Heterogeneous chemistry: a mechanism missing in current models to explain secondary inorganic aerosol formation during the January 2013 haze episode in North China

Zheng, B.; Zhang, Q.; Zhang, Y.; He, K. B.; Wang, K.; Zheng, G. J.; Duan, F. K.; Ma, Y. L.; Kimoto, T.

doi:10.5194/acp-15-2031-2015

Title: Heterogeneous chemistry: a mechanism missing in current models to explain secondary inorganic aerosol formation during the January 2013 haze episode in North China

Journal Article · Wed Feb 25 00:00:00 EST 2015 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-15-2031-2015· OSTI ID:1452792

Zheng, B. ^[1]; Zhang, Q. ^[2]; Zhang, Y. ^[3]; He, K. B. ^[4]; Wang, K. ^[5]; Zheng, G. J. ^[1]; Duan, F. K. ^[1]; Ma, Y. L. ^[1];

^[6]

Tsinghua Univ., Beijing (China)
Collaborative Innovation Center for Regional Environmental Quality, Beijing (China); Tsinghua Univ., Beijing (China)
Collaborative Innovation Center for Regional Environmental Quality, Beijing (China); North Carolina State Univ., Raleigh, NC (United States); Tsinghua Univ., Beijing (China)
Collaborative Innovation Center for Regional Environmental Quality, Beijing (China); State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex, Beijing (China); Tsinghua Univ., Beijing (China)
North Carolina State Univ., Raleigh, NC (United States)
Kimoto Electric Co., Ltd., Osaka (Japan)

Severe regional haze pollution events occurred in eastern and central China in January 2013, which had adverse effects on the environment and public health. Extremely high levels of particulate matter with aerodynamic diameter of 2.5 μm or less (PM_2.5) with dominant components of sulfate and nitrate are responsible for the haze pollution. Although heterogeneous chemistry is thought to play an important role in the production of sulfate and nitrate during haze episodes, few studies have comprehensively evaluated the effect of heterogeneous chemistry on haze formation in China by using the 3-D models due to of a lack of treatments for heterogeneous reactions in most climate and chemical transport models. In this work, the WRF-CMAQ model with newly added heterogeneous reactions is applied to East Asia to evaluate the impacts of heterogeneous chemistry and the meteorological anomaly during January 2013 on regional haze formation. As the parameterization of heterogeneous reactions on different types of particles is not well established yet, we arbitrarily selected the uptake coefficients from reactions on dust particles and then conducted several sensitivity runs to find the value that can best match observations. The revised CMAQ with heterogeneous chemistry not only captures the magnitude and temporal variation of sulfate and nitrate, but also reproduces the enhancement of relative contribution of sulfate and nitrate to PM_2.5 mass from clean days to polluted haze days. Finally, these results indicate the significant role of heterogeneous chemistry in regional haze formation and improve the understanding of the haze formation mechanisms during the January 2013 episode.

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Research Organization:: North Carolina State University, Raleigh, NC (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0006695

OSTI ID:: 1452792

Journal Information:: Atmospheric Chemistry and Physics (Online), Vol. 15, Issue 4; ISSN 1680-7324

Publisher:: European Geosciences UnionCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 424 works

