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ACP | Articles | Volume 20, issue 11
Atmos. Chem. Phys., 20, 6305–6321, 2020
https://doi.org/10.5194/acp-20-6305-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-6305-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 20, 6305–6321, 2020
https://doi.org/10.5194/acp-20-6305-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-6305-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
Research article 03 Jun 2020
Research article | 03 Jun 2020
Worsening urban ozone pollution in China from 2013 to 2017 – Part 1: The complex and varying roles of meteorology
Yiming Liu and Tao Wang
Related authors
Yiming Liu and Tao Wang
Atmos. Chem. Phys., 20, 6323–6337, https://doi.org/10.5194/acp-20-6323-2020, https://doi.org/10.5194/acp-20-6323-2020, 2020
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Surface ozone levels in urban areas of China were increasing despite the implementation of stringent emission control measures since 2013. Our modeling results show that the decrease in NOx, SO2, and PM emissions and increase in VOC emissions contributed to the urban ozone increases due to the nonlinear ozone chemistry and complex aerosol affects. VOC reduction measures should be implemented in the current and future policies to achieve the goal of improving the overall air quality.
Xiao Lu, Lin Zhang, Youfan Chen, Mi Zhou, Bo Zheng, Ke Li, Yiming Liu, Jintai Lin, Tzung-May Fu, and Qiang Zhang
Atmos. Chem. Phys., 19, 8339–8361, https://doi.org/10.5194/acp-19-8339-2019, https://doi.org/10.5194/acp-19-8339-2019, 2019
Short summary
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Severe and deteriorating surface ozone pollution over major Chinese cities has become an emerging environmental concern in China. This study assesses the source contributions (including anthropogenic, background, and individual natural sources) and meteorological influences of surface ozone over China in 2016–2017 using the GEOS-Chem chemical transport model at high horizontal resolution with the most up-to-date Chinese anthropogenic emission inventory.
Zhenhao Ling, Qianqian Xie, Min Shao, Zhe Wang, Tao Wang, Hai Guo, and Xuemei Wang
Atmos. Chem. Phys., 20, 11451–11467, https://doi.org/10.5194/acp-20-11451-2020, https://doi.org/10.5194/acp-20-11451-2020, 2020
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The observation data from a receptor site in the Pearl River Delta region were analyzed by a photochemical box model with near-explicit chemical mechanisms (i.e., the Master Chemical Mechanism, MCM), improvements with reversible and irreversible heterogeneous processes of glyoxal and methylglyoxal, and the gas-particle partitioning of oxidation products in the present study.
Yuting Wang, Yong-Feng Ma, Domingo Muñoz-Esparza, Cathy W. Y. Li, Mary Barth, Tao Wang, and Guy P. Brasseur
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-877, https://doi.org/10.5194/acp-2020-877, 2020
Preprint under review for ACP
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Large-eddy simulations (LES) were performed in the mountainous region of the Hong Kong island to investigate the degree to which the rates of chemical reactions between two reactive species are reduced due to the segregation of species within the convective boundary layer. We show that the inhomogeneity in emissions plays an important role in the segregation effect. Topography also has a significant influence on the segregation locally.
Wei Pu, Zhouxing Zou, Weihao Wang, David Tanner, Zhe Wang, and Tao Wang
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-252, https://doi.org/10.5194/amt-2020-252, 2020
Revised manuscript under review for AMT
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The hydroxyl radical (OH) is responsible for the degradation of trace gases and plays key roles in major environmental issues such as photochemical pollution. However, the measurement of atmospheric OH radical is a huge challenge due to its high reactivity. Our study provides systematic optimization of a chemical ionization mass spectrometer (CIMS) for OH measurement as a reference for other CIMS users. The ambient result demonstrates the capability of the CIMS for ambient OH measurement.
Yiming Liu and Tao Wang
Atmos. Chem. Phys., 20, 6323–6337, https://doi.org/10.5194/acp-20-6323-2020, https://doi.org/10.5194/acp-20-6323-2020, 2020
Short summary
Short summary
Surface ozone levels in urban areas of China were increasing despite the implementation of stringent emission control measures since 2013. Our modeling results show that the decrease in NOx, SO2, and PM emissions and increase in VOC emissions contributed to the urban ozone increases due to the nonlinear ozone chemistry and complex aerosol affects. VOC reduction measures should be implemented in the current and future policies to achieve the goal of improving the overall air quality.
Men Xia, Xiang Peng, Weihao Wang, Chuan Yu, Peng Sun, Yuanyuan Li, Yuliang Liu, Zhengning Xu, Zhe Wang, Zheng Xu, Wei Nie, Aijun Ding, and Tao Wang
Atmos. Chem. Phys., 20, 6147–6158, https://doi.org/10.5194/acp-20-6147-2020, https://doi.org/10.5194/acp-20-6147-2020, 2020
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ClNO2 and Cl2 can be photolyzed by sunlight to produce a highly reactive Cl atom which affects air quality and climate. We observed high ClNO2 and Cl2 concentrations during a recent field study in east China. We analyzed the data and proposed a new hypothesis on the Cl2 production mechanism. Yields of ClNO2 and Cl2 from N2O2 uptake were parameterized using observational constraints, and they can be used in air quality models to improve simulations of atmospheric photochemistry and air quality.
Yujiao Zhu, Likun Xue, Jian Gao, Jianmin Chen, Hongyong Li, Yong Zhao, Zhaoxin Guo, Tianshu Chen, Liang Wen, Penggang Zheng, Ye Shan, Xinfeng Wang, Tao Wang, Xiaohong Yao, and Wenxing Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-364, https://doi.org/10.5194/acp-2020-364, 2020
Preprint under review for ACP
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This work investigates the long-term changes in the new particle formation (NPF) events under reduced SO2 emissions at the summit of Mt. Tai, during seven campaigns from 2007 to 2018. We found the NPF intensity increased by 2–3 fold in 2018 against those in 2007. In contrast, the probability of new particles growing to the CCN size was largely decreased. The changes of the biogenic VOCs and anthropogenic emissions were proposed to explain the distinct NPF characteristics.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Chuan Yu, Zhe Wang, Men Xia, Xiao Fu, Weihao Wang, Yee Jun Tham, Tianshu Chen, Penggang Zheng, Hongyong Li, Ye Shan, Xinfeng Wang, Likun Xue, Yan Zhou, Dingli Yue, Yubo Ou, Jian Gao, Keding Lu, Steven S. Brown, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 20, 4367–4378, https://doi.org/10.5194/acp-20-4367-2020, https://doi.org/10.5194/acp-20-4367-2020, 2020
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This study provides a holistic picture of N2O5 heterogeneous uptake on ambient aerosols and the influencing factors under various climatic and chemical conditions in China, and it proposes an observation-based empirical parameterization. The empirical parameterization can be used in air quality models to improve the prediction of PM2.5 and photochemical pollution in China and similar polluted regions of the world.
Tao Li, Zhe Wang, Yaru Wang, Chen Wu, Yiheng Liang, Men Xia, Chuan Yu, Hui Yun, Weihao Wang, Yan Wang, Jia Guo, Hartmut Herrmann, and Tao Wang
Atmos. Chem. Phys., 20, 391–407, https://doi.org/10.5194/acp-20-391-2020, https://doi.org/10.5194/acp-20-391-2020, 2020
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This work presents a field study of cloud water chemistry and interactions of cloud, gas, and aerosols in the polluted coastal boundary layer in southern China. Substantial dissolved organic matter in the acidic cloud water was observed, and the gas- and aqueous-phase partitioning of carbonyl compounds was investigated. The results demonstrated the significant role of cloud processing in altering aerosol properties, especially in producing aqueous organics and droplet-mode aerosols.
