Simulations of aerosol pH in China using WRF-Chem (v4.0): sensitivities of aerosol pH and its temporal variations during haze episodes

Ruan, Xueyin; Zhao, Chun; Zaveri, Rahul A.; He, Pengzhen; Wang, Xinming; Shao, Jingyuan; Geng, Lei

doi:10.5194/gmd-15-6143-2022

Simulations of aerosol pH in China using WRF-Chem (v4.0): sensitivities of aerosol pH and its temporal variations during haze episodes

Journal Article · Thu Aug 04 00:00:00 EDT 2022 · Geoscientific Model Development (Online)

DOI:https://doi.org/10.5194/gmd-15-6143-2022· OSTI ID:1882842

^[1]; Zhao, Chun ^[1]; ^[2]; He, Pengzhen ^[3]; ^[4]; Shao, Jingyuan ^[5]; Geng, Lei ^[1]

University of Science and Technology of China, Hefei (China)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
West Anhui University (China)
Chinese Academy of Sciences (CAS), Guangzhou (China)
Civil Aviation University of China, Tianjin (China)

Aerosol pH is a fundamental property of aerosols in terms of atmospheric chemistry and its impact on air quality, climate, and health. Precise estimation of aerosol pH in chemical transport models (CTMs) is critical for aerosol modeling and thus influences policy development that partially relies on results from model simulations. We report the Weather Research and Forecasting Model coupled with Chemistry (WRF-Chem) simulated PM_2.5 pH over China during a period with heavy haze episodes in Beijing, and explore the sensitivity of the modeled aerosol pH to factors including emissions of nonvolatile cations (NVCs) and NH₃, aerosol phase state assumption, and heterogeneous production of sulfate. We find that default WRF-Chem could predict spatial patterns of PM_2.5 pH over China similar to other CTMs, but with generally lower pH values, largely due to the underestimation of alkaline species (NVCs and NH₃) and the difference in thermodynamic treatments between different models. Increasing NH₃ emissions in the model would improve the modeled pH in comparison with offline thermodynamic model calculations of pH constrained by observations. In addition, we find that the aerosol phase state assumption and heterogeneous sulfate production are important in aerosol pH predictions for regions with low relative humidity (RH) and high anthropogenic SO₂ emissions, respectively. These factors should be better constrained in model simulations of aerosol pH in the future. Analysis of the modeled temporal trend of PM_2.5 pH in Beijing over a haze episode reveals a clear decrease in pH from 5.2 ± 0.9 in a clean period to 3.6 ± 0.5 in a heavily polluted period. The increased acidity under more polluted conditions is largely due to the formation and accumulation of secondary species including sulfuric acid and nitric acid, even though being modified by alkaline species (NVCs, NH₃). Our result suggests that NO₂ oxidation is unlikely to be important for heterogeneous sulfate production during the Beijing haze as the effective pH for NO₂ oxidation of S(IV) is at a higher pH of ~6.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center; Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: Chinese Academy of Sciences (NSFC); National Natural Science Foundation of China; Natural Science Foundation of Anhui Province; USDOE Office of Science (SC), Biological and Environmental Research (BER); West Anhui University

Contributing Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1882842

Alternate ID(s):: OSTI ID: 1882843
OSTI ID: 2229707

Report Number(s):: PNNL-SA--175015

Journal Information:: Geoscientific Model Development (Online), Journal Name: Geoscientific Model Development (Online) Journal Issue: 15 Vol. 15; ISSN 1991-9603

Publisher:: Copernicus Publications, EGUCopyright Statement

Country of Publication:: United States

Language:: English

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