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The possible contribution of the periodic emissions from farmers' activities in the North China Plain to atmospheric water-soluble ions in Beijing Liu, Pengfei; Zhang, Chenglong; Mu, Yujing Atmospheric Chemistry and Physics, Vol. 16, Issue 15 https://doi.org/10.5194/acp-16-10097-2016	journal	January 2016
One-year simulation of ozone and particulate matter in China using WRF/CMAQ modeling system Hu, Jianlin; Chen, Jianjun; Ying, Qi Atmospheric Chemistry and Physics, Vol. 16, Issue 16 https://doi.org/10.5194/acp-16-10333-2016	journal	January 2016
Simulations of sulfate–nitrate–ammonium (SNA) aerosols during the extreme haze events over northern China in October 2014 Chen, Dan; Liu, Zhiquan; Fast, Jerome Atmospheric Chemistry and Physics, Vol. 16, Issue 16 https://doi.org/10.5194/acp-16-10707-2016	journal	January 2016
Modeling study of the 2010 regional haze event in the North China Plain Gao, M.; Carmichael, G. R.; Wang, Y. Atmospheric Chemistry and Physics, Vol. 16, Issue 3 https://doi.org/10.5194/acp-16-1673-2016	journal	January 2016
The contribution of residential coal combustion to atmospheric PM _2. 5 in northern China during winter Liu, Pengfei; Zhang, Chenglong; Xue, Chaoyang Atmospheric Chemistry and Physics, Vol. 17, Issue 18 https://doi.org/10.5194/acp-17-11503-2017	journal	January 2017
Improving PM_2. 5 forecast over China by the joint adjustment of initial conditions and source emissions with an ensemble Kalman filter Peng, Zhen; Liu, Zhiquan; Chen, Dan Atmospheric Chemistry and Physics, Vol. 17, Issue 7 https://doi.org/10.5194/acp-17-4837-2017	journal	January 2017
Chemical composition of ambient PM _2. 5 over China and relationship to precursor emissions during 2005–2012 Geng, Guannan; Zhang, Qiang; Tong, Dan Atmospheric Chemistry and Physics, Vol. 17, Issue 14 https://doi.org/10.5194/acp-17-9187-2017	journal	January 2017
Resolution dependence of uncertainties in gridded emission inventories: a case study in Hebei, China Zheng, Bo; Zhang, Qiang; Tong, Dan Atmospheric Chemistry and Physics, Vol. 17, Issue 2 https://doi.org/10.5194/acp-17-921-2017	journal	January 2017
Changes in the aerosol direct radiative forcing from 2001 to 2015: observational constraints and regional mechanisms Paulot, Fabien; Paynter, David; Ginoux, Paul Atmospheric Chemistry and Physics, Vol. 18, Issue 17 https://doi.org/10.5194/acp-18-13265-2018	journal	January 2018
Emission or atmospheric processes? An attempt to attribute the source of large bias of aerosols in eastern China simulated by global climate models Fan, Tianyi; Liu, Xiaohong; Ma, Po-Lun Atmospheric Chemistry and Physics, Vol. 18, Issue 2 https://doi.org/10.5194/acp-18-1395-2018	journal	January 2018
Atmospheric Δ¹⁷O(NO₃⁻) reveals nocturnal chemistry dominates nitrate production in Beijing haze He, Pengzhen; Xie, Zhouqing; Chi, Xiyuan Atmospheric Chemistry and Physics, Vol. 18, Issue 19 https://doi.org/10.5194/acp-18-14465-2018	journal	January 2018
Is there an aerosol signature of chemical cloud processing? Ervens, Barbara; Sorooshian, Armin; Aldhaif, Abdulmonam M. Atmospheric Chemistry and Physics, Vol. 18, Issue 21 https://doi.org/10.5194/acp-18-16099-2018	journal	January 2018
Feedback effects of boundary-layer meteorological factors on cumulative explosive growth of PM _2.5 during winter heavy pollution episodes in Beijing from 2013 to 2016 Zhong, Junting; Zhang, Xiaoye; Dong, Yunsheng Atmospheric Chemistry and Physics, Vol. 18, Issue 1 https://doi.org/10.5194/acp-18-247-2018	journal	January 2018