Xiao Lu, Lin Zhang, Youfan Chen, Mi Zhou, Bo Zheng, Ke Li, Yiming Liu, Jintai Lin, Tzung-May Fu, and Qiang Zhang
Atmos. Chem. Phys., 19, 8339–8361, https://doi.org/10.5194/acp-19-8339-2019, https://doi.org/10.5194/acp-19-8339-2019, 2019
Short summary
Short summary
Severe and deteriorating surface ozone pollution over major Chinese cities has become an emerging environmental concern in China. This study assesses the source contributions (including anthropogenic, background, and individual natural sources) and meteorological influences of surface ozone over China in 2016–2017 using the GEOS-Chem chemical transport model at high horizontal resolution with the most up-to-date Chinese anthropogenic emission inventory.
Lu Shen, Daniel J. Jacob, Xiong Liu, Guanyu Huang, Ke Li, Hong Liao, and Tao Wang
Atmos. Chem. Phys., 19, 6551–6560, https://doi.org/10.5194/acp-19-6551-2019, https://doi.org/10.5194/acp-19-6551-2019, 2019
Xiao Fu, Tao Wang, Li Zhang, Qinyi Li, Zhe Wang, Men Xia, Hui Yun, Weihao Wang, Chuan Yu, Dingli Yue, Yan Zhou, Junyun Zheng, and Rui Han
Atmos. Chem. Phys., 19, 1–14, https://doi.org/10.5194/acp-19-1-2019, https://doi.org/10.5194/acp-19-1-2019, 2019
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This study has identified the major contributors to the observed high HONO levels during a severe winter pollution episode and highlighted the importance of HONO chemistry in the combined photochemical and haze pollution in a subtropical region. It also highlighted the critical need to include and update HONO sources in regional air quality models in order to predict ozone and other secondary pollutants better during heavy pollution events in southern China and similar regions.
Hui Yun, Weihao Wang, Tao Wang, Men Xia, Chuan Yu, Zhe Wang, Steven C. N. Poon, Dingli Yue, and Yan Zhou
Atmos. Chem. Phys., 18, 17515–17527, https://doi.org/10.5194/acp-18-17515-2018, https://doi.org/10.5194/acp-18-17515-2018, 2018
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Based on the data analysis of simultaneous measurement of N2O5 and ClNO2 in a severe winter haze in the Pearl River Delta, this study underscores the importance of N2O5 heterogeneous reactions in nitrate formation and calls for better parameterization of N2O5 heterogeneous chemistry in order to predict haze pollution in China.
Weihao Wang, Zhe Wang, Chuan Yu, Men Xia, Xiang Peng, Yan Zhou, Dingli Yue, Yubo Ou, and Tao Wang
Atmos. Meas. Tech., 11, 5643–5655, https://doi.org/10.5194/amt-11-5643-2018, https://doi.org/10.5194/amt-11-5643-2018, 2018
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This study introduces an in situ experimental approach to direct measurement of N2O5 heterogeneous reactivity in polluted environments. Laboratory tests, model simulations, and field deployment of the method at a polluted site in south China demonstrated its applicability in accurately measuring N2O5 uptake coefficient with high ambient pollutants levels and air mass changes. The introduced method is also applicable to in situ measurement of reactivity of other trace gases on ambient aerosols.
Yee Jun Tham, Zhe Wang, Qinyi Li, Weihao Wang, Xinfeng Wang, Keding Lu, Nan Ma, Chao Yan, Simonas Kecorius, Alfred Wiedensohler, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 18, 13155–13171, https://doi.org/10.5194/acp-18-13155-2018, https://doi.org/10.5194/acp-18-13155-2018, 2018
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This study addresses the limited understanding of heterogeneous N2O5 uptake and ClNO2 production in the polluted environment of China. The results showed that N2O5 uptake and ClNO2 yield cannot be well explained by previous parameterizations and were largely influenced by factors like aerosol water content and biomass burning emission. Our findings illuminate the need to realistically parameterize these heterogeneous processes for better simulation of photochemical and haze pollution in China.
Michael Le Breton, Åsa M. Hallquist, Ravi Kant Pathak, David Simpson, Yujue Wang, John Johansson, Jing Zheng, Yudong Yang, Dongjie Shang, Haichao Wang, Qianyun Liu, Chak Chan, Tao Wang, Thomas J. Bannan, Michael Priestley, Carl J. Percival, Dudley E. Shallcross, Keding Lu, Song Guo, Min Hu, and Mattias Hallquist
Atmos. Chem. Phys., 18, 13013–13030, https://doi.org/10.5194/acp-18-13013-2018, https://doi.org/10.5194/acp-18-13013-2018, 2018
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We apply state-of-the-art chemical characterization to determine the chloride radical production in Beijing via measurement of inorganic halogens at a semi-rural site. The high concentration of inorganic halogens, namely nitryl chloride, enables the production of chlorinated volatile organic compounds which are measured in both the gas and particle phases simultaneously. This enables the secondary production of aerosols via chlorine oxidation to be directly observed in ambient air.
Liang Wen, Likun Xue, Xinfeng Wang, Caihong Xu, Tianshu Chen, Lingxiao Yang, Tao Wang, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys., 18, 11261–11275, https://doi.org/10.5194/acp-18-11261-2018, https://doi.org/10.5194/acp-18-11261-2018, 2018
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We present the first piece of observational evidence of the increasing trend of fine nitrate aerosol in the North China Plain (NCP) during 2005–2015. The summertime nitrate formation mechanism is dissected with a multiphase chemical box model based on observations at three different sites. The nitrate formation is most sensitive to NO2 and to a lesser extent to O3. NH3 plays a significant role in prompting the nitrate formation, but it is usually in excess in summer in the NCP region.
Liwei Wang, Xinfeng Wang, Rongrong Gu, Hao Wang, Lan Yao, Liang Wen, Fanping Zhu, Weihao Wang, Likun Xue, Lingxiao Yang, Keding Lu, Jianmin Chen, Tao Wang, Yuanghang Zhang, and Wenxing Wang
Atmos. Chem. Phys., 18, 4349–4359, https://doi.org/10.5194/acp-18-4349-2018, https://doi.org/10.5194/acp-18-4349-2018, 2018
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This study presents concentrations, variation characteristics, sources and secondary formations of nitrated phenols, a major component of brown carbon, in typical seasons at four sites in northern China. The results highlight the strong influences and contributions of anthropogenic activities, in particular coal combustion and the aging processes, to the atmospheric nitrated phenols in this region.
Zhe Wang, Weihao Wang, Yee Jun Tham, Qinyi Li, Hao Wang, Liang Wen, Xinfeng Wang, and Tao Wang
Atmos. Chem. Phys., 17, 12361–12378, https://doi.org/10.5194/acp-17-12361-2017, https://doi.org/10.5194/acp-17-12361-2017, 2017
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This work addresses unclear roles of heterogeneous N2O5 reactions and chlorine activation processes in the polluted residual layer from a mountaintop measurement in northern China. The results revealed efficient ClNO2 production in the coal-fired plumes in this region, having large impacts on next-morning photochemistry. Fast heterogeneous N2O5 reactions dominate the nocturnal NOx loss and contribute to substantial nitrate formation, which may boost the haze pollution in northern China.
