Articles | Volume 20, issue 7
Atmos. Chem. Phys., 20, 4153–4165, 2020
https://doi.org/10.5194/acp-20-4153-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Special issue: Multiphase chemistry of secondary aerosol formation under...
Atmos. Chem. Phys., 20, 4153–4165, 2020
https://doi.org/10.5194/acp-20-4153-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
07 Apr 2020
Research article
| 07 Apr 2020
Formation mechanisms of atmospheric nitrate and sulfate during the winter haze pollution periods in Beijing: gas-phase, heterogeneous and aqueous-phase chemistry
Pengfei Liu et al.
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Wei Ma, Zemin Feng, Junlei Zhan, Yongchun Liu, Pengfei Liu, Chengtang Liu, Qingxin Ma, Kang Yang, Yafei Wang, Hong He, Markku Kulmala, Yujing Mu, and Junfeng Liu
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The influence of photochemical loss of volatile organic compounds (VOCS) on O3 formation is investigated using an observation-based model. The sensitivity regime of ozone formation might be misdiagnosed due to the photochemical loss of VOCs in the atmosphere. The contribution of local photochemistry is underestimated regarding O3 pollution when one does not consider the photochemical loss of VOCs.
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Nitrous acid (HONO) and related parameters were measured at the foot and the summit of Mt. Tai in the summer of 2018. Based on measurements at the foot station, we utilized a box model to explore the roles of different sources in the HONO budget. We also studied radical chemistry in this high-ozone region.
Men Xia, Xiang Peng, Weihao Wang, Chuan Yu, Zhe Wang, Yee Jun Tham, Jianmin Chen, Hui Chen, Yujing Mu, Chenglong Zhang, Pengfei Liu, Likun Xue, Xinfeng Wang, Jian Gao, Hong Li, and Tao Wang
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ClNO2 is an important precursor of chlorine radical that affects photochemistry. However, its production and impact are not well understood. Our study presents field observations of ClNO2 at three sites in northern China. These observations provide new insights into nighttime processes that produce ClNO2 and the significant impact of ClNO2 on secondary pollutions during daytime. The results improve the understanding of photochemical pollution in the lower part of the atmosphere.
Yongchun Liu, Zemin Feng, Feixue Zheng, Xiaolei Bao, Pengfei Liu, Yanli Ge, Yan Zhao, Tao Jiang, Yunwen Liao, Yusheng Zhang, Xiaolong Fan, Chao Yan, Biwu Chu, Yonghong Wang, Wei Du, Jing Cai, Federico Bianchi, Tuukka Petäjä, Yujing Mu, Hong He, and Markku Kulmala
Atmos. Chem. Phys., 21, 13269–13286, https://doi.org/10.5194/acp-21-13269-2021, https://doi.org/10.5194/acp-21-13269-2021, 2021
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The mechanisms and kinetics of particulate sulfate formation in the atmosphere are still open questions although they have been extensively discussed. We found that uptake of SO2 is the rate-determining step for the conversion of SO2 to particulate sulfate. NH4NO3 plays an important role in AWC, the phase state of aerosol particles, and subsequently the uptake kinetics of SO2 under high-RH conditions. This work is a good example of the feedback between aerosol physics and aerosol chemistry.
Tianzeng Chen, Jun Liu, Qingxin Ma, Biwu Chu, Peng Zhang, Jinzhu Ma, Yongchun Liu, Cheng Zhong, Pengfei Liu, Yafei Wang, Yujing Mu, and Hong He
Atmos. Chem. Phys., 21, 1341–1356, https://doi.org/10.5194/acp-21-1341-2021, https://doi.org/10.5194/acp-21-1341-2021, 2021
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Effects of photochemical aging on the formation and evolution of summertime secondary aerosol were systematically investigated in a suburb of Beijing. Higher PM1 concentration accompanied longer photochemical age (ta). Sulfate and more-oxidized OOA formation were significantly sensitive to the increase in ta, and their contributions were greatly enhanced at elevated ta levels. Our results suggested that photochemical aging process played a crucial role in PM1 and O3 pollution in summertime.
Jiarong Li, Chao Zhu, Hui Chen, Defeng Zhao, Likun Xue, Xinfeng Wang, Hongyong Li, Pengfei Liu, Junfeng Liu, Chenglong Zhang, Yujing Mu, Wenjin Zhang, Luming Zhang, Hartmut Herrmann, Kai Li, Min Liu, and Jianmin Chen
Atmos. Chem. Phys., 20, 13735–13751, https://doi.org/10.5194/acp-20-13735-2020, https://doi.org/10.5194/acp-20-13735-2020, 2020
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Based on a field study at Mt. Tai, China, the simultaneous variations of cloud microphysics, aerosol microphysics and their potential interactions during cloud life cycles were discussed. Results demonstrated that clouds on clean days were more susceptible to the concentrations of particle number, while clouds formed on polluted days might be more sensitive to meteorological parameters. Particles larger than 150 nm played important roles in forming cloud droplets with sizes of 5–10 μm.
Pengfei Liu, Chenglong Zhang, Chaoyang Xue, Yujing Mu, Junfeng Liu, Yuanyuan Zhang, Di Tian, Can Ye, Hongxing Zhang, and Jian Guan
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The North China Plain in winter frequently suffers from severe haze pollution which is mainly ascribed to elevation of PM2. 5. Although the government has performed a series of control measures for major pollution sources, the PM2. 5 levels were still above 1000 ug m-3 in some areas of the Beijing–Tianjin–Hebei region. In this study, we found that residential coal combustion made an evident contribution to PM2. 5 in the region, the contributions of which were estimated to be about 32–58 %.
Chengtang Liu, Zhuobiao Ma, Yujing Mu, Junfeng Liu, Chenglong Zhang, Yuanyuan Zhang, Pengfei Liu, and Hongxing Zhang
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NMHCs were measured during wintertime in Beijing to recognize their pollution levels, variation characteristics, and sources. The difference of the diurnal variations in NMHCs between clear days and haze days indicated that the relative contribution of vehicular emissions to NMHCs depended on the pollution status. Both the correlation coefficients of hydrocarbon pairs and PMF analysis revealed that coal combustion was an important source for atmospheric NMHCs, especially on haze days.
Pengfei Liu, Chenglong Zhang, Yujing Mu, Chengtang Liu, Chaoyang Xue, Can Ye, Junfeng Liu, Yuanyuan Zhang, and Hongxing Zhang
Atmos. Chem. Phys., 16, 10097–10109, https://doi.org/10.5194/acp-16-10097-2016, https://doi.org/10.5194/acp-16-10097-2016, 2016
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The periodic emissions from farmers' activities in the NCP were found to make a great contribution to atmospheric WSIs in Beijing: crop straw burning contributed to K+ in Beijing; coal combustion for heating by farmers in winter and the use of NH4Cl fertilizers in the NCP contributed to Cl− in Beijing. The harvest and soil ploughing in autumn contributed to the regional Ca2+. In addition, the mineral dust greatly accelerated formation of sulfate and nitrate through heterogeneous reactions.
Wei Ma, Zemin Feng, Junlei Zhan, Yongchun Liu, Pengfei Liu, Chengtang Liu, Qingxin Ma, Kang Yang, Yafei Wang, Hong He, Markku Kulmala, Yujing Mu, and Junfeng Liu
Atmos. Chem. Phys., 22, 4841–4851, https://doi.org/10.5194/acp-22-4841-2022, https://doi.org/10.5194/acp-22-4841-2022, 2022
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The influence of photochemical loss of volatile organic compounds (VOCS) on O3 formation is investigated using an observation-based model. The sensitivity regime of ozone formation might be misdiagnosed due to the photochemical loss of VOCs in the atmosphere. The contribution of local photochemistry is underestimated regarding O3 pollution when one does not consider the photochemical loss of VOCs.
