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(HONO) on Photochemical Smog Pollution Over the Pearl River Delta: Improvement and Application of WRF-Chem

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(HONO) on Photochemical Smog Pollution Over the Pearl River Delta: Improvement and Application of WRF-Chem Copyright Undertaking This thesis is protected by copyright, with all rights reserved. By reading and using the thesis, the reader understands and agrees to the following terms: 1. The reader will abide by the rules and legal ordinances governing copyright regarding the use of the thesis. 2. The reader will use the thesis for the purpose of research or private study only and not for distribution or further reproduction or any other purpose. 3. The reader agrees to indemnify and hold the University harmless from and against any loss, damage, cost, liability or expenses arising from copyright infringement or unauthorized usage. IMPORTANT If you have reasons to believe that any materials in this thesis are deemed not suitable to be distributed in this form, or a copyright owner having difficulty with the material being included in our database, please contact [email protected] providing details. The Library will look into your claim and consider taking remedial action upon receipt of the written requests. Pao Yue-kong Library, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong http://www.lib.polyu.edu.hk NUMERICAL STUDIES ON HAZE AND PHOTOCHEMICAL SMOG POLLUTION IN CHINA: TOWARD A BETTER UNDERSTANDING OF THEIR FORMATION MECHANISMS ZHANG LI Ph.D The Hong Kong Polytechnic University 2017 The Hong Kong Polytechnic University Department of Civil and Environmental Engineering Numerical Studies on Haze and Photochemical Smog Pollution in China: Toward a Better Understanding of Their Formation Mechanisms ZHANG Li A thesis submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy September 2016 i CERTIFICATE OF ORIGINALITY I hereby declare that this thesis is my own work and that, to the best of my knowledge and belief, it reproduces no material previously published or written, nor material that has been accepted for the award of any other degree or diploma, except where due acknowledgement has been made in the text. _____ _________ (Signed) ___________Li ZHANG ______________(Name of student) ii Abstract As a result of extremely fast economic developments since the late 1970’s, severe air pollution problems have emerged in major cities/city clusters in China. Among them are the Northern China Plain (NCP) and the Pearl River Delta region and Hong Kong (PRD-HK) which have suffered from severe haze pollution and photochemical smog pollution, respectively, and thus have been of great concern to the public and scientific community. The NCP is frequently assaulted by severe haze events especially in winter, while in the PRD-HK area, smog pollution is one of the major air quality problems. Although many modeling efforts have been conducted to study the formation mechanisms, varying from regional transport/local formation under unfavorable meteorological conditions to gaseous/aqueous chemistry, few have comprehensively investigated the role that heterogeneous chemistry plays in the haze pollution over the NCP or unveiled the potential effects of nitrous acid (HONO), an important source of OH radical, on the smog pollution in the PRD-HK. In this present study, heterogeneous processes were incorporated into a state-of-the-art chemical transport model (WRF-Chem) and four typical winter haze events over the NCP during January of 2010-2014, including an unprecedentedly severe one in January 2013, were selected and investigated by using the revised model. Simulations of these haze events indicated that the strong local accumulation of pollutants within the stable and shallow PBL and continuous regional transport under weak southerly winds were the major causes of the winter haze pollution over the NCP. The added heterogeneous processes further enhanced the regional -3 -3 -3 averaged PM2.5 over the NCP by 8.0 µg m (6.4%), 7.6 µg m (5.6%), 11.3 µg m (7.6%), and 2.3 µg m-3 (2.5%) during the 2010, 2012, 2013, and 2014 episode, respectively. During the severest 2013 episode, the climate anomalies characterized with extremely weak winds, high humidity, and strong vertical temperature inversion within the PBL resulted in stronger accumulation and more intensive heterogeneous formations of secondary aerosols over the NCP, making this haze event much worse than other three historical episodes. Our results showed that under humid conditions, heterogeneous reactions led to strong secondary formations of aerosols and noticeably contributed to the haze pollution, indicating the needs for considering iii heterogeneous chemistry in chemical transport models to better simulate the haze pollution in China. We also concluded that, due to the special location and topography, Beijing was naturally susceptible to heavy haze in winter, making it tough to control the air pollution in this megacity. Much more stringent control