Li Zhang, Qinyi Li, Tao Wang, Ravan Ahmadov, Qiang Zhang, Meng Li, and Mengyao Lv
Atmos. Chem. Phys., 17, 9733–9750, https://doi.org/10.5194/acp-17-9733-2017, https://doi.org/10.5194/acp-17-9733-2017, 2017
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Little is known of the integrated impacts of HONO and ClNO2 on lower-tropospheric ozone so far. In this study, we updated WRF-Chem with the CBMZ_ReNOM module, which considers both the sources and chemistry of HONO and ClNO2. The revised model revealed that the two reactive nitrogen compounds significantly affected the oxidation capacity and ozone formation at the surface and within the lower troposphere over polluted regions and noticeably improved summertime O3 predictions over China.
Jiaping Wang, Aki Virkkula, Yuan Gao, Shuncheng Lee, Yicheng Shen, Xuguang Chi, Wei Nie, Qiang Liu, Zheng Xu, Xin Huang, Tao Wang, Long Cui, and Aijun Ding
Atmos. Chem. Phys., 17, 2653–2671, https://doi.org/10.5194/acp-17-2653-2017, https://doi.org/10.5194/acp-17-2653-2017, 2017
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Multi-year observations at a coastal station in Hong Kong reveals that aerosol optical properties showed clear temporal variations according to the dominant sources of aerosols. LPDM modeling and correlation analysis gave similar signals about the freshness of aerosols during different seasons. Fresh emissions of particles from nearby cities and ship exhausts affected light optical properties and particle size in summer and aged air mass in winter caused larger variability of light extinction.
Yee Jun Tham, Zhe Wang, Qinyi Li, Hui Yun, Weihao Wang, Xinfeng Wang, Likun Xue, Keding Lu, Nan Ma, Birger Bohn, Xin Li, Simonas Kecorius, Johannes Größ, Min Shao, Alfred Wiedensohler, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 16, 14959–14977, https://doi.org/10.5194/acp-16-14959-2016, https://doi.org/10.5194/acp-16-14959-2016, 2016
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This work addresses the unclear global significance of chlorine activation processes in the troposphere. The first high-quality measurement data set of ClNO2 in northern China revealed strong ClNO2 production in the residual layers, and demonstrated its significant effects on radical budget and ozone production. Our findings imply the widespread effects of ClNO2 over the polluted regions of northern China, which may increase photochemical and haze pollution.
Qinyi Li, Li Zhang, Tao Wang, Yee Jun Tham, Ravan Ahmadov, Likun Xue, Qiang Zhang, and Junyu Zheng
Atmos. Chem. Phys., 16, 14875–14890, https://doi.org/10.5194/acp-16-14875-2016, https://doi.org/10.5194/acp-16-14875-2016, 2016
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The regional distributions and impacts of N2O5 and ClNO2 remain poorly understood. To address the problem, we developed a chemical transport model further and conducted the first high-resolution simulation of the distributions of the two species. Our research demonstrated the significant impacts of the two gases on the lifetime of nitrogen oxides, secondary nitrate production and ozone formation in southern China and highlighted the necessity of considering this chemistry in air quality models.
Lei Sun, Likun Xue, Tao Wang, Jian Gao, Aijun Ding, Owen R. Cooper, Meiyun Lin, Pengju Xu, Zhe Wang, Xinfeng Wang, Liang Wen, Yanhong Zhu, Tianshu Chen, Lingxiao Yang, Yan Wang, Jianmin Chen, and Wenxing Wang
Atmos. Chem. Phys., 16, 10637–10650, https://doi.org/10.5194/acp-16-10637-2016, https://doi.org/10.5194/acp-16-10637-2016, 2016
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We compiled the available observations of surface O3 at Mt. Tai – the highest mountain in the North China Plain, and found a significant increase of O3 concenrations from 2003 to 2015. The observed O3 increase was mainly due to the increase of O3 precursors, especially VOCs. Our analysis shows that controlling NOx alone, in the absence of VOC controls, is not sufficient to reduce regional O3 levels in North China in a short period.
Likun Xue, Rongrong Gu, Tao Wang, Xinfeng Wang, Sandra Saunders, Donald Blake, Peter K. K. Louie, Connie W. Y. Luk, Isobel Simpson, Zheng Xu, Zhe Wang, Yuan Gao, Shuncheng Lee, Abdelwahid Mellouki, and Wenxing Wang
Atmos. Chem. Phys., 16, 9891–9903, https://doi.org/10.5194/acp-16-9891-2016, https://doi.org/10.5194/acp-16-9891-2016, 2016
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The chemical budgets and principal sources of ROx and NO3 radicals during a multi-day photochemical smog episode in Hong Kong are elucidated by an observation-constrained MCM model. NO3 was shown to be an important oxidant even during daytime in a pollution case when high aerosol loading attenuated the solar irradiation. This study suggests the potential important role of daytime NO3 chemistry in polluted atmospheres under conditions with the co-existence of abundant O3, NO2, VOCs, and aerosols.
L. K. Xue, S. M. Saunders, T. Wang, R. Gao, X. F. Wang, Q. Z. Zhang, and W. X. Wang
Geosci. Model Dev., 8, 3151–3162, https://doi.org/10.5194/gmd-8-3151-2015, https://doi.org/10.5194/gmd-8-3151-2015, 2015
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A detailed chemical mechanism including 205 reactions is developed for use in the Master Chemical Mechanism. With this new chlorine mechanism, it was found that the nocturnal formation of ClNO2 has high potential to perturb the next day's atmospheric photochemistry, by enhancing the radical production and cycling, VOC oxidation and O3 formation, in the polluted coastal environments.
T. Li, Y. Wang, W. J. Li, J. M. Chen, T. Wang, and W. X. Wang
Atmos. Chem. Phys., 15, 8987–9002, https://doi.org/10.5194/acp-15-8987-2015, https://doi.org/10.5194/acp-15-8987-2015, 2015
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Twelve trace elements in fine particles and clouds at a mountain site in southern China were investigated.
Long-range transport contributed the most to element concentrations, whereas the YRD and the area around Mt. Lushan exhibited the highest element solubility.
We demonstrated that cloud processing can enhance aerosol element solubility and increase sulfate concentration correspondingly, by irreversibly altering the morphology of metal particles in cloud droplet residues.