Chaoyang Xue, Can Ye, Jörg Kleffmann, Chenglong Zhang, Valéry Catoire, Fengxia Bao, Abdelwahid Mellouki, Likun Xue, Jianmin Chen, Keding Lu, Yong Zhao, Hengde Liu, Zhaoxin Guo, and Yujing Mu
Atmos. Chem. Phys., 22, 3149–3167, https://doi.org/10.5194/acp-22-3149-2022, https://doi.org/10.5194/acp-22-3149-2022, 2022
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Summertime measurements of nitrous acid (HONO) and related parameters were conducted at the foot and the summit of Mt. Tai (1534 m above sea level). We proposed a rapid vertical air mass exchange between the foot and the summit level, which enhances the role of HONO in the oxidizing capacity of the upper boundary layer. Kinetics for aerosol-derived HONO sources were constrained. HONO formation from different paths was quantified and discussed.
Chaoyang Xue, Can Ye, Jörg Kleffmann, Wenjin Zhang, Xiaowei He, Pengfei Liu, Chenglong Zhang, Xiaoxi Zhao, Chengtang Liu, Zhuobiao Ma, Junfeng Liu, Jinhe Wang, Keding Lu, Valéry Catoire, Abdelwahid Mellouki, and Yujing Mu
Atmos. Chem. Phys., 22, 1035–1057, https://doi.org/10.5194/acp-22-1035-2022, https://doi.org/10.5194/acp-22-1035-2022, 2022
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Nitrous acid (HONO) and related parameters were measured at the foot and the summit of Mt. Tai in the summer of 2018. Based on measurements at the foot station, we utilized a box model to explore the roles of different sources in the HONO budget. We also studied radical chemistry in this high-ozone region.
Men Xia, Xiang Peng, Weihao Wang, Chuan Yu, Zhe Wang, Yee Jun Tham, Jianmin Chen, Hui Chen, Yujing Mu, Chenglong Zhang, Pengfei Liu, Likun Xue, Xinfeng Wang, Jian Gao, Hong Li, and Tao Wang
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ClNO2 is an important precursor of chlorine radical that affects photochemistry. However, its production and impact are not well understood. Our study presents field observations of ClNO2 at three sites in northern China. These observations provide new insights into nighttime processes that produce ClNO2 and the significant impact of ClNO2 on secondary pollutions during daytime. The results improve the understanding of photochemical pollution in the lower part of the atmosphere.
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Atmos. Chem. Phys., 21, 15809–15826, https://doi.org/10.5194/acp-21-15809-2021, https://doi.org/10.5194/acp-21-15809-2021, 2021
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Six heterogeneous HONO chemistry updates in CMAQ significantly improve HONO concentration. HONO production is primarily controlled by the heterogeneous reactions on ground and aerosol surfaces during haze. Additional HONO chemistry updates increase OH and production of secondary aerosols: sulfate, nitrate, and SOA.
Huan Song, Keding Lu, Can Ye, Huabin Dong, Shule Li, Shiyi Chen, Zhijun Wu, Mei Zheng, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 13713–13727, https://doi.org/10.5194/acp-21-13713-2021, https://doi.org/10.5194/acp-21-13713-2021, 2021
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Secondary sulfate aerosols are an important component of fine particles in severe air pollution events. We calculated the sulfate formation rates via a state-of-the-art multiphase model constrained to the observed values. We showed that transition metals in urban aerosols contribute significantly to sulfate formation during haze periods and thus play an important role in mitigation strategies and public health measures in megacities worldwide.
Yongchun Liu, Zemin Feng, Feixue Zheng, Xiaolei Bao, Pengfei Liu, Yanli Ge, Yan Zhao, Tao Jiang, Yunwen Liao, Yusheng Zhang, Xiaolong Fan, Chao Yan, Biwu Chu, Yonghong Wang, Wei Du, Jing Cai, Federico Bianchi, Tuukka Petäjä, Yujing Mu, Hong He, and Markku Kulmala
Atmos. Chem. Phys., 21, 13269–13286, https://doi.org/10.5194/acp-21-13269-2021, https://doi.org/10.5194/acp-21-13269-2021, 2021
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The mechanisms and kinetics of particulate sulfate formation in the atmosphere are still open questions although they have been extensively discussed. We found that uptake of SO2 is the rate-determining step for the conversion of SO2 to particulate sulfate. NH4NO3 plays an important role in AWC, the phase state of aerosol particles, and subsequently the uptake kinetics of SO2 under high-RH conditions. This work is a good example of the feedback between aerosol physics and aerosol chemistry.
Tianzeng Chen, Jun Liu, Qingxin Ma, Biwu Chu, Peng Zhang, Jinzhu Ma, Yongchun Liu, Cheng Zhong, Pengfei Liu, Yafei Wang, Yujing Mu, and Hong He
Atmos. Chem. Phys., 21, 1341–1356, https://doi.org/10.5194/acp-21-1341-2021, https://doi.org/10.5194/acp-21-1341-2021, 2021
Short summary
Short summary
Effects of photochemical aging on the formation and evolution of summertime secondary aerosol were systematically investigated in a suburb of Beijing. Higher PM1 concentration accompanied longer photochemical age (ta). Sulfate and more-oxidized OOA formation were significantly sensitive to the increase in ta, and their contributions were greatly enhanced at elevated ta levels. Our results suggested that photochemical aging process played a crucial role in PM1 and O3 pollution in summertime.
Jiarong Li, Chao Zhu, Hui Chen, Defeng Zhao, Likun Xue, Xinfeng Wang, Hongyong Li, Pengfei Liu, Junfeng Liu, Chenglong Zhang, Yujing Mu, Wenjin Zhang, Luming Zhang, Hartmut Herrmann, Kai Li, Min Liu, and Jianmin Chen
Atmos. Chem. Phys., 20, 13735–13751, https://doi.org/10.5194/acp-20-13735-2020, https://doi.org/10.5194/acp-20-13735-2020, 2020
Short summary
Short summary
Based on a field study at Mt. Tai, China, the simultaneous variations of cloud microphysics, aerosol microphysics and their potential interactions during cloud life cycles were discussed. Results demonstrated that clouds on clean days were more susceptible to the concentrations of particle number, while clouds formed on polluted days might be more sensitive to meteorological parameters. Particles larger than 150 nm played important roles in forming cloud droplets with sizes of 5–10 μm.
Dawei Lu, Jihua Tan, Xuezhi Yang, Xu Sun, Qian Liu, and Guibin Jiang
Atmos. Chem. Phys., 19, 2861–2870, https://doi.org/10.5194/acp-19-2861-2019, https://doi.org/10.5194/acp-19-2861-2019, 2019
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We investigated for the first time the role of Si during secondary formation process of PM2.5. We show the noncorrelation of Si with the secondary aerosol (SA) formation in Beijing, which reveals a new conservative tracer for aerosol chemistry. The SA contribution can be estimated by using Si as a single tracer instead of commonly used multiple chemical tracers. The correlation analysis of SA with the Si isotopic composition of PM2.5 can also reveal the sources of the precursors of SA.
Pengfei Liu, Chenglong Zhang, Chaoyang Xue, Yujing Mu, Junfeng Liu, Yuanyuan Zhang, Di Tian, Can Ye, Hongxing Zhang, and Jian Guan
Atmos. Chem. Phys., 17, 11503–11520, https://doi.org/10.5194/acp-17-11503-2017, https://doi.org/10.5194/acp-17-11503-2017, 2017
Short summary
Short summary
The North China Plain in winter frequently suffers from severe haze pollution which is mainly ascribed to elevation of PM2. 5. Although the government has performed a series of control measures for major pollution sources, the PM2. 5 levels were still above 1000 ug m-3 in some areas of the Beijing–Tianjin–Hebei region. In this study, we found that residential coal combustion made an evident contribution to PM2. 5 in the region, the contributions of which were estimated to be about 32–58 %.
