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

Abstract

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 (PM2.5) 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 ofmore » sulfate and nitrate, but also reproduces the enhancement of relative contribution of sulfate and nitrate to PM2.5 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.« less

Authors:
 [1];  [2];  [3];  [4];  [5];  [1];  [1];  [1]; ORCiD logo [6]
  1. Tsinghua Univ., Beijing (China)
  2. Collaborative Innovation Center for Regional Environmental Quality, Beijing (China); Tsinghua Univ., Beijing (China)
  3. Collaborative Innovation Center for Regional Environmental Quality, Beijing (China); North Carolina State Univ., Raleigh, NC (United States); Tsinghua Univ., Beijing (China)
  4. 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)
  5. North Carolina State Univ., Raleigh, NC (United States)
  6. Kimoto Electric Co., Ltd., Osaka (Japan)
Publication Date:
Research Org.:
North Carolina State University, Raleigh, NC (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1452792
Grant/Contract Number:  
SC0006695
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 15; Journal Issue: 4; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zheng, B., Zhang, Q., Zhang, Y., He, K. B., Wang, K., Zheng, G. J., Duan, F. K., Ma, Y. L., and Kimoto, T. Heterogeneous chemistry: a mechanism missing in current models to explain secondary inorganic aerosol formation during the January 2013 haze episode in North China. United States: N. p., 2015. Web. doi:10.5194/acp-15-2031-2015.
Zheng, B., Zhang, Q., Zhang, Y., He, K. B., Wang, K., Zheng, G. J., Duan, F. K., Ma, Y. L., & Kimoto, T. Heterogeneous chemistry: a mechanism missing in current models to explain secondary inorganic aerosol formation during the January 2013 haze episode in North China. United States. https://doi.org/10.5194/acp-15-2031-2015
Zheng, B., Zhang, Q., Zhang, Y., He, K. B., Wang, K., Zheng, G. J., Duan, F. K., Ma, Y. L., and Kimoto, T. Wed . "Heterogeneous chemistry: a mechanism missing in current models to explain secondary inorganic aerosol formation during the January 2013 haze episode in North China". United States. https://doi.org/10.5194/acp-15-2031-2015. https://www.osti.gov/servlets/purl/1452792.
@article{osti_1452792,
title = {Heterogeneous chemistry: a mechanism missing in current models to explain secondary inorganic aerosol formation during the January 2013 haze episode in North China},
author = {Zheng, B. and Zhang, Q. and Zhang, Y. and He, K. B. and Wang, K. and Zheng, G. J. and Duan, F. K. and Ma, Y. L. and Kimoto, T.},
abstractNote = {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 (PM2.5) 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 PM2.5 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.},
doi = {10.5194/acp-15-2031-2015},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 4,
volume = 15,
place = {United States},
year = {Wed Feb 25 00:00:00 EST 2015},
month = {Wed Feb 25 00:00:00 EST 2015}
}

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Relative humidity and O3 concentration as two prerequisites for sulfate formation
journal, January 2019

  • Fang, Yanhua; Ye, Chunxiang; Wang, Junxia
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 19
  • DOI: 10.5194/acp-19-12295-2019

Possible heterogeneous chemistry of hydroxymethanesulfonate (HMS) in northern China winter haze
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
journal, January 2019


Unraveling the role of silicon in atmospheric aerosol secondary formation: a new conservative tracer for aerosol chemistry
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
journal, January 2019

  • Cheng, Jing; Su, Jingping; Cui, Tong
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 9
  • DOI: 10.5194/acp-19-6125-2019

Significant source of secondary aerosol: formation from gasoline evaporative emissions in the presence of SO 2 and NH 3
journal, January 2019

  • Chen, Tianzeng; Liu, Yongchun; Ma, Qingxin
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 12
  • DOI: 10.5194/acp-19-8063-2019

IAP-AACM v1.0: a global to regional evaluation of the atmospheric chemistry model in CAS-ESM
journal, January 2019