L. K. Xue, T. Wang, J. Gao, A. J. Ding, X. H. Zhou, D. R. Blake, X. F. Wang, S. M. Saunders, S. J. Fan, H. C. Zuo, Q. Z. Zhang, and W. X. Wang
Atmos. Chem. Phys., 14, 13175–13188, https://doi.org/10.5194/acp-14-13175-2014, https://doi.org/10.5194/acp-14-13175-2014, 2014
X. Wang, T. Wang, C. Yan, Y. J. Tham, L. Xue, Z. Xu, and Q. Zha
Atmos. Meas. Tech., 7, 1–12, https://doi.org/10.5194/amt-7-1-2014, https://doi.org/10.5194/amt-7-1-2014, 2014
L. K. Xue, T. Wang, J. Gao, A. J. Ding, X. H. Zhou, D. R. Blake, X. F. Wang, S. M. Saunders, S. J. Fan, H. C. Zuo, Q. Z. Zhang, and W. X. Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-27243-2013, https://doi.org/10.5194/acpd-13-27243-2013, 2013
Revised manuscript not accepted
L. K. Xue, T. Wang, H. Guo, D. R. Blake, J. Tang, X. C. Zhang, S. M. Saunders, and W. X. Wang
Atmos. Chem. Phys., 13, 8551–8567, https://doi.org/10.5194/acp-13-8551-2013, https://doi.org/10.5194/acp-13-8551-2013, 2013
W. Nie, T. Wang, L. K. Xue, A. J. Ding, X. F. Wang, X. M. Gao, Z. Xu, Y. C. Yu, C. Yuan, Z. S. Zhou, R. Gao, X. H. Liu, Y. Wang, S. J. Fan, S. Poon, Q. Z. Zhang, and W. X. Wang
Atmos. Chem. Phys., 12, 11985–11995, https://doi.org/10.5194/acp-12-11985-2012, https://doi.org/10.5194/acp-12-11985-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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Comprehensive isoprene and terpene gas-phase chemistry improves simulated surface ozone in the southeastern US
Evaluating China's anthropogenic CO2 emissions inventories: a northern China case study using continuous surface observations from 2005 to 2009
Influence of aerosol copper on HO2 uptake: A novel parameterized equation
Modeling stratospheric intrusion and trans-Pacific transport on tropospheric ozone using hemispheric CMAQ during April 2010 – Part 1: Model evaluation and air mass characterization for stratosphere–troposphere transport
Modeling stratospheric intrusion and trans-Pacific transport on tropospheric ozone using hemispheric CMAQ during April 2010 – Part 2: Examination of emission impacts based on the higher-order decoupled direct method
The long-term trend and production sensitivity change in the US ozone pollution from observations and model simulations
Comparison of tropospheric NO2 columns from MAX-DOAS retrievals and regional air quality model simulations
Street-scale air quality modelling for Beijing during a winter 2016 measurement campaign
Pan-Arctic surface ozone: modelling vs measurements
Magnitude, trends, and impacts of ambient long-term ozone exposure in the United States from 2000 to 2015
On the limit to the accuracy of regional-scale air quality models
Peiyu Cao, Chaoqun Lu, Jien Zhang, and Avani Khadilkar
Atmos. Chem. Phys., 20, 11907–11922, https://doi.org/10.5194/acp-20-11907-2020, https://doi.org/10.5194/acp-20-11907-2020, 2020
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In this study, we estimate monthly ammonia emission from synthetic nitrogen fertilizer use across the contiguous US from 1900 to 2015. The results indicate the important role that cropland expansion and nitrogen fertilizer enrichment played in enhancing NH3 emissions. It shows such long-term human activities have dramatically changed the spatiotemporal and seasonal patterns of NH3 emission, impacting air pollution and public health in the US.
Pengfei Han, Ning Zeng, Tom Oda, Xiaohui Lin, Monica Crippa, Dabo Guan, Greet Janssens-Maenhout, Xiaolin Ma, Zhu Liu, Yuli Shan, Shu Tao, Haikun Wang, Rong Wang, Lin Wu, Xiao Yun, Qiang Zhang, Fang Zhao, and Bo Zheng
Atmos. Chem. Phys., 20, 11371–11385, https://doi.org/10.5194/acp-20-11371-2020, https://doi.org/10.5194/acp-20-11371-2020, 2020
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An accurate estimation of China’s fossil-fuel CO2 emissions (FFCO2) is significant for quantification of carbon budget and emissions reductions towards the Paris Agreement goals. Here we assessed 9 global and regional inventories. Our findings highlight the significance of using locally measured coal emission factors. We call on the enhancement of physical measurements for validation and provide comprehensive information for inventory, monitoring, modeling, assimilation, and reducing emissions.
Ke Li, Daniel J. Jacob, Lu Shen, Xiao Lu, Isabelle De Smedt, and Hong Liao
Atmos. Chem. Phys., 20, 11423–11433, https://doi.org/10.5194/acp-20-11423-2020, https://doi.org/10.5194/acp-20-11423-2020, 2020
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Surface summer ozone increased in China from 2013 to 2019 despite new governmental efforts targeting ozone pollution. We find that the ozone increase is mostly due to anthropogenic drivers, although meteorology also plays a role. Further analysis for the North China Plain shows that PM2.5 continued to decrease through 2019, while emissions of volatile organic compounds (VOCs) stayed flat. This could explain the anthropogenic increase in ozone, as PM2.5 scavenges the radical precursors of ozone.
Hervé Petetin, Dene Bowdalo, Albert Soret, Marc Guevara, Oriol Jorba, Kim Serradell, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 20, 11119–11141, https://doi.org/10.5194/acp-20-11119-2020, https://doi.org/10.5194/acp-20-11119-2020, 2020
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To control the spread of the COVID-19 coronavirus, the Spanish Government recently implemented a strict lockdown of the population, which strongly reduced the levels of nitrogen dioxide (NO2), one of the most critical air pollutants in Spain. This study quantifies the contribution of the lockdown on these reduced NO2 levels in Spain, taking the confounding effect of meteorology on artificial intelligence techniques into account.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
James Weber, Scott Archer-Nicholls, Paul Griffiths, Torsten Berndt, Michael Jenkin, Hamish Gordon, Christoph Knote, and Alexander T. Archibald
Atmos. Chem. Phys., 20, 10889–10910, https://doi.org/10.5194/acp-20-10889-2020, https://doi.org/10.5194/acp-20-10889-2020, 2020
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Highly oxygenated organic molecules (HOMs) are important for aerosol growth and new particle formation, particularly in air masses with less sulphuric acid. This new chemical mechanism reproduces measured [HOM] and [HOM precursors] and is concise enough for use in global climate models. The mechanism also reproduces the observed suppression of HOMs by isoprene, suggesting enhanced emissions may not necessarily lead to more aerosols. Greater HOM importance in the pre-industrial era is also shown.
Martin O. P. Ramacher, Lin Tang, Jana Moldanová, Volker Matthias, Matthias Karl, Erik Fridell, and Lasse Johansson
Atmos. Chem. Phys., 20, 10667–10686, https://doi.org/10.5194/acp-20-10667-2020, https://doi.org/10.5194/acp-20-10667-2020, 2020
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The effects of shipping emissions on air quality and health in the harbour city of Gothenburg were simulated for different scenarios for the year 2040 with coupled regional and city-scale chemistry transport models to evaluate the impact of regional emission regulations and onshore electricity for ships at berth. The results show that contributions of shipping to exposure and associated health impacts from particulate matter and NO2 decrease significantly compared to 2012 in all scenarios.
Tim Butler, Aurelia Lupascu, and Aditya Nalam
Atmos. Chem. Phys., 20, 10707–10731, https://doi.org/10.5194/acp-20-10707-2020, https://doi.org/10.5194/acp-20-10707-2020, 2020
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Ground-level ozone (O3) is not directly emitted; it is formed chemically in the atmosphere. Some ground-level O3 is transported from the stratosphere, but most O3 is produced from reactive precursors that are emitted by both natural and anthropogenic sources. We present the results of a novel source apportionment method for ground-level O3. Our results are consistent with previous work and also provide new insights. In particular, we highlight the roles of methane and international shipping.