Chengtang Liu, Zhuobiao Ma, Yujing Mu, Junfeng Liu, Chenglong Zhang, Yuanyuan Zhang, Pengfei Liu, and Hongxing Zhang
Atmos. Chem. Phys., 17, 10633–10649, https://doi.org/10.5194/acp-17-10633-2017, https://doi.org/10.5194/acp-17-10633-2017, 2017
Short summary
Short summary
NMHCs were measured during wintertime in Beijing to recognize their pollution levels, variation characteristics, and sources. The difference of the diurnal variations in NMHCs between clear days and haze days indicated that the relative contribution of vehicular emissions to NMHCs depended on the pollution status. Both the correlation coefficients of hydrocarbon pairs and PMF analysis revealed that coal combustion was an important source for atmospheric NMHCs, especially on haze days.
Pengfei Liu, Chenglong Zhang, Yujing Mu, Chengtang Liu, Chaoyang Xue, Can Ye, Junfeng Liu, Yuanyuan Zhang, and Hongxing Zhang
Atmos. Chem. Phys., 16, 10097–10109, https://doi.org/10.5194/acp-16-10097-2016, https://doi.org/10.5194/acp-16-10097-2016, 2016
Short summary
Short summary
The periodic emissions from farmers' activities in the NCP were found to make a great contribution to atmospheric WSIs in Beijing: crop straw burning contributed to K+ in Beijing; coal combustion for heating by farmers in winter and the use of NH4Cl fertilizers in the NCP contributed to Cl− in Beijing. The harvest and soil ploughing in autumn contributed to the regional Ca2+. In addition, the mineral dust greatly accelerated formation of sulfate and nitrate through heterogeneous reactions.
Y. Zhang, Y. Mu, Y. Zhou, J. Liu, and C. Zhang
Biogeosciences, 11, 1717–1726, https://doi.org/10.5194/bg-11-1717-2014, https://doi.org/10.5194/bg-11-1717-2014, 2014
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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Ziyong Guo, Yuxiang Yang, Xiaodong Hu, Xiaocong Peng, Yuzhen Fu, Wei Sun, Guohua Zhang, Duohong Chen, Xinhui Bi, Xinming Wang, and Ping'an Peng
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We show that in-cloud aqueous processing facilitates the formation of brown carbon (BrC), based on the simultaneous measurements of the light-absorption properties of the cloud residuals, cloud interstitial, and cloud-free particles. While extensive laboratory evidence indicated the formation of BrC in aqueous phase, our study represents the first attempt to show the possibility in real clouds, which would have potential implications in the atmospheric evolution and radiation forcing of BrC.
Han Zang, Yue Zhao, Juntao Huo, Qianbiao Zhao, Qingyan Fu, Yusen Duan, Jingyuan Shao, Cheng Huang, Jingyu An, Likun Xue, Ziyue Li, Chenxi Li, and Huayun Xiao
Atmos. Chem. Phys., 22, 4355–4374, https://doi.org/10.5194/acp-22-4355-2022, https://doi.org/10.5194/acp-22-4355-2022, 2022
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Particulate nitrate plays an important role in wintertime haze pollution in eastern China, yet quantitative constraints on detailed nitrate formation mechanisms remain limited. Here we quantified the contributions of the heterogeneous N2O5 hydrolysis (66 %) and gas-phase OH + NO2 reaction (32 %) to nitrate formation in this region and identified the atmospheric oxidation capacity (i.e., availability of O3 and OH radicals) as the driving factor of nitrate formation from both processes.
Laura Tositti, Erika Brattich, Claudio Cassardo, Pietro Morozzi, Alessandro Bracci, Angela Marinoni, Silvana Di Sabatino, Federico Porcù, and Alessandro Zappi
Atmos. Chem. Phys., 22, 4047–4073, https://doi.org/10.5194/acp-22-4047-2022, https://doi.org/10.5194/acp-22-4047-2022, 2022
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Christine D. Groot Zwaaftink, Wenche Aas, Sabine Eckhardt, Nikolaos Evangeliou, Paul Hamer, Mona Johnsrud, Arve Kylling, Stephen M. Platt, Kerstin Stebel, Hilde Uggerud, and Karl Espen Yttri
Atmos. Chem. Phys., 22, 3789–3810, https://doi.org/10.5194/acp-22-3789-2022, https://doi.org/10.5194/acp-22-3789-2022, 2022
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We investigate causes of a poor-air-quality episode in northern Europe in October 2020 during which EU health limits for air quality were vastly exceeded. Such episodes may trigger measures to improve air quality. Analysis based on satellite observations, transport simulations, and surface observations revealed two sources of pollution. Emissions of mineral dust in Central Asia and biomass burning in Ukraine arrived almost simultaneously in Norway, and transport continued into the Arctic.
Adrien Deroubaix, Laurent Menut, Cyrille Flamant, Peter Knippertz, Andreas H. Fink, Anneke Batenburg, Joel Brito, Cyrielle Denjean, Cheikh Dione, Régis Dupuy, Valerian Hahn, Norbert Kalthoff, Fabienne Lohou, Alfons Schwarzenboeck, Guillaume Siour, Paolo Tuccella, and Christiane Voigt
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During the summer monsoon in West Africa, pollutants emitted in urbanized areas modify cloud cover and precipitation patterns. We analyze these patterns with the WRF-CHIMERE model, integrating the effects of aerosols on meteorology, based on the numerous observations provided by the Dynamics-Aerosol-Climate-Interactions campaign. This study adds evidence to recent findings that increased pollution levels in West Africa delay the breakup time of low-level clouds and reduce precipitation.
Julia Schmale, Sangeeta Sharma, Stefano Decesari, Jakob Pernov, Andreas Massling, Hans-Christen Hansson, Knut von Salzen, Henrik Skov, Elisabeth Andrews, Patricia K. Quinn, Lucia M. Upchurch, Konstantinos Eleftheriadis, Rita Traversi, Stefania Gilardoni, Mauro Mazzola, James Laing, and Philip Hopke
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Long-term data sets of Arctic aerosol properties from 10 stations across the Arctic provide evidence that anthropogenic influence on the Arctic atmospheric chemical composition has declined in winter, a season which is typically dominated by mid-latitude emissions. The number of significant trends in summer is smaller than in winter, and overall the pattern is ambiguous with some significant positive and negative trends. This reflects the mixed influence of natural and anthropogenic emissions.
Jenna C. Ditto, Jo Machesky, and Drew R. Gentner
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We analyzed gases and aerosols sampled in summer and winter in a coastal region that is often downwind of urban areas and observed large contributions of nitrogen-containing organic compounds influenced by a mix of biogenic, anthropogenic, and/or marine sources as well as photochemical and aqueous-phase atmospheric processes. The results show the prevalence of key reduced and oxidized nitrogen functional groups and advance knowledge on the chemical structure of nitrogen-containing compounds.
Yanhong Zhu, Weijun Li, Yue Wang, Jian Zhang, Lei Liu, Liang Xu, Jingsha Xu, Jinhui Shi, Longyi Shao, Pingqing Fu, Daizhou Zhang, and Zongbo Shi
Atmos. Chem. Phys., 22, 2191–2202, https://doi.org/10.5194/acp-22-2191-2022, https://doi.org/10.5194/acp-22-2191-2022, 2022
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The solubilities of iron in fine particles in a megacity in Eastern China were studied under haze, fog, dust, clear, and rain weather conditions. For the first time, a receptor model was used to quantify the sources of dissolved and total iron aerosol. Microscopic analysis further confirmed the aging of iron aerosol during haze and fog conditions that facilitated dissolution of insoluble iron.