strategies must be taken over the NCP as well as a regional effort over the entire eastern China to alleviate the haze pollution in Beijing and the NCP. To investigate the effects of HONO on smog pollution over the PRD-HK, comprehensive sources of HONO, including the heterogeneous formations on the ocean, urban, and vegetation surfaces, traffic emissions, new gaseous formation pathways, and recently proposed biological sources, were parameterized into WRF-Chem. The updated model was applied to study a severe multiple-day smog episode in August 2011 over PRD-HK. Our simulations suggested that the heterogeneous source of HONO from ground, ocean, and aerosol surfaces were the major contributor (~54%) to the observed HONO concentration in Hong Kong, followed by the biological source (~29%) and gaseous sources (~9%). The new HONO sources noticeably affect the regional oxidation capacity with an increase of 10-20% in OH radical and significantly enhanced the smog pollution with increases of 8-15%, 20-30%, and 10-15% in O3, nitrate, and total PM2.5, respectively, over the PRD-HK. The results clearly show that HONO plays an important role in photochemical smog pollution over the PRD-HK region and underscores the needs of implementations of comprehensive HONO formations into regional air quality models before utilizing them for refining ozone-control or PM2.5-control policies in the future. iv Publications arising from the thesis Peer-reviewed Papers 1) Lefohn, A.S., Malley, C.S., Simon, H., Wells B., Xu, X., Zhang, L., Wang, T., Responses of human health and vegetation exposure metrics to changes in ozone concentration distributions associated with changing emissions patterns in the European Union, United States, and China. Atmos. Environ. (2016), accepted. 2) Li, Q., Zhang, L., Wang, T., et al..: Impacts of heterogeneous uptake of dinitrogen pentoxide and chlorine activation on ozone and reactive nitrogen partitioning: Improvement and application of WRF-Chem model in southern China, Atmos. Chem. Phys. (2016), doi:10.5194/acp-2016-412. 3) Wang, T., Xue, L., Brimblecombe, P., Lam, Y.F., Li L., Zhang, L., Ozone pollution in China: A review of concentrations, meteorological influences, chemical precursors, and effect, Sci. Total. Environ. (2016), accepted. 4) Zhang, L., Wang, T., Zhang, Q., et al., Potential sources of nitrous acid (HONO) and their impacts on ozone: A WRF-Chem study in a polluted subtropical region. J. Geophys. Res. (2016), 121: 3645-3662. 5) Zhang, L., Wang, T., Lv, M., Zhang, Q., On the severe haze in Beijing during January 2013: Unraveling the effects of meteorological anomalies with WRF-Chem. Atmos. Environ. (2015), 104: 11-21. Book Chapter 1) Wang, T., Liang, Y., Zha, Q., Zhang, L., Wang,Z., Wang, W., Poon, S., Photochemical smog in southern China: a synthesis of observation and model investigations of sources and effects of nitrous acid, Brasseur G., et al., (Eds.), ISSI Scientific Series, to be published in 2016/2017. 2) Lefohn, A.S., Malley, C.S., Mills, G., Smith, L., Hazucha, M., Naik, V., Schultz, M.G., Simon, H., Wells B., De Marco, A., Xu, X., Zhang, L., Wang, T., Neufeld, H., Musselman, R., Tarasick, D., Parrish, D., Brauer, M., Coyle, M., Feng, Z., Tang, H., Kobayashi, K., Sicard, P., Chapter 3: Global Ozone Metrics for Climate Change, Human Health, and Crop/Ecosystem Research, Cooper, O., et al., (Eds.), Tropospheric Ozone Assessment Report (TOAR), to be published in 2016. Manuscript in Preparation 1) Zhang, L., Li, Q., Wang, T., Ahmadov, R., Zhang, Q., et al., Impacts of Nitryl Chloride and Nitrous Acid on Air Quality in China: Part I. A New Module for Reactive Nitrogen in WRF-Chem and Evaluations. (2016) 2) Zhang, L., Li, Q., Wang, T., Ahmadov, R., Zhang, Q., et al., Impacts of Nitryl Chloride and Nitrous Acid on Air Quality in China: Part II. Applications in China and sensitivity simulations. (2016) v ACKNOWLEDGEMENTS This thesis is the outcome of not only research works but also mental lessons I have learned during my almost four years of study and stay at Hong Kong Polytechnic University. It is also the fruit of lots of memorable experiences I have got from many remarkable colleagues and friends in Hong Kong to whom I would like to express my sincere thanks and appreciations here. First and foremost I would like to thank my supervisor Professor Tao Wang for his supervision and mentoring during my Ph.D. study at PolyU. Prof. Wang has been the guide in my early research career in atmospheric environment and chemistry. He has supported me not only by providing me with guidance in academic research and work over the past three years as a supervisor, but also emotional encouragements on the rough path of academic life as a mentor. His dedication and endeavor in scientific research have set up a good example for me. I would like to take this chance to thank my previous and present group members and my friends. They are, if not all, Mr. Yujun Tham, Mr. Qiaozhi Zha, Ms. Yuan Gao, Mr. Qinyi Li, Ms. Hui Yun, Ms. Jueqi Wu, Mr.
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