Multiphase oxidation of SO 2 by NO 2 on CaCO 3 particles Zhao, Defeng; Song, Xiaojuan; Zhu, Tong Atmospheric Chemistry and Physics, Vol. 18, Issue 4 https://doi.org/10.5194/acp-18-2481-2018	journal	January 2018
Vertically resolved characteristics of air pollution during two severe winter haze episodes in urban Beijing, China Wang, Qingqing; Sun, Yele; Xu, Weiqi Atmospheric Chemistry and Physics, Vol. 18, Issue 4 https://doi.org/10.5194/acp-18-2495-2018	journal	January 2018
Air quality and climate change, Topic 3 of the Model Inter-Comparison Study for Asia Phase III (MICS-Asia III) – Part 1: Overview and model evaluation Gao, Meng; Han, Zhiwei; Liu, Zirui Atmospheric Chemistry and Physics, Vol. 18, Issue 7 https://doi.org/10.5194/acp-18-4859-2018	journal	January 2018
Isotopic constraints on heterogeneous sulfate production in Beijing haze He, Pengzhen; Alexander, Becky; Geng, Lei Atmospheric Chemistry and Physics, Vol. 18, Issue 8 https://doi.org/10.5194/acp-18-5515-2018	journal	January 2018
Seasonal characteristics, formation mechanisms and source origins of PM_2.5 in two megacities in Sichuan Basin, China Wang, Huanbo; Tian, Mi; Chen, Yang Atmospheric Chemistry and Physics, Vol. 18, Issue 2 https://doi.org/10.5194/acp-18-865-2018	journal	January 2018
Characteristics of marine shipping emissions at berth: profiles for particulate matter and volatile organic compounds Xiao, Qian; Li, Mei; Liu, Huan Atmospheric Chemistry and Physics, Vol. 18, Issue 13 https://doi.org/10.5194/acp-18-9527-2018	journal	January 2018
Relative importance of gas uptake on aerosol and ground surfaces characterized by equivalent uptake coefficients Li, Meng; Su, Hang; Li, Guo Atmospheric Chemistry and Physics, Vol. 19, Issue 16 https://doi.org/10.5194/acp-19-10981-2019	journal	January 2019
Atmospheric new particle formation in China Chu, Biwu; Kerminen, Veli-Matti; Bianchi, Federico Atmospheric Chemistry and Physics, Vol. 19, Issue 1 https://doi.org/10.5194/acp-19-115-2019	journal	January 2019
Relative humidity and O₃ concentration as two prerequisites for sulfate formation Fang, Yanhua; Ye, Chunxiang; Wang, Junxia Atmospheric Chemistry and Physics, Vol. 19, Issue 19 https://doi.org/10.5194/acp-19-12295-2019	journal	January 2019
Possible heterogeneous chemistry of hydroxymethanesulfonate (HMS) in northern China winter haze Song, Shaojie; Gao, Meng; Xu, Weiqi Atmospheric Chemistry and Physics, Vol. 19, Issue 2 https://doi.org/10.5194/acp-19-1357-2019	journal	January 2019
Sulfate formation during heavy winter haze events and the potential contribution from heterogeneous SO₂ + NO₂ reactions in the Yangtze River Delta region, China Huang, Ling; An, Jingyu; Koo, Bonyoung Atmospheric Chemistry and Physics, Vol. 19, Issue 22 https://doi.org/10.5194/acp-19-14311-2019	journal	January 2019
Effects of NO₂ and C₃H₆ on the heterogeneous oxidation of SO₂ on TiO₂ in the presence or absence of UV–Vis irradiation Chu, Biwu; Wang, Yali; Yang, Weiwei Atmospheric Chemistry and Physics, Vol. 19, Issue 23 https://doi.org/10.5194/acp-19-14777-2019	journal	January 2019
Unraveling the role of silicon in atmospheric aerosol secondary formation: a new conservative tracer for aerosol chemistry Lu, Dawei; Tan, Jihua; Yang, Xuezhi Atmospheric Chemistry and Physics, Vol. 19, Issue 5 https://doi.org/10.5194/acp-19-2861-2019	journal	January 2019
Heterogeneous sulfate aerosol formation mechanisms during wintertime Chinese haze events: air quality model assessment using observations of sulfate oxygen isotopes in Beijing Shao, Jingyuan; Chen, Qianjie; Wang, Yuxuan Atmospheric Chemistry and Physics, Vol. 19, Issue 9 https://doi.org/10.5194/acp-19-6107-2019	journal	January 2019