Yating Gao, Dihui Chen, Yanjie Shen, Yang Gao, Huiwang Gao, and Xiaohong Yao
Atmos. Chem. Phys., 22, 1515–1528, https://doi.org/10.5194/acp-22-1515-2022, https://doi.org/10.5194/acp-22-1515-2022, 2022
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This study focuses on spatiotemporal heterogeneity of observed gaseous amines, NH3, their particulate counterparts in PM2.5 over different sea zones, and the disproportional release of alkaline gases and corresponding particulate counterparts from seawater in the sea zones in terms of different extents of enrichment of TMAH+ and DMAH+ in the sea surface microlayer (SML). A novel hypothesis is delivered.
Johannes Passig, Julian Schade, Robert Irsig, Thomas Kröger-Badge, Hendryk Czech, Thomas Adam, Henrik Fallgren, Jana Moldanova, Martin Sklorz, Thorsten Streibel, and Ralf Zimmermann
Atmos. Chem. Phys., 22, 1495–1514, https://doi.org/10.5194/acp-22-1495-2022, https://doi.org/10.5194/acp-22-1495-2022, 2022
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The single-particle distribution of health-relevant polycyclic aromatic hydrocarbons (PAHs) was studied at the Swedish coast in autumn. We found PAHs bound to long-range transported particles from eastern and central Europe and also from ship emissions and local sources. This is the first field study using a new technology revealing single-particle data from both inorganic components and PAHs. We discuss PAH profiles that are indicative of several sources and atmospheric aging processes.
Daniel A. Knopf, Joseph C. Charnawskas, Peiwen Wang, Benny Wong, Jay M. Tomlin, Kevin A. Jankowski, Matthew Fraund, Daniel P. Vegthe, Swarup China, Alexander Laskin, Ryan C. Moffet, Mary K. Gilles, Josephine Y. Aller, Matthew A. Marcus, Shira Raveh-Rubin, and Jian Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-61, https://doi.org/10.5194/acp-2022-61, 2022
Revised manuscript accepted for ACP
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Marine boundary layer aerosols collected in the remote region of the eastern north Atlantic induce immersion freezing and deposition ice nucleation under typical mixed-phase and cirrus clouds conditions. Corresponding ice nucleation parameterizations for model applications have been derived. Chemical imaging of ambient aerosol and ice-nucleating particles demonstrates that the latter is dominated by sea salt and organics, while also representing a major particle type in the particle population.
Md. Mozammel Haque, Yanlin Zhang, Srinivas Bikkina, Meehye Lee, and Kimitaka Kawamura
Atmos. Chem. Phys., 22, 1373–1393, https://doi.org/10.5194/acp-22-1373-2022, https://doi.org/10.5194/acp-22-1373-2022, 2022
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We attempt to understand the current state of East Asian organic aerosols with both the molecular marker approach and 14° C data of carbonaceous components. A significant positive correlation of nonfossil- and fossil-derived organic carbon with levoglucosan suggests the importance of biomass burning (BB) and coal combustion sources in the East Asian outflow. Thus, attribution of ambient levoglucosan levels over the western North Pacific to the impact of BB emission may cause large uncertainty.
Jing Cai, Cheng Wu, Jiandong Wang, Wei Du, Feixue Zheng, Simo Hakala, Xiaolong Fan, Biwu Chu, Lei Yao, Zemin Feng, Yongchun Liu, Yele Sun, Jun Zheng, Chao Yan, Federico Bianchi, Markku Kulmala, Claudia Mohr, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 22, 1251–1269, https://doi.org/10.5194/acp-22-1251-2022, https://doi.org/10.5194/acp-22-1251-2022, 2022
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This study investigates the connection between organic aerosol (OA) molecular composition and particle absorptive properties in autumn in Beijing. We find that the molecular properties of OA compounds in different episodes influence particle light absorption properties differently: the light absorption enhancement of black carbon and light absorption coefficient of brown carbon were mostly related to more oxygenated OA (low C number and four O atoms) and aromatics/nitro-aromatics, respectively.
Jessica M. Burger, Julie Granger, Emily Joyce, Meredith G. Hastings, Kurt A. M. Spence, and Katye E. Altieri
Atmos. Chem. Phys., 22, 1081–1096, https://doi.org/10.5194/acp-22-1081-2022, https://doi.org/10.5194/acp-22-1081-2022, 2022
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The nitrogen (N) isotopic composition of atmospheric nitrate in the Southern Ocean (SO) marine boundary layer (MBL) reveals the importance of oceanic alkyl nitrate emissions as a source of reactive N to the atmosphere. The oxygen isotopic composition suggests peroxy radicals contribute up to 63 % to NO oxidation and that nitrate forms via the OH pathway. This work improves our understanding of reactive N sources and cycling in a remote marine region, a proxy for the pre-industrial atmosphere.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys., 22, 805–821, https://doi.org/10.5194/acp-22-805-2022, https://doi.org/10.5194/acp-22-805-2022, 2022
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. CHOCHO concentration was high in large cities, aromatics being the most important precursors. Loss path to aerosol was the highest sink, contributing to ~ 20 % of secondary organic aerosol formation. Our work highlights that simple CHOCHO surface uptake approach is valid only for low aerosol conditions and more work is required to understand CHOCHO solubility in high-aerosol conditions.
Juanjuan Qin, Jihua Tan, Xueming Zhou, Yanrong Yang, Yuanyuan Qin, Xiaobo Wang, Shaoxuan Shi, Kang Xiao, and Xinming Wang
Atmos. Chem. Phys., 22, 465–479, https://doi.org/10.5194/acp-22-465-2022, https://doi.org/10.5194/acp-22-465-2022, 2022
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Water-soluble organic compounds (WSOCs) play important roles in atmospheric particle formation, migration, and transformation processes. In this work, size-segregated atmospheric particles were collected in a rural area of Beijing, and 3D fluorescence spectroscopy was used to investigate the optical properties of WSOCs as a means of inferring information about their atmospheric sources. It was found that these data could efficiently reveal the secondary transformation processes of WSOCs.
Guangjie Zheng, Hang Su, Siwen Wang, Andrea Pozzer, and Yafang Cheng
Atmos. Chem. Phys., 22, 47–63, https://doi.org/10.5194/acp-22-47-2022, https://doi.org/10.5194/acp-22-47-2022, 2022
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The recently proposed multiphase buffer theory provides a framework to reconstruct long-term trends and spatial variations in aerosol pH, while non-ideality is a major limitation for its broad applications. Here we proposed a parameterization method to estimate the impact of non-ideality and validated it against long-term observations and global simulations. With this method, the multiphase buffer theory can reproduce well aerosol pH variations estimated by comprehensive thermodynamic models.
Yee Ka Wong, Kin Man Liu, Claisen Yeung, Kenneth K. M. Leung, and Jian Zhen Yu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1030, https://doi.org/10.5194/acp-2021-1030, 2021
Revised manuscript accepted for ACP
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Coarse PM has been shown to cause adverse health impacts, but compared to PM2.5, the source of coarse PM is much less studied through field measurements. We collected chemical composition data for coarse PM in Hong Kong for a one year period. Using statistical models to analyze the data, we found that regional transport of fugitive dust is responsible for the elevated coarse PM. This work sets an example of how field measurements can be effectively utilized for evidence-based policymaking.
