheric Chemistry and Physics, Vol. 20, Issue 6 https://doi.org/10.5194/acp-20-3793-2020	journal	January 2020
Simulation of organic aerosol formation during the CalNex study: updated mobile emissions and secondary organic aerosol parameterization for intermediate-volatility organic compounds Lu, Quanyang; Murphy, Benjamin N.; Qin, Momei Atmospheric Chemistry and Physics, Vol. 20, Issue 7 https://doi.org/10.5194/acp-20-4313-2020	journal	January 2020
Contribution of nitrous acid to the atmospheric oxidation capacity in an industrial zone in the Yangtze River Delta region of China Zheng, Jun; Shi, Xiaowen; Ma, Yan Atmospheric Chemistry and Physics, Vol. 20, Issue 9 https://doi.org/10.5194/acp-20-5457-2020	journal	January 2020
Evaluating the sensitivity of radical chemistry and ozone formation to ambient VOCs and NO_x in Beijing Whalley, Lisa K.; Slater, Eloise J.; Woodward-Massey, Robert Atmospheric Chemistry and Physics, Vol. 21, Issue 3 https://doi.org/10.5194/acp-21-2125-2021	journal	January 2021
Organic aerosol volatility and viscosity in the North China Plain: contrast between summer and winter Xu, Weiqi; Chen, Chun; Qiu, Yanmei Atmospheric Chemistry and Physics, Vol. 21, Issue 7 https://doi.org/10.5194/acp-21-5463-2021	journal	January 2021
ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K⁺–Ca²⁺–Mg²⁺–NH₄⁺–Na⁺–SO₄²⁻–NO₃⁻–Cl⁻–H₂O aerosols Fountoukis, C.; Nenes, A. Atmospheric Chemistry and Physics, Vol. 7, Issue 17 https://doi.org/10.5194/acp-7-4639-2007	journal	January 2007
Laboratory investigation of photochemical oxidation of organic aerosol from wood fires 1: measurement and simulation of organic aerosol evolution Grieshop, A. P.; Logue, J. M.; Donahue, N. M. Atmospheric Chemistry and Physics, Vol. 9, Issue 4 https://doi.org/10.5194/acp-9-1263-2009	journal	January 2009
Secondary organic aerosol formation from photooxidation of naphthalene and alkylnaphthalenes: implications for oxidation of intermediate volatility organic compounds (IVOCs) Chan, A. W. H.; Kautzman, K. E.; Chhabra, P. S. Atmospheric Chemistry and Physics, Vol. 9, Issue 9 https://doi.org/10.5194/acp-9-3049-2009	journal	January 2009
Characterization of anthropogenic organic aerosols by TOF-ACSM with the new capture vaporizer Zheng, Yan; Cheng, Xi; Liao, Keren Atmospheric Measurement Techniques, Vol. 13, Issue 5 https://doi.org/10.5194/amt-13-2457-2020	journal	January 2020
Changes in China's anthropogenic emissions and air quality during the COVID-19 pandemic in 2020 Zheng, Bo; Zhang, Qiang; Geng, Guannan Earth System Science Data, Vol. 13, Issue 6 https://doi.org/10.5194/essd-13-2895-2021	journal	January 2021
Historical (1750–2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS) Hoesly, Rachel M.; Smith, Steven J.; Feng, Leyang Geoscientific Model Development, Vol. 11, Issue 1 https://doi.org/10.5194/gmd-11-369-2018	journal	January 2018
Mechanistic representation of soil nitrogen emissions in the Community Multiscale Air Quality (CMAQ) model v 5.1 Rasool, Quazi Z.; Bash, Jesse O.; Cohan, Daniel S. Geoscientific Model Development, Vol. 12, Issue 2 https://doi.org/10.5194/gmd-12-849-2019	journal	January 2019
Modeling anthropogenically controlled secondary organic aerosols in a megacity: a simplified framework for global and climate models Hodzic, A.; Jimenez, J. L. Geoscientific Model Development, Vol. 4, Issue 4 https://doi.org/10.5194/gmd-4-901-2011	journal	January 2011
The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions Guenther, A. B.; Jiang, X.; Heald, C. L. Geoscientific Model Development, Vol. 5, Issue 6 https://doi.org/10.5194/gmd-5-1471-2012	journal	January 2012
A gridded emission inventory of semi-volatile and intermediate volatility organic compounds in China Wu, Liqing; Ling, Zhenhao; Wang, Xuemei Science Data Bank https://doi.org/10.57760/sciencedb.00109	dataset	January 2020
Trends in China’s anthropogenic emissions since 2010 as the consequence of clean air actions Zheng, Bo; Tong, Dan; Li, Meng figshare https://doi.org/10.6084/m9.figshare.7028249.v4	dataset	January 2018

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