Li Zhang, Meiyun Lin, Andrew O. Langford, Larry W. Horowitz, Christoph J. Senff, Elizabeth Klovenski, Yuxuan Wang, Raul J. Alvarez II, Irina Petropavlovskikh, Patrick Cullis, Chance W. Sterling, Jeff Peischl, Thomas B. Ryerson, Steven S. Brown, Zachary C. J. Decker, Guillaume Kirgis, and Stephen Conley
Atmos. Chem. Phys., 20, 10379–10400, https://doi.org/10.5194/acp-20-10379-2020, https://doi.org/10.5194/acp-20-10379-2020, 2020
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Measuring and quantifying the sources of elevated springtime ozone in the southwestern US is challenging but relevant to the implications for control policy. Here we use intensive field measurements and two global models to study ozone sources in the region. We find that ozone from the stratosphere, wildfires, and Asia is an important source of high-ozone events in the region. Our analysis also helps understand the uncertainties in ozone simulations with individual models.
Amir H. Souri, Caroline R. Nowlan, Gonzalo González Abad, Lei Zhu, Donald R. Blake, Alan Fried, Andrew J. Weinheimer, Armin Wisthaler, Jung-Hun Woo, Qiang Zhang, Christopher E. Chan Miller, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 20, 9837–9854, https://doi.org/10.5194/acp-20-9837-2020, https://doi.org/10.5194/acp-20-9837-2020, 2020
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For the first time, we provide a joint nonlinear optimal estimate of NOx and NMVOC emissions during the KORUS-AQ campaign by simultaneously incorporating SAO's new product of HCHO columns from OMPS and OMI tropospheric NO2 columns into a regional model. Results demonstrate a promising improvement in the performance of the model in terms of HCHO and NO2 concentrations, which in turn enables us to quantify the impact of the emission changes on different pathways of ozone formation and loss.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Edward J. Dlugokencky, Ray L. Langenfelds, Michel Ramonet, Doug Worthy, and Bo Zheng
Atmos. Chem. Phys., 20, 9525–9546, https://doi.org/10.5194/acp-20-9525-2020, https://doi.org/10.5194/acp-20-9525-2020, 2020
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The hydroxyl radical (OH), which is the dominant sink of methane (CH4), plays a key role in closing the global methane budget. This study quantifies how uncertainties in the hydroxyl radical can influence top-down estimates of CH4 emissions based on 4D Bayesian inversions with different OH fields and the same surface observations. We show that uncertainties in CH4 emissions driven by different OH fields are comparable to the uncertainties given by current bottom-up and top-down estimations.
Johannes G. M. Barten, Laurens N. Ganzeveld, Auke J. Visser, Rodrigo Jiménez, and Maarten C. Krol
Atmos. Chem. Phys., 20, 9441–9458, https://doi.org/10.5194/acp-20-9441-2020, https://doi.org/10.5194/acp-20-9441-2020, 2020
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Combining satellite and urban air pollution measurements with a meteorology and air quality model, we present the state of air quality in Colombia. We found four distinctly different emission regimes. The simulated pollution levels compare well with satellite data, but the comparison also indicates misrepresentation of prescribed fire emissions and simulated lightning emissions. Comparison of urban measurements requires careful consideration of (nocturnal) boundary layer dynamics and advection.
Martin Cussac, Virginie Marécal, Valérie Thouret, Béatrice Josse, and Bastien Sauvage
Atmos. Chem. Phys., 20, 9393–9417, https://doi.org/10.5194/acp-20-9393-2020, https://doi.org/10.5194/acp-20-9393-2020, 2020
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Biomass burning emissions are a major source of carbon monoxide in the atmosphere. Here, the vertical transport that these emissions can undergo until the upper troposphere is investigated, as well as their contribution to carbon monoxide concentrations. It was found that boreal forest emissions were specific to the occurrence of pyroconvection directly above the fires, whereas biomass burning emissions from other regions of the globe relied more on the occurrence of deep convection.
Eirini Boleti, Christoph Hueglin, Stuart K. Grange, André S. H. Prévôt, and Satoshi Takahama
Atmos. Chem. Phys., 20, 9051–9066, https://doi.org/10.5194/acp-20-9051-2020, https://doi.org/10.5194/acp-20-9051-2020, 2020
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Long-term temporal evolution of ozone concentrations between 2000 and 2015 in Europe was estimated using a signal decomposition technique. The seasonal cycles are correlated with local climate conditions and vary according to geographic region, while ozone levels are indicative of distance to emission sources. The site's environment plays a key role in ozone trends, with the most polluted environments showing the least reduction in ozone, while in less polluted areas ozone has decreased.
Tiantian Wang, Yu Song, Zhenying Xu, Mingxu Liu, Tingting Xu, Wenling Liao, Lifei Yin, Xuhui Cai, Ling Kang, Hongsheng Zhang, and Tong Zhu
Atmos. Chem. Phys., 20, 8727–8736, https://doi.org/10.5194/acp-20-8727-2020, https://doi.org/10.5194/acp-20-8727-2020, 2020
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Satellite measurements have revealed that the Indo-Gangetic Plain (IGP) has the global maximum ammonia concentrations, with a peak from June to August. Here, we studied the reasons for this phenomenon through computer simulations. Low sulfur dioxide and nitrogen oxides emissions and high air temperature over the IGP weaken the swallowing of gaseous ammonia by acidic gases. Additionally, the barrier effects of the Himalayas, like a windshield, are also conducive to the accumulation of ammonia.
Jia Xing, Siwei Li, Yueqi Jiang, Shuxiao Wang, Dian Ding, Zhaoxin Dong, Yun Zhu, and Jiming Hao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-522, https://doi.org/10.5194/acp-2020-522, 2020
Revised manuscript accepted for ACP
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Quantifying emission changes is a prerequisite for assessment of control effectiveness in improving air quality. However, traditional bottom-up method usually takes months to perform and limits timely assessments. A novel method was developed by using a response model that provides real-time estimation of emission changes based on air quality observations. It was successfully applied to quantify emission changes in the North China Plain due to the COVID-19 pandemic shutdown.
Peter D. Ivatt and Mathew J. Evans
Atmos. Chem. Phys., 20, 8063–8082, https://doi.org/10.5194/acp-20-8063-2020, https://doi.org/10.5194/acp-20-8063-2020, 2020
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We investigate the potential of using a decision tree algorithm to identify and correct the tropospheric ozone bias in a chemical transport model. We train the algorithm on 2010–2015 ground and column observation data and test the algorithm on the 2016–2017 data using the ground data as well as independent flight data. We find the algorithm is successfully able to identify and correct the bias, improving the model performance.
Mariano Mertens, Astrid Kerkweg, Volker Grewe, Patrick Jöckel, and Robert Sausen
Atmos. Chem. Phys., 20, 7843–7873, https://doi.org/10.5194/acp-20-7843-2020, https://doi.org/10.5194/acp-20-7843-2020, 2020
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We investigate the contribution of land transport emissions to ozone and ozone precursors in Europe and Germany. Our results show that land transport emissions are one of the most important contributors to reactive nitrogen in Europe. The contribution to ozone is in the range of 8 % to 16 % and varies strongly for different seasons. The hots-pots with the largest ozone concentrations are the Po Valley, while the largest concentration to reactive nitrogen is located mainly in western Europe.