Lingling Xu, Jiayan Shi, Yuping Chen, Yanru Zhang, Mengrong Yang, Yanting Chen, Liqian Yin, Lei Tong, Hang Xiao, and Jinsheng Chen
Atmos. Chem. Phys., 21, 18543–18555, https://doi.org/10.5194/acp-21-18543-2021, https://doi.org/10.5194/acp-21-18543-2021, 2021
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Mercury (Hg) isotopic compositions in aerosols are the mixed results of emission sources and atmospheric processes. This study presents Hg isotopic compositions in PM2.5 from different types of locations and total Hg from offshore surface seawater. The results indicate that atmospheric transformations induce significant mass independent fractionation of Hg isotopes, which obscures Hg isotopic signatures of initial emissions.
Michael A. Battaglia Jr., Nicholas Balasus, Katherine Ball, Vanessa Caicedo, Ruben Delgado, Annmarie G. Carlton, and Christopher J. Hennigan
Atmos. Chem. Phys., 21, 18271–18281, https://doi.org/10.5194/acp-21-18271-2021, https://doi.org/10.5194/acp-21-18271-2021, 2021
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This study characterizes aerosol liquid water content and aerosol pH at a land–water transition site near Baltimore, Maryland. We characterize the effects of unique meteorology associated with the close proximity to the Chesapeake Bay and episodic NH3 events derived from industrial and agricultural sources on aerosol chemistry during the summer. We also examine two events where primary Bay emissions underwent aging in the polluted urban atmosphere.
Nabil Deabji, Khanneh Wadinga Fomba, Souad El Hajjaji, Abdelwahid Mellouki, Laurent Poulain, Sebastian Zeppenfeld, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 18147–18174, https://doi.org/10.5194/acp-21-18147-2021, https://doi.org/10.5194/acp-21-18147-2021, 2021
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Mountain and high-altitude sites provide representative data for the lower free troposphere, various pathways for aerosol interactions, and changing boundary layer heights useful in understanding atmospheric composition. However, only few studies exist in African regions despite diversity in both natural and anthropogenic emissions. This study provides detailed atmospheric studies in the northern African high-altitude region.
Jay M. Tomlin, Kevin A. Jankowski, Daniel P. Veghte, Swarup China, Peiwen Wang, Matthew Fraund, Johannes Weis, Guangjie Zheng, Yang Wang, Felipe Rivera-Adorno, Shira Raveh-Rubin, Daniel A. Knopf, Jian Wang, Mary K. Gilles, Ryan C. Moffet, and Alexander Laskin
Atmos. Chem. Phys., 21, 18123–18146, https://doi.org/10.5194/acp-21-18123-2021, https://doi.org/10.5194/acp-21-18123-2021, 2021
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Analysis of individual atmospheric particles shows that aerosol transported from North America during meteorological dry intrusion episodes may have a substantial impact on the mixing state and particle-type population over the mid-Atlantic, as organic contribution and particle-type diversity are significantly enhanced during these periods. These observations need to be considered in current atmospheric models.
Qi En Zhong, Chunlei Cheng, Zaihua Wang, Lei Li, Mei Li, Dafeng Ge, Lei Wang, Yuanyuan Li, Wei Nie, Xuguang Chi, Aijun Ding, Suxia Yang, Duohong Chen, and Zhen Zhou
Atmos. Chem. Phys., 21, 17953–17967, https://doi.org/10.5194/acp-21-17953-2021, https://doi.org/10.5194/acp-21-17953-2021, 2021
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Particulate amines play important roles in new particle formation, aerosol acidity, and hygroscopicity. Most of the field observations did not distinguish the different behavior of each type amine under the same ambient influencing factors. In this study, two amine-containing single particles exhibited different mixing states and disparate enrichment of secondary organics, which provide insight into the discriminated fates of organics during the formation and evolution processes.
Liang Xu, Xiaohuan Liu, Huiwang Gao, Xiaohong Yao, Daizhou Zhang, Lei Bi, Lei Liu, Jian Zhang, Yinxiao Zhang, Yuanyuan Wang, Qi Yuan, and Weijun Li
Atmos. Chem. Phys., 21, 17715–17726, https://doi.org/10.5194/acp-21-17715-2021, https://doi.org/10.5194/acp-21-17715-2021, 2021
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We quantified different types of marine aerosols and explored the Cl depletion of sea salt aerosol (SSA) in the eastern China seas and the northwestern Pacific Ocean. We found that anthropogenic acidic gases in the troposphere were transported longer distances compared to the anthropogenic aerosols and could significantly impact remote marine aerosols. Meanwhile, variations of chloride depletion in SSA can serve as a potential indicator for anthropogenic gaseous pollutants in remote marine air.
Jean-Eudes Petit, Jean-Charles Dupont, Olivier Favez, Valérie Gros, Yunjiang Zhang, Jean Sciare, Leila Simon, François Truong, Nicolas Bonnaire, Tanguy Amodeo, Robert Vautard, and Martial Haeffelin
Atmos. Chem. Phys., 21, 17167–17183, https://doi.org/10.5194/acp-21-17167-2021, https://doi.org/10.5194/acp-21-17167-2021, 2021
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The COVID-19 outbreak led to lockdowns at national scales in spring 2020. Large cuts in emissions occurred, but the quantitative assessment of their role from observations is hindered by weather and interannual variability. That is why we developed an innovative methodology in order to best characterize the impact of lockdown on atmospheric chemistry. We find that a local decrease in traffic-related pollutants triggered a decrease of secondary aerosols and an increase in ozone.
Manuela van Pinxteren, Tiera-Brandy Robinson, Sebastian Zeppenfeld, Xianda Gong, Enno Bahlmann, Khanneh Wadinga Fomba, Nadja Triesch, Frank Stratmann, Oliver Wurl, Anja Engel, Heike Wex, and Hartmut Herrmann
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-845, https://doi.org/10.5194/acp-2021-845, 2021
Revised manuscript accepted for ACP
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A class of marine particles (Transparent exopolymer particles – TEP) that is ubiquitously found in the world oceans was measured for the first time in ambient marine aerosol particles and marine clouds in the tropical Atlantic Ocean. TEP are likely to have good properties to influence clouds. We show that TEP are transferred from the ocean to the marine atmosphere via sea spray formation and our results suggest that they can also form directly in the aerosol particles and in cloud water.
Alexander A. T. Bui, Henry W. Wallace, Sarah Kavassalis, Hariprasad D. Alwe, James H. Flynn, Matt H. Erickson, Sergio Alvarez, Dylan B. Millet, Allison L. Steiner, and Robert J. Griffin
Atmos. Chem. Phys., 21, 17031–17050, https://doi.org/10.5194/acp-21-17031-2021, https://doi.org/10.5194/acp-21-17031-2021, 2021
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Differences in atmospheric species above and below a forest canopy provide insight into the relative importance of local mixing, long-range transport, and chemical processes in determining vertical gradients in atmospheric particles in a forested environment. This helps in understanding the flux of climate-relevant material out of the forest to the atmosphere. We studied this in a remote forest using vertically resolved measurements of gases and particles.
Sharmine Akter Simu, Yuzo Miyazaki, Eri Tachibana, Henning Finkenzeller, Jérôme Brioude, Aurélie Colomb, Olivier Magand, Bert Verreyken, Stephanie Evan, Rainer Volkamer, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 21, 17017–17029, https://doi.org/10.5194/acp-21-17017-2021, https://doi.org/10.5194/acp-21-17017-2021, 2021
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The tropical Indian Ocean (IO) is expected to be a significant source of water-soluble organic carbon (WSOC), which is relevant to cloud formation. Our study showed that marine secondary organic formation dominantly contributed to the aerosol WSOC mass at the high-altitude observatory in the southwest IO in the wet season in both marine boundary layer and free troposphere (FT). This suggests that the effect of marine secondary sources is important up to FT, a process missing in climate models.