Dominant role of emission reduction in PM 2.5 air quality improvement in Beijing during 2013–2017: a model-based decomposition analysis Cheng, Jing; Su, Jingping; Cui, Tong Atmospheric Chemistry and Physics, Vol. 19, Issue 9 https://doi.org/10.5194/acp-19-6125-2019	journal	January 2019
Significant source of secondary aerosol: formation from gasoline evaporative emissions in the presence of SO 2 and NH 3 Chen, Tianzeng; Liu, Yongchun; Ma, Qingxin Atmospheric Chemistry and Physics, Vol. 19, Issue 12 https://doi.org/10.5194/acp-19-8063-2019	journal	January 2019
Effects of organic coating on the nitrate formation by suppressing the N 2 O 5 heterogeneous hydrolysis: a case study during wintertime in Beijing–Tianjin–Hebei (BTH) Liu, Lang; Wu, Jiarui; Liu, Suixin Atmospheric Chemistry and Physics, Vol. 19, Issue 12 https://doi.org/10.5194/acp-19-8189-2019	journal	January 2019
IAP-AACM v1.0: a global to regional evaluation of the atmospheric chemistry model in CAS-ESM Wei, Ying; Chen, Xueshun; Chen, Huansheng Atmospheric Chemistry and Physics, Vol. 19, Issue 12 https://doi.org/10.5194/acp-19-8269-2019	journal	January 2019
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Evaluation of the effect of regional joint-control measures on changing photochemical transformation: a comprehensive study of the optimization scenario analysis Li, Li; Zhu, Shuhui; An, Jingyu Atmospheric Chemistry and Physics, Vol. 19, Issue 14 https://doi.org/10.5194/acp-19-9037-2019	journal	January 2019
Photochemical impacts of haze pollution in an urban environment Hollaway, Michael; Wild, Oliver; Yang, Ting Atmospheric Chemistry and Physics, Vol. 19, Issue 15 https://doi.org/10.5194/acp-19-9699-2019	journal	January 2019
Large contributions of biogenic and anthropogenic sources to fine organic aerosols in Tianjin, North China Fan, Yanbing; Liu, Cong-Qiang; Li, Linjie Atmospheric Chemistry and Physics, Vol. 20, Issue 1 https://doi.org/10.5194/acp-20-117-2020	journal	January 2020
Significant contribution of organics to aerosol liquid water content in winter in Beijing, China Jin, Xiaoai; Wang, Yuying; Li, Zhanqing Atmospheric Chemistry and Physics, Vol. 20, Issue 2 https://doi.org/10.5194/acp-20-901-2020	journal	January 2020
Ensemble forecasts of air quality in eastern China – Part 1: Model description and implementation of the MarcoPolo–Panda prediction system, version 1 Brasseur, Guy P.; Xie, Ying; Petersen, Anna Katinka Geoscientific Model Development, Vol. 12, Issue 1 https://doi.org/10.5194/gmd-12-33-2019	journal	January 2019
Enhanced sulfate formation by nitrogen dioxide: Implications from in situ observations at the SORPES station: Sulfate Formation by Nitrogen Dioxide Xie, Yuning; Ding, Aijun; Nie, Wei Journal of Geophysical Research: Atmospheres, Vol. 120, Issue 24 https://doi.org/10.1002/2015jd023607	journal	December 2015
Secondary aerosol formation and oxidation capacity in photooxidation in the presence of Al2O3 seed particles and SO2 Chu, Biwu; Liu, Tengyu; Zhang, Xiao Science China Chemistry, Vol. 58, Issue 9 https://doi.org/10.1007/s11426-015-5456-0	journal	July 2015
Air quality and health benefits of China’s emission control policies on coal-fired power plants during 2005–2020 Wu, Ruili; Liu, Fei; Tong, Dan Environmental Research Letters, Vol. 14, Issue 9 https://doi.org/10.1088/1748-9326/ab3bae	journal	September 2019
Air quality and health impacts from the updated industrial emission standards in China Yang, Haozhe; Tao, Wei; Wang, Yuqing Environmental Research Letters, Vol. 14, Issue 12 https://doi.org/10.1088/1748-9326/ab54fa	journal	December 2019
