Contribution of Particulate Nitrate Photolysis to Heterogeneous Sulfate Formation for Winter Haze in China,Environmental Science & Technology Letters

当前位置： X-MOL 学术 › Environ. Sci. Technol. Lett. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Contribution of Particulate Nitrate Photolysis to Heterogeneous Sulfate Formation for Winter Haze in China
Environmental Science & Technology Letters ( IF 10.9 ) Pub Date : 2020-06-25 , DOI: 10.1021/acs.estlett.0c00368
Haotian Zheng _{1,

2,

3} , Shaojie Song ₃ , Golam Sarwar ₄ , Masao Gen ₅ , Shuxiao Wang _{1,

2,

3} , Dian Ding _{1,

2} , Xing Chang _{1,

2} , Shuping Zhang ₁ , Jia Xing _{1,

2} , Yele Sun ₆ , Dongsheng Ji ₇ , Chak K Chan ₈ , Jian Gao ₉ , Michael B McElroy ₃

Affiliation

School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University, Beijing 100084, China.
State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex, Beijing 100084, China.
School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, United States.
Center for Environmental Measurement and Modeling, U.S. Environmental Protection Agency, 109 T.W. Alexander Drive, Research Triangle Park, NC, 27711, USA.
Faculty of Frontier Engineering, Institute of Science and Engineering, Kanazawa University, Kanazawa 920-1192, Japan.
State Key Laboratory of Atmospheric Boundary Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China.
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC), Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, 100029, China.
School of Energy and Environment, City University of Hong Kong, Tat Chee Avenue, Kowloon, Hong Kong 999077, China.
State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 10084, China.

Nitrate and sulfate are two key components of airborne particulate matter (PM). While multiple formation mechanisms have been proposed for sulfate, current air quality models commonly underestimate its concentrations and mass fractions during northern China winter haze events. On the other hand, current models usually overestimate the mass fractions of nitrate. Very recently, laboratory studies have proposed that nitrous acid (N(III)) produced by particulate nitrate photolysis can oxidize sulfur dioxide to produce sulfate. Here, for the first time, we parametrize this heterogeneous mechanism into a state-of-the-art Community Multiscale Air Quality (CMAQ) model and quantify its contributions to sulfate formation. We find that the significance of this mechanism mainly depends on the enhancement effects (by 1–3 orders of magnitude as suggested by the available experimental studies) of the nitrate photolysis rate constant (J_NO₃^–) in aerosol liquid water compared to that in the gas phase. Comparisons between model simulations and in situ observations in Beijing suggest that this pathway can explain from about 15% (assuming an enhancement factor (EF) of 10) to 65% (assuming EF = 100) of the model–observation gaps in sulfate concentrations during winter haze. Our study strongly calls for future research on reducing the uncertainty in EF.

更新日期：2020-06-25

点击分享查看原文

点击收藏

阅读更多本刊最新论文本刊介绍/投稿指南

全部期刊列表>>