Larissa Lacher, Hans-Christian Clemen, Xiaoli Shen, Stephan Mertes, Martin Gysel-Beer, Alireza Moallemi, Martin Steinbacher, Stephan Henne, Harald Saathoff, Ottmar Möhler, Kristina Höhler, Thea Schiebel, Daniel Weber, Jann Schrod, Johannes Schneider, and Zamin A. Kanji
Atmos. Chem. Phys., 21, 16925–16953, https://doi.org/10.5194/acp-21-16925-2021, https://doi.org/10.5194/acp-21-16925-2021, 2021
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We investigate ice-nucleating particle properties at Jungfraujoch during the 2017 joint INUIT/CLACE field campaign, to improve the knowledge about those rare particles in a cloud-relevant environment. By quantifying ice-nucleating particles in parallel to single-particle mass spectrometry measurements, we find that mineral dust and aged sea spray particles are potential candidates for ice-nucleating particles. Our findings are supported by ice residual analysis and source region modeling.
Haoran Yu, Joseph Varghese Puthussery, Yixiang Wang, and Vishal Verma
Atmos. Chem. Phys., 21, 16363–16386, https://doi.org/10.5194/acp-21-16363-2021, https://doi.org/10.5194/acp-21-16363-2021, 2021
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We assessed the oxidative potential (OP) of ambient PM2.5 collected from many sites in the US Midwest through multiple acellular endpoints. Compared to homogeneously distributed PM2.5, OP showed higher spatiotemporal variation. Poor correlations for the regression between mass and OP indicated a limited role of mass in determining the OP. Moreover, weak correlations among different OP endpoints justify the need for using multiple assays to determine oxidative levels of particles.
Xinyao Feng, Yingze Tian, Qianqian Xue, Danlin Song, Fengxia Huang, and Yinchang Feng
Atmos. Chem. Phys., 21, 16219–16235, https://doi.org/10.5194/acp-21-16219-2021, https://doi.org/10.5194/acp-21-16219-2021, 2021
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This study focused on PM2.5 compositions and sources and explored their spatiotemporal and policy-related variations based on observation at 19 sites during wintertime of 2015–2019 in a fast-developing megacity. We found that PM2.5 compositions for the outermost zone in 2019 were similar to those for the core zone 2 or 3 years ago. Percentage contributions of coal and biomass combustion dramatically declined in the core zone, while the traffic source showed an increasing trend.
Minako Kurisu, Kohei Sakata, Mitsuo Uematsu, Akinori Ito, and Yoshio Takahashi
Atmos. Chem. Phys., 21, 16027–16050, https://doi.org/10.5194/acp-21-16027-2021, https://doi.org/10.5194/acp-21-16027-2021, 2021
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Aerosol iron (Fe) input can enhance oceanic primary production. We analyzed Fe isotope ratios of size-fractionated aerosols over the northwestern Pacific to evaluate the contribution of natural and combustion Fe. It was found that combustion Fe was an important soluble Fe source in marine aerosols and possibly in surface seawater when air masses were from East Asia. This study shows the applicability of Fe isotope ratios for a more quantitative understanding of the Fe cycle in the surface ocean.
Kaori Kawana, Kazuhiko Matsumoto, Fumikazu Taketani, Takuma Miyakawa, and Yugo Kanaya
Atmos. Chem. Phys., 21, 15969–15983, https://doi.org/10.5194/acp-21-15969-2021, https://doi.org/10.5194/acp-21-15969-2021, 2021
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Atmospheric autofluorescent particles observed over the central Pacific Ocean were identified as bioaerosols from comparisons to a DNA-nuclear-staining method. Their number concentrations in the pristine marine air masses showed high correlations with concentrations of bacteria and transparent exopolymer particles in the surface seawater, providing strong evidence of their marine origins. We propose equations to derive the atmospheric bioaerosol number concentrations from oceanic parameters.
Yange Deng, Hiroaki Fujinari, Hikari Yai, Kojiro Shimada, Yuzo Miyazaki, Eri Tachibana, Dhananjay Deshmukh, Kimitaka Kawamura, Tomoki Nakayama, Shiori Tatsuta, Mingfu Cai, Hanbing Xu, Fei Li, Haobo Tan, Sho Ohata, Yutaka Kondo, Akinori Takami, Shiro Hatakeyama, and Michihiro Mochida
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-704, https://doi.org/10.5194/acp-2021-704, 2021
Revised manuscript accepted for ACP
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Offline analyses of the hygroscopicity and composition of atmospheric aerosols is complementary to online analyses in view of the applicability to broader sizes, specific compound groups, and investigations at remote sites. This offline study characterized the composition of water-soluble matter in aerosols and their humidity-dependent hygroscopicity in Okinawa, a receptor site of East Asian outflow. Further, comparison with online analyses showed the appropriateness of the offline method.
Yuan Cheng, Qin-qin Yu, Jiu-meng Liu, Xu-bing Cao, Ying-jie Zhong, Zhen-yu Du, Lin-lin Liang, Guan-nan Geng, Wan-li Ma, Hong Qi, Qiang Zhang, and Ke-bin He
Atmos. Chem. Phys., 21, 15199–15211, https://doi.org/10.5194/acp-21-15199-2021, https://doi.org/10.5194/acp-21-15199-2021, 2021
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Open burning policies in Heilongjiang Province experienced a rapid transition during 2018 to 2020. This study evaluated the responses of PM2.5 pollution to this transition and suggested that neither of the policies could be considered successful. In addition, heterogeneous reactions were found to be at play in secondary aerosol formation, even in the frigid atmosphere in Heilongjiang. The unique haze in northeast China deserves more attention.
Gang Chen, Yulia Sosedova, Francesco Canonaco, Roman Fröhlich, Anna Tobler, Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Christoph Hueglin, Peter Graf, Urs Baltensperger, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 15081–15101, https://doi.org/10.5194/acp-21-15081-2021, https://doi.org/10.5194/acp-21-15081-2021, 2021
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A novel, advanced source apportionment technique was applied to a dataset measured in Magadino. Rolling positive matrix factorisation (PMF) allows for retrieving more realistic, time-dependent, and detailed information on organic aerosol sources. The strength of the rolling PMF mechanism is highlighted by comparing it with results derived from conventional seasonal PMF. Overall, this comprehensive interpretation of aerosol chemical speciation monitor data could be a role model for similar work.
Anna K. Tobler, Alicja Skiba, Francesco Canonaco, Griša Močnik, Pragati Rai, Gang Chen, Jakub Bartyzel, Miroslaw Zimnoch, Katarzyna Styszko, Jaroslaw Nęcki, Markus Furger, Kazimierz Różański, Urs Baltensperger, Jay G. Slowik, and Andre S. H. Prevot
Atmos. Chem. Phys., 21, 14893–14906, https://doi.org/10.5194/acp-21-14893-2021, https://doi.org/10.5194/acp-21-14893-2021, 2021
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Kraków is among the cities with the highest particulate matter levels within Europe. We conducted long-term and highly time-resolved measurements of the chemical composition of submicron particlulate matter (PM1). Combined with advanced source apportionment techniques, which allow for time-dependent factor profiles, our results elucidate that traffic and residential heating (biomass burning and coal combustion) as well as oxygenated organic aerosol are the key PM sources in Kraków.
Sanna Saarikoski, Jarkko V. Niemi, Minna Aurela, Liisa Pirjola, Anu Kousa, Topi Rönkkö, and Hilkka Timonen
Atmos. Chem. Phys., 21, 14851–14869, https://doi.org/10.5194/acp-21-14851-2021, https://doi.org/10.5194/acp-21-14851-2021, 2021
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This study presents the main sources of black carbon (BC) at two urban environments. The largest fraction of BC originated from biomass burning at the residential site (38 %) and from vehicular emissions (57 %) in the street canyon. Also, a significant fraction of BC was associated with urban background or long-range transport. The data are needed by modelers and authorities when assessing climate and air quality impact of BC as well as directing the emission legislation and mitigation actions.