  • Wei, Ying; Chen, Xueshun; Chen, Huansheng
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 12
  • DOI: 10.5194/acp-19-8269-2019

The 2015 and 2016 wintertime air pollution in China: SO 2 emission changes derived from a WRF-Chem/EnKF coupled data assimilation system
journal, January 2019

  • Chen, Dan; Liu, Zhiquan; Ban, Junmei
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 13
  • DOI: 10.5194/acp-19-8619-2019

Photochemical impacts of haze pollution in an urban environment
journal, January 2019

  • Hollaway, Michael; Wild, Oliver; Yang, Ting
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 15
  • DOI: 10.5194/acp-19-9699-2019

Large contributions of biogenic and anthropogenic sources to fine organic aerosols in Tianjin, North China
journal, January 2020

  • Fan, Yanbing; Liu, Cong-Qiang; Li, Linjie
  • Atmospheric Chemistry and Physics, Vol. 20, Issue 1
  • DOI: 10.5194/acp-20-117-2020

Significant contribution of organics to aerosol liquid water content in winter in Beijing, China
journal, January 2020

  • Jin, Xiaoai; Wang, Yuying; Li, Zhanqing
  • Atmospheric Chemistry and Physics, Vol. 20, Issue 2
  • DOI: 10.5194/acp-20-901-2020

Ensemble forecasts of air quality in eastern China – Part 1: Model description and implementation of the MarcoPolo–Panda prediction system, version 1
journal, January 2019

  • Brasseur, Guy P.; Xie, Ying; Petersen, Anna Katinka
  • Geoscientific Model Development, Vol. 12, Issue 1
  • DOI: 10.5194/gmd-12-33-2019

Enhanced sulfate formation by nitrogen dioxide: Implications from in situ observations at the SORPES station: Sulfate Formation by Nitrogen Dioxide
journal, December 2015

  • Xie, Yuning; Ding, Aijun; Nie, Wei
  • Journal of Geophysical Research: Atmospheres, Vol. 120, Issue 24
  • DOI: 10.1002/2015jd023607

Secondary aerosol formation and oxidation capacity in photooxidation in the presence of Al2O3 seed particles and SO2
journal, July 2015


Air quality and health benefits of China’s emission control policies on coal-fired power plants during 2005–2020
journal, September 2019


Air quality and health impacts from the updated industrial emission standards in China
journal, December 2019


A Review of Aerosol Chemical Composition and Sources in Representative Regions of China during Wintertime
journal, May 2019


Intermittent turbulence contributes to vertical dispersion of PM2.5 in the North China Plain: cases from Tianjin
journal, January 2018


The impact of multi-species surface chemical observation assimilation on air quality forecasts in China
journal, January 2018


Fine particulate matter (PM 2.5 ) trends in China, 2013–2018: separating contributions from anthropogenic emissions and meteorology
journal, January 2019

  • Zhai, Shixian; Jacob, Daniel J.; Wang, Xuan
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 16
  • DOI: 10.5194/acp-19-11031-2019

Rapid transition in winter aerosol composition in Beijing from 2014 to 2017: response to clean air actions
journal, January 2019


Spatiotemporal variability of NO2 and PM2.5 over Eastern China: observational and model analyses with a novel statistical method
posted_content, March 2018

  • Liu, Mengyao; Lin, Jintai; Wang, Yuchen
  • Atmospheric Chemistry and Physics Discussions
  • DOI: 10.5194/acp-2017-1180

Characterization of organic aerosols from a Chinese Mega-City during winter: predominance of fossil fuel combustion
journal, October 2018

  • Haque, Mozammel; Kawamura, Kimitaka; Deshmukh, Dhananjay K.
  • Atmospheric Chemistry and Physics Discussions
  • DOI: 10.5194/acp-2018-969

Photochemical impacts of haze pollution in an urban environment
posted_content, January 2019

  • Hollaway, Michael; Wild, Oliver; Yang, Ting
  • Atmospheric Chemistry and Physics
  • DOI: 10.5194/acp-2019-29