A Review of Aerosol Chemical Composition and Sources in Representative Regions of China during Wintertime Wang, Yichen; Wang, Qiyuan; Ye, Jianhuai Atmosphere, Vol. 10, Issue 5 https://doi.org/10.3390/atmos10050277	journal	May 2019
Intermittent turbulence contributes to vertical dispersion of PM_2.5 in the North China Plain: cases from Tianjin Wei, Wei; Zhang, Hongsheng; Wu, Bingui Atmospheric Chemistry and Physics, Vol. 18, Issue 17 https://doi.org/10.5194/acp-18-12953-2018	journal	January 2018
The impact of multi-species surface chemical observation assimilation on air quality forecasts in China Peng, Zhen; Lei, Lili; Liu, Zhiquan Atmospheric Chemistry and Physics, Vol. 18, Issue 23 https://doi.org/10.5194/acp-18-17387-2018	journal	January 2018
Fine particulate matter (PM 2.5 ) trends in China, 2013–2018: separating contributions from anthropogenic emissions and meteorology Zhai, Shixian; Jacob, Daniel J.; Wang, Xuan Atmospheric Chemistry and Physics, Vol. 19, Issue 16 https://doi.org/10.5194/acp-19-11031-2019	journal	January 2019
Rapid transition in winter aerosol composition in Beijing from 2014 to 2017: response to clean air actions Li, Haiyan; Cheng, Jing; Zhang, Qiang Atmospheric Chemistry and Physics, Vol. 19, Issue 17 https://doi.org/10.5194/acp-19-11485-2019	journal	January 2019
Spatiotemporal variability of NO₂ and PM_2.5 over Eastern China: observational and model analyses with a novel statistical method Liu, Mengyao; Lin, Jintai; Wang, Yuchen Atmospheric Chemistry and Physics Discussions https://doi.org/10.5194/acp-2017-1180	posted_content	March 2018
Characterization of organic aerosols from a Chinese Mega-City during winter: predominance of fossil fuel combustion Haque, Mozammel; Kawamura, Kimitaka; Deshmukh, Dhananjay K. Atmospheric Chemistry and Physics Discussions https://doi.org/10.5194/acp-2018-969	journal	October 2018
Photochemical impacts of haze pollution in an urban environment Hollaway, Michael; Wild, Oliver; Yang, Ting Atmospheric Chemistry and Physics https://doi.org/10.5194/acp-2019-29	posted_content	January 2019
Significant contribution of organics to aerosol liquid water content in winter in Beijing, China Jin, Xiaoai; Wang, Yuying; Li, Zhanqing Atmospheric Chemistry and Physics Discussions https://doi.org/10.5194/acp-2019-503	posted_content	July 2019
Organic Aerosol Processing During Winter Severe Haze Episodes in Beijing Zhao, Jian; Qiu, Yanmei; Zhou, Wei Journal of Geophysical Research: Atmospheres, Vol. 124, Issue 17-18 https://doi.org/10.1029/2019jd030832	journal	September 2019
New positive feedback mechanism between boundary layer meteorology and secondary aerosol formation during severe haze events Liu, Quan; Jia, Xingcan; Quan, Jiannong Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-018-24366-3	journal	April 2018
Effect of model errors in ambient air humidity on the aerosol optical depth obtained via aerosol hygroscopicity in eastern China in the Atmospheric Chemistry and Climate Model Intercomparison Project datasets Chang, Wenyuan Atmospheric and Oceanic Science Letters, Vol. 12, Issue 3 https://doi.org/10.1080/16742834.2019.1588063	journal	March 2019
Evidence of heterogeneous HONO formation from aerosols and the regional photochemical impact of this HONO source Lu, Xingcheng; Wang, Yuhang; Li, Jianfeng Environmental Research Letters, Vol. 13, Issue 11 https://doi.org/10.1088/1748-9326/aae492	journal	October 2018
Wintertime aerosol chemistry and haze evolution in an extremely polluted city of the North China Plain: significant contribution from coal and biomass combustion Li, Haiyan; Zhang, Qi; Zhang, Qiang Atmospheric Chemistry and Physics, Vol. 17, Issue 7 https://doi.org/10.5194/acp-17-4751-2017	journal	January 2017