Quan Liu, Dantong Liu, Yangzhou Wu, Kai Bi, Wenkang Gao, Ping Tian, Delong Zhao, Siyuan Li, Chenjie Yu, Guiqian Tang, Yunfei Wu, Kang Hu, Shuo Ding, Qian Gao, Fei Wang, Shaofei Kong, Hui He, Mengyu Huang, and Deping Ding
Atmos. Chem. Phys., 21, 14749–14760, https://doi.org/10.5194/acp-21-14749-2021, https://doi.org/10.5194/acp-21-14749-2021, 2021
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Through simultaneous online measurements of detailed aerosol compositions at both surface and surface-influenced mountain sites, the evolution of aerosol composition during daytime vertical transport was investigated. The results show that, from surface to the top of the planetary boundary layer, the oxidation state of organic aerosol had been significantly enhanced due to evaporation and further oxidation of these evaporated gases.
Magdalena Reizer, Giulia Calzolai, Katarzyna Maciejewska, José A. G. Orza, Luca Carraresi, Franco Lucarelli, and Katarzyna Juda-Rezler
Atmos. Chem. Phys., 21, 14471–14492, https://doi.org/10.5194/acp-21-14471-2021, https://doi.org/10.5194/acp-21-14471-2021, 2021
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The elemental composition of atmospheric PM2.5 and PM2.5–10 was measured during wintertime, with 1 h resolution, using a streaker sampler for the first time at a Central European urban background site. A set of multivariate and wind- and trajectory-based receptor models identified the main sources of ambient aerosol. Fine PM fraction was mainly comprised of regionally transported aged secondary sulfate from residential solid fuel combustion, while the coarse mode showed traffic-related origins.
Tatiana Drotikova, Alena Dekhtyareva, Roland Kallenborn, and Alexandre Albinet
Atmos. Chem. Phys., 21, 14351–14370, https://doi.org/10.5194/acp-21-14351-2021, https://doi.org/10.5194/acp-21-14351-2021, 2021
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A total of 86 polycyclic aromatic compounds (PACs), toxic compounds mainly emitted after fossil fuel combustion, were measured during 8 months in the urban air of Longyearbyen (78° N, 15° E), the most populated settlement in Svalbard. Contrary to a stereotype of pristine Arctic conditions with very low human activity, considerable PAC concentrations were detected, with spring levels comparable to European levels. Air pollution was caused by local snowmobiles in spring and shipping in summer.
John MacInnis, Jai Prakash Chaubey, Crystal Weagle, David Atkinson, and Rachel Ying-Wen Chang
Atmos. Chem. Phys., 21, 14199–14213, https://doi.org/10.5194/acp-21-14199-2021, https://doi.org/10.5194/acp-21-14199-2021, 2021
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This study measured particulate matter in the western Canadian Arctic during 2018 as part of the Year of Polar Prediction. It was found that the particles were likely from the ocean, soil, road dust, and combustion. The concentrations of small aerosol particles, which can affect human health, were low, suggesting they had little impact on local air quality. These results can be used to understand future changes in local aerosol particle sources and concentrations.
Yongchun Liu, Zemin Feng, Feixue Zheng, Xiaolei Bao, Pengfei Liu, Yanli Ge, Yan Zhao, Tao Jiang, Yunwen Liao, Yusheng Zhang, Xiaolong Fan, Chao Yan, Biwu Chu, Yonghong Wang, Wei Du, Jing Cai, Federico Bianchi, Tuukka Petäjä, Yujing Mu, Hong He, and Markku Kulmala
Atmos. Chem. Phys., 21, 13269–13286, https://doi.org/10.5194/acp-21-13269-2021, https://doi.org/10.5194/acp-21-13269-2021, 2021
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The mechanisms and kinetics of particulate sulfate formation in the atmosphere are still open questions although they have been extensively discussed. We found that uptake of SO2 is the rate-determining step for the conversion of SO2 to particulate sulfate. NH4NO3 plays an important role in AWC, the phase state of aerosol particles, and subsequently the uptake kinetics of SO2 under high-RH conditions. This work is a good example of the feedback between aerosol physics and aerosol chemistry.
Alex R. Baker and Chan Yodle
Atmos. Chem. Phys., 21, 13067–13076, https://doi.org/10.5194/acp-21-13067-2021, https://doi.org/10.5194/acp-21-13067-2021, 2021
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Iodine is emitted from the ocean and helps to destroy ozone in the lower atmosphere before being taken up into aerosol particles. We measured the chemical forms of iodine in aerosols over the Atlantic Ocean, because some of these forms can return to the gas phase and destroy more ozone. Our results indicate that aerosol acidity exerts a strong control on iodine speciation and therefore on its recycling behaviour and impact on ozone concentrations.
Nicholas Balasus, Michael A. Battaglia Jr., Katherine Ball, Vanessa Caicedo, Ruben Delgado, Annmarie G. Carlton, and Christopher J. Hennigan
Atmos. Chem. Phys., 21, 13051–13065, https://doi.org/10.5194/acp-21-13051-2021, https://doi.org/10.5194/acp-21-13051-2021, 2021
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Measurements of aerosol and gas composition were carried out at a land–water transition site near Baltimore, MD. Gas-phase ammonia concentrations were highly elevated compared to measurements at a nearby inland site. Our analysis reveals that NH2 was from both industrial and agricultural sources. This had a pronounced effect on aerosol chemical composition at the site, most notably contributing to episodic spikes of aerosol nitrate.
Hong Ren, Wei Hu, Lianfang Wei, Siyao Yue, Jian Zhao, Linjie Li, Libin Wu, Wanyu Zhao, Lujie Ren, Mingjie Kang, Qiaorong Xie, Sihui Su, Xiaole Pan, Zifa Wang, Yele Sun, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 21, 12949–12963, https://doi.org/10.5194/acp-21-12949-2021, https://doi.org/10.5194/acp-21-12949-2021, 2021
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This study presents vertical profiles of biogenic and anthropogenic secondary organic aerosols (SOAs) in the urban boundary layer based on a 325 m tower in Beijing in late summer. The increases in the isoprene and toluene SOAs with height were found to be more related to regional transport, whereas the decrease in those from monoterpenes and sesquiterpene were more subject to local emissions. Such complicated vertical distributions of SOA should be considered in future modeling work.
Vaios Moschos, Martin Gysel-Beer, Robin L. Modini, Joel C. Corbin, Dario Massabò, Camilla Costa, Silvia G. Danelli, Athanasia Vlachou, Kaspar R. Daellenbach, Sönke Szidat, Paolo Prati, André S. H. Prévôt, Urs Baltensperger, and Imad El Haddad
Atmos. Chem. Phys., 21, 12809–12833, https://doi.org/10.5194/acp-21-12809-2021, https://doi.org/10.5194/acp-21-12809-2021, 2021
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This study provides a holistic approach to studying the spectrally resolved light absorption by atmospheric brown carbon (BrC) and black carbon using long time series of daily samples from filter-based measurements. The obtained results provide (1) a better understanding of the aerosol absorption profile and its dependence on BrC and on lensing from less absorbing coatings and (2) an estimation of the most important absorbers at typical European locations.