Lya Lugon, Karine Sartelet, Youngseob Kim, Jérémy Vigneron, and Olivier Chrétien
Atmos. Chem. Phys., 20, 7717–7740, https://doi.org/10.5194/acp-20-7717-2020, https://doi.org/10.5194/acp-20-7717-2020, 2020
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This study presents a new version of the multi-scale model Street-in-Grid (SinG) that interconnects regional and local scales in air-quality modeling in urban areas. The new version of SinG performs the finest coupling between transport and chemistry, leading to a numerically stable partitioning between NO and NO2. Multi-scale, local-scale and regional-scale simulations of NO, NO2 and NOx over Paris are compared to observations, and SinG shows good performance for both local and regional scales.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Benjamin Gaubert, Louisa K. Emmons, Kevin Raeder, Simone Tilmes, Kazuyuki Miyazaki, Avelino F. Arellano Jr., Nellie Elguindi, Claire Granier, Wenfu Tang, Jérôme Barré, Helen M. Worden, Rebecca R. Buchholz, David P. Edwards, Philipp Franke, Jeffrey L. Anderson, Marielle Saunois, Jason Schroeder, Jung-Hun Woo, Isobel J. Simpson, Donald R. Blake, Simone Meinardi, Paul O. Wennberg, John Crounse, Alex Teng, Michelle Kim, Russell R. Dickerson, Hao He, and Xinrong Ren
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-599, https://doi.org/10.5194/acp-2020-599, 2020
Revised manuscript accepted for ACP
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This study investigates carbon monoxide pollution in East-Asia during Spring using a numerical model, satellite remote sensing and aircraft measurements. We found an underestimation of emissions source. Correcting the emission bias can improve air quality forecasting of carbon monoxide and other species including ozone. Results also suggest that controlling VOC and CO emissions, in addition to wide spread NOx controls, can improve pollution ozone over East Asia.
Michael E. Jenkin, Richard Valorso, Bernard Aumont, Mike J. Newland, and Andrew R. Rickard
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-583, https://doi.org/10.5194/acp-2020-583, 2020
Revised manuscript accepted for ACP
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Unsaturated organic compounds are emitted in large quantities from natural and human-influenced sources. Atmospheric removal occurs significantly by reaction with ozone, initiating reaction sequences forming free radicals and organic pollutants in the gaseous and particulate phases. Due to their very large number, it is impossible to study the reaction rate for every compound, and most have to be estimated. Updated and extended estimation methods are reported for use in atmospheric models.
Luc Vereecken and Barbara Nozière
Atmos. Chem. Phys., 20, 7429–7458, https://doi.org/10.5194/acp-20-7429-2020, https://doi.org/10.5194/acp-20-7429-2020, 2020
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Alkyl peroxy radicals, RO2, are important intermediates in the oxidation of organic material in the atmosphere. It was shown earlier that hydrogen atom migration within RO2 can be important and results in the formation of additional oxidants and large highly oxygenated molecules that lead to more and larger aerosols. In this work we propose a method for predicting the chemical rate for these H migrations in RO2, helping atmospheric models to correctly include these reactions.
Susann Tegtmeier, Elliot Atlas, Birgit Quack, Franziska Ziska, and Kirstin Krüger
Atmos. Chem. Phys., 20, 7103–7123, https://doi.org/10.5194/acp-20-7103-2020, https://doi.org/10.5194/acp-20-7103-2020, 2020
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We investigate emissions of brominated gases from the ocean and their contribution to stratospheric ozone depletion. Once in the atmosphere, these gases usually break down in less than 6 months. Their impact on the ozone layer depends on the prevailing atmospheric circulation, since transport to the stratosphere requires uplift. We combine aircraft and ship observations with atmospheric modelling to analyse how, where, and when these gases are transported from the ocean into the stratosphere.
Rachel L. Tunnicliffe, Anita L. Ganesan, Robert J. Parker, Hartmut Boesch, Nicola Gedney, Benjamin Poulter, Zhen Zhang, Jošt V. Lavrič, David Walter, Matthew Rigby, Stephan Henne, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-438, https://doi.org/10.5194/acp-2020-438, 2020
Revised manuscript accepted for ACP
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This study quantifies Brazil’s emissions of a potent atmospheric greenhouse gas, methane. The study is in the field of atmospheric modelling and uses remotely sensed and surface measurements of methane concentrations and an atmospheric transport model to interpret the data. Because of Brazil’s large emissions from wetlands, agriculture and biomass burning, these emissions affect global methane concentrations and thus are of global significance.
Simon Rosanka, Giang H. T. Vu, Hue M. T. Nguyen, Tien V. Pham, Umar Javed, Domenico Taraborrelli, and Luc Vereecken
Atmos. Chem. Phys., 20, 6671–6686, https://doi.org/10.5194/acp-20-6671-2020, https://doi.org/10.5194/acp-20-6671-2020, 2020
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Isocyanic acid, HNCO, is a toxic chemical compound emitted to the atmosphere by biomass burning and by unwanted release in NOx mitigation systems in vehicles such as the AdBlue system. We have studied the loss processes of HNCO, finding that it is unreactive to most atmospheric oxidants and thus has a long chemical lifetime. The main removal is then by deposition on surfaces and transition to aqueous phase, such as clouds. The long lifetime also allows it to be transported to the stratosphere.
Yi Wang, Jun Wang, Meng Zhou, Daven K. Henze, Cui Ge, and Wei Wang
Atmos. Chem. Phys., 20, 6651–6670, https://doi.org/10.5194/acp-20-6651-2020, https://doi.org/10.5194/acp-20-6651-2020, 2020
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We developed four different methods to downscale SO2 and NO2 emissions derived from OMPS satellite observations (in Part 1) for regional air quality modeling at a spatial resolution that is finer than satellite observations. The VIIRS (city lights), TROPOMI, and OMI satellite data as well as surface data are used to evaluate the model. The method of using the top-down emissions from the past month for the air quality forecast in the present month is also shown to have practical merit.
Yiming Liu and Tao Wang
Atmos. Chem. Phys., 20, 6323–6337, https://doi.org/10.5194/acp-20-6323-2020, https://doi.org/10.5194/acp-20-6323-2020, 2020
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Surface ozone levels in urban areas of China were increasing despite the implementation of stringent emission control measures since 2013. Our modeling results show that the decrease in NOx, SO2, and PM emissions and increase in VOC emissions contributed to the urban ozone increases due to the nonlinear ozone chemistry and complex aerosol affects. VOC reduction measures should be implemented in the current and future policies to achieve the goal of improving the overall air quality.
Rui Li, Yilong Zhao, Wenhui Zhou, Ya Meng, Ziyu Zhang, and Hongbo Fu
Atmos. Chem. Phys., 20, 6159–6175, https://doi.org/10.5194/acp-20-6159-2020, https://doi.org/10.5194/acp-20-6159-2020, 2020
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The Tibetan Plateau lacks ground-level O3 observation due to its unique geographical environment. It is imperative to employ modelling methods to simulate the O3 level. The present study proposed a novel technique for estimating the surface O3 level in remote regions. The result captured long-term O3 concentration on the Tibetan Plateau, which was beneficial for assessing the effects of O3 on climate change and ecosystem safety, especially in a vulnerable area of the ecological environment.
Zhi-Zhen Ni, Kun Luo, Yang Gao, Xiang Gao, Fei Jiang, Cheng Huang, Jian-Ren Fan, Joshua S. Fu, and Chang-Hong Chen
Atmos. Chem. Phys., 20, 5963–5976, https://doi.org/10.5194/acp-20-5963-2020, https://doi.org/10.5194/acp-20-5963-2020, 2020
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The Weather Research Forecast with Chemistry (WRF-Chem) model was used to simulate spatial and temporal O3 evolution in the Yangtze River Delta (YRD) region. Various atmospheric processes were analyzed to determine the influential factors of ozone formation through the integrated process rate method. This paper provides insight into urban O3 formation and dispersion during tropical cyclone events and supports the Model Intercomparison Study Asia Phase III (MICS-Asia Phase III).