Significant contribution of organics to aerosol liquid water content in winter in Beijing, China
posted_content, July 2019

  • Jin, Xiaoai; Wang, Yuying; Li, Zhanqing
  • Atmospheric Chemistry and Physics Discussions
  • DOI: 10.5194/acp-2019-503

Organic Aerosol Processing During Winter Severe Haze Episodes in Beijing
journal, September 2019

  • Zhao, Jian; Qiu, Yanmei; Zhou, Wei
  • Journal of Geophysical Research: Atmospheres, Vol. 124, Issue 17-18
  • DOI: 10.1029/2019jd030832

New positive feedback mechanism between boundary layer meteorology and secondary aerosol formation during severe haze events
journal, April 2018


Evidence of heterogeneous HONO formation from aerosols and the regional photochemical impact of this HONO source
journal, October 2018

  • Lu, Xingcheng; Wang, Yuhang; Li, Jianfeng
  • Environmental Research Letters, Vol. 13, Issue 11
  • DOI: 10.1088/1748-9326/aae492

Spatiotemporal variability of NO2 and PM2.5 over Eastern China: observational and model analyses with a novel statistical method
journal, January 2018

  • Liu, Mengyao; Lin, Jintai; Wang, Yuchen
  • Atmospheric Chemistry and Physics, Vol. 18, Issue 17
  • DOI: 10.5194/acp-18-12933-2018

MICS-Asia III: multi-model comparison and evaluation of aerosol over East Asia
journal, January 2019


Atmospheric Δ17O(NO3) reveals nocturnal chemistry dominates nitrate production in Beijing haze
posted_content, May 2018

  • He, Pengzhen; Xie, Zhouqing; Chi, Xiyuan
  • Atmospheric Chemistry and Physics Discussions
  • DOI: 10.5194/acp-2018-334

Unraveling the role of silicon in atmospheric aerosol secondary formation: A new conservative tracer for aerosol chemistry
journal, November 2018

  • Lu, Dawei; Tan, Jihua; Yang, Xuezhi
  • Atmospheric Chemistry and Physics Discussions
  • DOI: 10.5194/acp-2018-914

Characterization of organic aerosols from a Chinese megacity during winter: predominance of fossil fuel combustion
journal, January 2019

  • Haque, Md. Mozammel; Kawamura, Kimitaka; Deshmukh, Dhananjay K.
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 7
  • DOI: 10.5194/acp-19-5147-2019

A Review of the Representation of Aerosol Mixing State in Atmospheric Models
journal, March 2019


Modeling study of the 2010 regional haze event in the North China Plain
posted_content, August 2015


Vertical Characterization of Aerosol Particle Composition in Beijing, China: Insights From 3‐Month Measurements With Two Aerosol Mass Spectrometers
journal, November 2018

  • Zhou, Wei; Sun, Yele; Xu, Weiqi
  • Journal of Geophysical Research: Atmospheres, Vol. 123, Issue 22
  • DOI: 10.1029/2018jd029337

Nitrate-driven urban haze pollution during summertime over the North China Plain
journal, January 2018


One-Year Simulation of Ozone and Particulate Matter in China Using WRF/CMAQ Modeling System
posted_content, April 2016

  • Hu, Jianlin; Chen, Jianjun; Ying, Qi
  • Atmospheric Chemistry and Physics Discussions
  • DOI: 10.5194/acp-2016-148

Rapid transition in winter aerosol composition in Beijing from 2014 to 2017: response to clean air actions
posted_content, May 2019

  • Li, Haiyan; Cheng, Jing; Zhang, Qiang
  • Atmospheric Chemistry and Physics Discussions
  • DOI: 10.5194/acp-2019-450

Examining the physical and chemical contributions to size spectrum evolution during the development of hazes
journal, March 2020


Source Contributions of PM2.5in the Severe Haze Episode in Hebei Cities
journal, January 2015

  • Wei, Zhe; Wang, Litao; Ma, Simeng
  • The Scientific World Journal, Vol. 2015
  • DOI: 10.1155/2015/480542