Spatiotemporal variability of NO₂ and PM_2.5 over Eastern China: observational and model analyses with a novel statistical method Liu, Mengyao; Lin, Jintai; Wang, Yuchen Atmospheric Chemistry and Physics, Vol. 18, Issue 17 https://doi.org/10.5194/acp-18-12933-2018	journal	January 2018
MICS-Asia III: multi-model comparison and evaluation of aerosol over East Asia Chen, Lei; Gao, Yi; Zhang, Meigen Atmospheric Chemistry and Physics, Vol. 19, Issue 18 https://doi.org/10.5194/acp-19-11911-2019	journal	January 2019
Modeling of aerosol property evolution during winter haze episodes over a megacity cluster in northern China: roles of regional transport and heterogeneous reactions of SO₂ Du, Huiyun; Li, Jie; Chen, Xueshun Atmospheric Chemistry and Physics, Vol. 19, Issue 14 https://doi.org/10.5194/acp-19-9351-2019	journal	January 2019
Atmospheric Δ¹⁷O(NO₃^–) reveals nocturnal chemistry dominates nitrate production in Beijing haze He, Pengzhen; Xie, Zhouqing; Chi, Xiyuan Atmospheric Chemistry and Physics Discussions https://doi.org/10.5194/acp-2018-334	posted_content	May 2018
Unraveling the role of silicon in atmospheric aerosol secondary formation: A new conservative tracer for aerosol chemistry Lu, Dawei; Tan, Jihua; Yang, Xuezhi Atmospheric Chemistry and Physics Discussions https://doi.org/10.5194/acp-2018-914	journal	November 2018
Characterization of organic aerosols from a Chinese megacity during winter: predominance of fossil fuel combustion Haque, Md. Mozammel; Kawamura, Kimitaka; Deshmukh, Dhananjay K. Atmospheric Chemistry and Physics, Vol. 19, Issue 7 https://doi.org/10.5194/acp-19-5147-2019	journal	January 2019
A Review of the Representation of Aerosol Mixing State in Atmospheric Models Stevens, Robin; Dastoor, Ashu Atmosphere, Vol. 10, Issue 4 https://doi.org/10.3390/atmos10040168	journal	March 2019
Modeling study of the 2010 regional haze event in the North China Plain Gao, M.; Carmichael, G. R.; Wang, Y. Atmospheric Chemistry and Physics Discussions https://doi.org/10.5194/acpd-15-22781-2015	posted_content	August 2015
Vertical Characterization of Aerosol Particle Composition in Beijing, China: Insights From 3‐Month Measurements With Two Aerosol Mass Spectrometers Zhou, Wei; Sun, Yele; Xu, Weiqi Journal of Geophysical Research: Atmospheres, Vol. 123, Issue 22 https://doi.org/10.1029/2018jd029337	journal	November 2018
Nitrate-driven urban haze pollution during summertime over the North China Plain Li, Haiyan; Zhang, Qiang; Zheng, Bo Atmospheric Chemistry and Physics, Vol. 18, Issue 8 https://doi.org/10.5194/acp-18-5293-2018	journal	January 2018
One-Year Simulation of Ozone and Particulate Matter in China Using WRF/CMAQ Modeling System Hu, Jianlin; Chen, Jianjun; Ying, Qi Atmospheric Chemistry and Physics Discussions https://doi.org/10.5194/acp-2016-148	posted_content	April 2016
Rapid transition in winter aerosol composition in Beijing from 2014 to 2017: response to clean air actions Li, Haiyan; Cheng, Jing; Zhang, Qiang Atmospheric Chemistry and Physics Discussions https://doi.org/10.5194/acp-2019-450	posted_content	May 2019
Examining the physical and chemical contributions to size spectrum evolution during the development of hazes Zhang, Liyuan; Su, Junwei; Huang, Yu Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-62296-1	journal	March 2020
Source Contributions of PM_2.5in the Severe Haze Episode in Hebei Cities Wei, Zhe; Wang, Litao; Ma, Simeng The Scientific World Journal, Vol. 2015 https://doi.org/10.1155/2015/480542	journal	January 2015

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