Peter H. Zimmermann, Carl A. M. Brenninkmeijer, Andrea Pozzer, Patrick Jöckel, Franziska Winterstein, Andreas Zahn, Sander Houweling, and Jos Lelieveld
Atmos. Chem. Phys., 20, 5787–5809, https://doi.org/10.5194/acp-20-5787-2020, https://doi.org/10.5194/acp-20-5787-2020, 2020
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The atmospheric abundance of the greenhouse gas methane is determined by interacting emission sources and sinks in a dynamic global environment. In this study, its global budget from 1997 to 2016 is simulated with a general circulation model using emission estimates of 11 source categories. The model results are evaluated against 17 ground station and 320 intercontinental flight observation series. Deviations are used to re-scale the emission quantities with the aim of matching observations.
Thibaud M. Fritz, Sebastian D. Eastham, Raymond L. Speth, and Steven R. H. Barrett
Atmos. Chem. Phys., 20, 5697–5727, https://doi.org/10.5194/acp-20-5697-2020, https://doi.org/10.5194/acp-20-5697-2020, 2020
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Aircraft exhaust drives formation of ozone and is a dominant anthropogenic influence in the upper troposphere. These impacts are mitigated by non-linear chemistry inside the aircraft plume, which cuts off part of the ozone production pathway and reduces the long-term impact of aircraft in a way which is not captured by current models. The ice clouds which form in aircraft exhaust ("contrails") also play a role, converting emitted nitrogen oxides into more stable forms such as nitric acid.
Audrey Fortems-Cheiney, Gaëlle Dufour, Karine Dufossé, Florian Couvidat, Jean-Marc Gilliot, Guillaume Siour, Matthias Beekmann, Gilles Foret, Frederik Meleux, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Cathy Clerbaux, and Sophie Génermont
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-292, https://doi.org/10.5194/acp-2020-292, 2020
Revised manuscript accepted for ACP
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Studies have suggested the importance of ammonia emissions on pollution particle formation over Europe, whose main atmospheric source is agriculture. In this study, we performed an inter-comparison of two alternative inventories with a reference inventory that quantify the French ammonia emissions during spring 2011. Over regions with large mineral fertilizer use, like over North-Eastern France, NH3 emissions are probably considerably underestimated by the reference inventory.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-308, https://doi.org/10.5194/acp-2020-308, 2020
Revised manuscript accepted for ACP
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Decadal trends and variations in the OH are critical for understanding the atmospheric CH4 evolution. We quantify the impacts of OH trends and variations on the CH4 budget by conducting CH4 inversions on decadal-scale with an ensemble of OH fields. We find the negative OH anomalies due to enhanced fires can reduce the optimized CH4 emissions by up to 10 Tg yr−1 during El Niño years, and the positive OH trend from 1986 to 2010 results in ~ 23 Tg yr−1 additional increase in optimized CH4 emissions.
Yuting Wang, Yong-Feng Ma, Henk Eskes, Antje Inness, Johannes Flemming, and Guy P. Brasseur
Atmos. Chem. Phys., 20, 4493–4521, https://doi.org/10.5194/acp-20-4493-2020, https://doi.org/10.5194/acp-20-4493-2020, 2020
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The paper presents an evaluation of the CAMS global reanalysis of reactive gases performed for the period 2003–2016. The evaluation is performed by comparing concentrations of chemical species gathered during airborne field campaigns with calculated values. The reanalysis successfully reproduces the observed concentrations of ozone and carbon monoxide but generally underestimates the abundance of hydrocarbons. Large discrepancies exist for fast-reacting radicals such as OH and HO2.
Yu Zhao, Mengchen Yuan, Xin Huang, Feng Chen, and Jie Zhang
Atmos. Chem. Phys., 20, 4275–4294, https://doi.org/10.5194/acp-20-4275-2020, https://doi.org/10.5194/acp-20-4275-2020, 2020
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We estimated the ammonia emissions based on the constant emission factors and those characterizing the agricultural processes for the Yangtze River Delta, China. The discrepancies between the two estimates and their causes were analyzed. Based on ground and satellite observations, the two estimates were evaluated with air quality modeling. This work indicates ways to improve the emission estimation and helps better understand the necessity of multi-pollutant control strategy.
Zhen Qu, Daven K. Henze, Owen R. Cooper, and Jessica L. Neu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-307, https://doi.org/10.5194/acp-2020-307, 2020
Revised manuscript accepted for ACP
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We use satellite observations and chemical transport modeling to quantify sources of NOx, a major air pollutant, over the past decade. We find improved simulations of the magnitude, seasonality and trends of NO2 and ozone concentrations using these derived emissions. Changes in ozone pollution driven by human and natural sources are identified in different regions. This work shows the benefits of remote sensing data and inverse modeling for more accurate ozone simulations.
Hajime Akimoto, Tatsuya Nagashima, Li Jie, Joshua S. Fu, and Zifa Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-228, https://doi.org/10.5194/acp-2020-228, 2020
Revised manuscript accepted for ACP
Oliver Wild, Apostolos Voulgarakis, Fiona O'Connor, Jean-François Lamarque, Edmund M. Ryan, and Lindsay Lee
Atmos. Chem. Phys., 20, 4047–4058, https://doi.org/10.5194/acp-20-4047-2020, https://doi.org/10.5194/acp-20-4047-2020, 2020
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Global models of tropospheric chemistry and transport show a persistent diversity in results that has not been fully explained. We demonstrate the first use of global sensitivity analysis consistently across three independent models to explore these differences and reveal both clear similarities and surprising differences which have important implications for our assessment of future atmospheric composition change.
Rebecca H. Schwantes, Louisa K. Emmons, John J. Orlando, Mary C. Barth, Geoffrey S. Tyndall, Samuel R. Hall, Kirk Ullmann, Jason M. St. Clair, Donald R. Blake, Armin Wisthaler, and Thao Paul V. Bui
Atmos. Chem. Phys., 20, 3739–3776, https://doi.org/10.5194/acp-20-3739-2020, https://doi.org/10.5194/acp-20-3739-2020, 2020
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Ozone is a greenhouse gas and air pollutant that is harmful to human health and plants. During the summer in the southeastern US, many regional and global models are biased high for surface ozone compared to observations. Here adding more complex and updated chemistry for isoprene and terpenes, which are biogenic hydrocarbons emitted from trees and vegetation, into an earth system model greatly reduces the simulated surface ozone bias compared to aircraft and monitoring station data.
Archana Dayalu, J. William Munger, Yuxuan Wang, Steven C. Wofsy, Yu Zhao, Thomas Nehrkorn, Chris Nielsen, Michael B. McElroy, and Rachel Chang
Atmos. Chem. Phys., 20, 3569–3588, https://doi.org/10.5194/acp-20-3569-2020, https://doi.org/10.5194/acp-20-3569-2020, 2020
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China has pledged to reduce carbon dioxide emissions per unit GDP by 60–65 % relative to 2005 levels, and to peak carbon emissions overall by 2030. Disagreement among available inventories of Chinese emissions makes it difficult for China to track progress toward its goals and evaluate the efficacy of regional control measures. This study uses a unique set of historical atmospheric observations for the key period from 2005 to 2009 to independently evaluate three different CO2 emission estimates.
Huan Song, Xiaorui Chen, Keding Lu, Qi Zou, Zhaofeng Tan, Hendrik Fuchs, Alfred Wiedensohler, Mei Zheng, Andreas Wahner, Astrid Kiendler-Scharr, and Yuanhang Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-218, https://doi.org/10.5194/acp-2020-218, 2020
Revised manuscript accepted for ACP
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Accurate calculation of the HO2 uptake coefficient is one of the key parameter to quantifying the co-reduction of both aerosol and ozone pollutions. We modelled various lab measurements of γHO2 based on a gas-liquid phase kinetic model and developed a state of art parameterized equation. Based on a dataset from a comprehensive field campaign in North China Plain, we proposed that the determination of heterogeneous uptake process for HO2 should be added for the future field campaigns.
Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, and Yang Zhang
Atmos. Chem. Phys., 20, 3373–3396, https://doi.org/10.5194/acp-20-3373-2020, https://doi.org/10.5194/acp-20-3373-2020, 2020
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The state-of-the-science Community Multiscale Air Quality model extended for hemispheric applications (H-CMAQ) is used to model the trans-Pacific transport which has been recognized as a potential source of air pollutants over the US. In Part 1, modeled ozone is evaluated with observations at surface, by ozonesonde and airplane, and by satellite across the Northern Hemisphere. In addition, a newly developed air mass characterization method to estimate stratospheric intrusion is presented.
Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, Sergey L. Napelenok, and Yang Zhang
Atmos. Chem. Phys., 20, 3397–3413, https://doi.org/10.5194/acp-20-3397-2020, https://doi.org/10.5194/acp-20-3397-2020, 2020
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The state-of-the-science Community Multiscale Air Quality model extended for hemispheric applications (H-CMAQ) is used to model the trans-Pacific transport which has been recognized as a potential source of air pollutants over the US. In Part 2, the higher-order decoupled direct method (HDDM) is applied to investigate the emission impacts from east Asia and the US during April 2010. Furthermore, changes in trans-Pacific transport caused by the recent emissions are examined.
Hao He, Xin-Zhong Liang, Chao Sun, Zhining Tao, and Daniel Q. Tong
Atmos. Chem. Phys., 20, 3191–3208, https://doi.org/10.5194/acp-20-3191-2020, https://doi.org/10.5194/acp-20-3191-2020, 2020
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We studied the trend of US ozone pollution from 1990 to 2015 using EPA observations and computer simulations. Observations indicated a decrease in peak ozone at noon due to regulations and a slight increase in ozone in early morning and late afternoon possibly. Our modeling system confirmed these findings and provided detailed information about ozone photochemistry. These results revealed the success of previous control measures and provide scientific evidence for the future regulations.
Anne-Marlene Blechschmidt, Joaquim Arteta, Adriana Coman, Lyana Curier, Henk Eskes, Gilles Foret, Clio Gielen, Francois Hendrick, Virginie Marécal, Frédérik Meleux, Jonathan Parmentier, Enno Peters, Gaia Pinardi, Ankie J. M. Piters, Matthieu Plu, Andreas Richter, Arjo Segers, Mikhail Sofiev, Álvaro M. Valdebenito, Michel Van Roozendael, Julius Vira, Tim Vlemmix, and John P. Burrows
Atmos. Chem. Phys., 20, 2795–2823, https://doi.org/10.5194/acp-20-2795-2020, https://doi.org/10.5194/acp-20-2795-2020, 2020
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MAX-DOAS tropospheric NO2 vertical column retrievals from a set of European measurement stations are compared to regional air quality models which contribute to the operational Copernicus Atmosphere Monitoring Service (CAMS). Correlations are on the order of 35 %–75 %; large differences occur for individual pollution plumes. The results demonstrate that future model development needs to concentrate on improving representation of diurnal cycles and associated temporal scalings.
Michael Biggart, Jenny Stocker, Ruth M. Doherty, Oliver Wild, Michael Hollaway, David Carruthers, Jie Li, Qiang Zhang, Ruili Wu, Simone Kotthaus, Sue Grimmond, Freya A. Squires, James Lee, and Zongbo Shi
Atmos. Chem. Phys., 20, 2755–2780, https://doi.org/10.5194/acp-20-2755-2020, https://doi.org/10.5194/acp-20-2755-2020, 2020
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Ambient air pollution is a major cause of premature death in China. We examine the street-scale variation of pollutant levels in Beijing using air pollution dispersion and chemistry model ADMS-Urban. Campaign measurements are compared with simulated pollutant levels, providing a valuable means of evaluating the impact of key processes on urban air quality. Air quality modelling at such fine scales is essential for human exposure studies and for informing choices on future emission controls.
Xin Yang, Anne-M Blechschmidt, Kristof Bognar, Audra McClure–Begley, Sara Morris, Irina Petropavlovskikh, Andreas Richter, Henrik Skov, Kimberly Strong, David Tarasick, Taneil Uttal, Mika Vestenius, and Xiaoyi Zhao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-984, https://doi.org/10.5194/acp-2019-984, 2020
Revised manuscript accepted for ACP
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We report a modelling-based study on surface ozone across the Arctic. Two global chemistry models and surface ozone from six sites are used in this study. Model simulations show that, in spring, surface ozone can be greatly reduced by bromine chemistry, with almost half attributable to open-ocean-sourced bromine and the rest to sea-ice-sourced bromine. However, the open-ocean-sourced bromine cannot by itself produce ozone depletion at concentrations < 10 ppbv, while sea-ice-sourced bromine can.
Karl M. Seltzer, Drew T. Shindell, Prasad Kasibhatla, and Christopher S. Malley
Atmos. Chem. Phys., 20, 1757–1775, https://doi.org/10.5194/acp-20-1757-2020, https://doi.org/10.5194/acp-20-1757-2020, 2020
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Long-term exposure to ambient ozone is associated with a variety of impacts, including adverse human-health effects and reduced commercial crop yields. We apply machine learning to empirically model long-term O3 exposure over the continental United States from 2000 to 2015 and generate a measurement-based assessment of impacts on human health and crop yields. Notably, our results illustrate how different conclusions regarding historical impacts can be drawn through the use of varying metrics.
S. Trivikrama Rao, Huiying Luo, Marina Astitha, Christian Hogrefe, Valerie Garcia, and Rohit Mathur
Atmos. Chem. Phys., 20, 1627–1639, https://doi.org/10.5194/acp-20-1627-2020, https://doi.org/10.5194/acp-20-1627-2020, 2020
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Since numerical air quality models do not explicitly simulate stochastic variations in the atmosphere, there will always be differences between modeled and measured pollutant levels even when the model's physics, chemistry, numerical analysis, and its input data are perfect. This paper quantifies the inherent uncertainty in regional models due to the stochastic nature of the atmosphere. A knowledge of the expected error helps model developers in evaluating the real progress in improving models.
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Short summary
This study revealed the effects of changes in meteorology and anthropogenic emissions on the summer ozone variations from 2013 to 2017 across China by conducting numerical experiments. We highlighted the important but varying roles of meteorology in ozone variations attributed to the synergistic or counteracting effects from individual meteorological factors. Developing future ozone pollution mitigation policies should consider the counteracting impact of meteorological changes.
This study revealed the effects of changes in meteorology and anthropogenic emissions on the...
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