Michele Bertò, David Cappelletti, Elena Barbaro, Cristiano Varin, Jean-Charles Gallet, Krzysztof Markowicz, Anna Rozwadowska, Mauro Mazzola, Stefano Crocchianti, Luisa Poto, Paolo Laj, Carlo Barbante, and Andrea Spolaor
Atmos. Chem. Phys., 21, 12479–12493, https://doi.org/10.5194/acp-21-12479-2021, https://doi.org/10.5194/acp-21-12479-2021, 2021
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We present the daily and seasonal variability in black carbon (BC) in surface snow inferred from two specific experiments based on the hourly and daily time resolution sampling during the Arctic spring in Svalbard. These unique data sets give us, for the first time, the opportunity to evaluate the associations between the observed surface snow BC mass concentration and a set of predictors corresponding to the considered meteorological and snow physico-chemical parameters.
Zhuohui Lin, Yonghong Wang, Feixue Zheng, Ying Zhou, Yishuo Guo, Zemin Feng, Chang Li, Yusheng Zhang, Simo Hakala, Tommy Chan, Chao Yan, Kaspar R. Daellenbach, Biwu Chu, Lubna Dada, Juha Kangasluoma, Lei Yao, Xiaolong Fan, Wei Du, Jing Cai, Runlong Cai, Tom V. Kokkonen, Putian Zhou, Lili Wang, Tuukka Petäjä, Federico Bianchi, Veli-Matti Kerminen, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 12173–12187, https://doi.org/10.5194/acp-21-12173-2021, https://doi.org/10.5194/acp-21-12173-2021, 2021
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We find that ammonium nitrate and aerosol water content contributed most during low mixing layer height conditions; this may further trigger enhanced formation of sulfate and organic aerosol via heterogeneous reactions. The results of this study contribute towards a more detailed understanding of the aerosol–chemistry–radiation–boundary layer feedback that is likely to be responsible for explosive aerosol mass growth events in urban Beijing.
Zhenzhen Wang, Di Wu, Zhuoyu Li, Xiaona Shang, Qing Li, Xiang Li, Renjie Chen, Haidong Kan, Huiling Ouyang, Xu Tang, and Jianmin Chen
Atmos. Chem. Phys., 21, 12227–12241, https://doi.org/10.5194/acp-21-12227-2021, https://doi.org/10.5194/acp-21-12227-2021, 2021
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This study firstly investigates the composition of sugars in the fine fraction of aerosol over three sites in southwest China. The result suggested no significant reduction in biomass burning emissions in southwest Yunnan Province to some extent. The result shown sheds light on the contributions of biomass burning and the characteristics of biogenic saccharides in these regions, which could be further applied to regional source apportionment models and global climate models.
Cited articles
Bei, N., Wu, J., Elser, M., Feng, T., Cao, J., El-Haddad, I., Li, X., Huang, R., Li, Z.,
Long, X., Xing, L., Zhao, S., Tie, X., Prévôt, A. S. H., and Li, G.: Impacts of meteorological uncertainties on the haze formation in Beijing–Tianjin–Hebei (BTH) during wintertime: a case study, Atmos. Chem. Phys., 17, 14579–14591, https://doi.org/10.5194/acp-17-14579-2017, 2017.
Bougiatioti, A., Nikolaou, P., Stavroulas, I., Kouvarakis, G., Weber, R., Nenes, A., Kanakidou, M., and Mihalopoulos, N.: Particle water and pH in the eastern Mediterranean: source variability and implications for nutrient availability, Atmos. Chem. Phys., 16, 4579–4591, https://doi.org/10.5194/acp-16-4579-2016, 2016.
Chan, C. K. and Yao, X.: Air pollution in mega cities in China, Atmos.
Environ., 42, 1–42, https://doi.org/10.1016/j.atmosenv.2007.09.003, 2008.
Chen, L. H., Sun, Y. Y., Wu, X. C., Zhang, Y. X., Zheng, C. H., Gao, X., and
Cen, K.: Unit-based emission inventory and uncertainty assessment of
coal-fired power plants, Atmos. Environ., 99, 527–535,
https://doi.org/10.1016/j.atmosenv.2014.10.023, 2014.
Cheng, Y., Zheng, G., Wei, C., Mu, Q., Zheng, B., Wang, Z., Gao, M., Zhang,
Q., He, K., Carmichael, G., Pöschl, U., and Su, H.: Reactive nitrogen
chemistry in aerosol water as a source of sulfate during haze events in
China, Sci. Adv., 2, 1–11, https://doi.org/10.1126/sciadv.1601530, 2016.
Clifton, C. L., Altstein, N., and Huie, R. E.: Rate-constant for the
reaction of NO2 with sulfur(IV) over the pH range 5.3–13, Environ. Sci.
Technol., 22, 586–589, https://doi.org/10.1021/es00170a018, 1988.
Dai, Q., Bi, X., Song, W., Li, T., Liu, B., Ding, J., Xu, J., Song, C.,
Yang, N., Schulze, B. C., Zhang, Y., Feng, Y., and Hopke, P. K.: Residential
coal combustion as a source of primary sulfate in Xi'an, China, Atmos.
Environ., 196, 66–76, https://doi.org/10.1016/j.atmosenv.2018.10.002, 2019.
Ding, J., Zhao, P., Su, J., Dong, Q., Du, X., and Zhang, Y.: Aerosol pH and its driving factors in Beijing, Atmos. Chem. Phys., 19, 7939–7954, https://doi.org/10.5194/acp-19-7939-2019, 2019.
Du, Q., Zhang, C., Mu, Y., Cheng, Y., Zhang, Y., Liu, C., Song, M., Tian,
D., Liu, P., Liu, J., Xue, C., and Ye, C.: An important missing source of
atmospheric carbonyl sulfide: Domestic coal combustion, Geophys. Res.
Lett., 43, 8720–8727, https://doi.org/10.1002/2016gl070075, 2016.
Fountoukis, C. and Nenes, A.: ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K+-Ca2+-Mg2+-
Graedel, T. E. and Weschler, C. J.: Chemistry within aqueous atmospheric
aerosols and raindrops, Rev. Geophys., 19, 505–539,
https://doi.org/10.1029/RG019i004p00505, 1981.
Guo, H., Xu, L., Bougiatioti, A., Cerully, K. M., Capps, S. L., Hite Jr., J. R., Carlton, A. G., Lee, S.-H., Bergin, M. H., Ng, N. L., Nenes, A., and Weber, R. J.: Fine-particle water and pH in the southeastern United States, Atmos. Chem. Phys., 15, 5211–5228, https://doi.org/10.5194/acp-15-5211-2015, 2015.
Guo, H., Weber, R. J., and Nenes, A.: High levels of ammonia do not raise
fine particle pH sufficiently to yield nitrogen oxide-dominated sulfate
production, Sci. Rep.-UK, 7, 12109, https://doi.org/10.1038/s41598-017-11704-0, 2017.
Guo, S., Hu, M., Zamora, M. L., Peng, J., Shang, D., Zheng, J., Du, Z., Wu,
Z., Shao, M., Zeng, L., Molina, M. J., and Zhang, R.: Elucidating severe
urban haze formation in China, P. Natl. Acad.
Sci. USA, 111, 17373–17378,
https://doi.org/10.1073/pnas.1419604111, 2014.
He, H., Wang, Y., Ma, Q., Ma, J., Chu, B., Ji, D., Tang, G., Liu, C., Zhang,
H., and Hao, J.: Mineral dust and NOx promote the conversion of
SO2 to sulfate in heavy pollution days, Sci. Rep.-UK, 4, 1–5,
https://doi.org/10.1038/srep04172, 2014.
He, P., Xie, Z., Chi, X., Yu, X., Fan, S., Kang, H., Liu, C., and Zhan, H.: Atmospheric
Hennigan, C. J., Izumi, J., Sullivan, A. P., Weber, R. J., and Nenes, A.: A critical evaluation of proxy methods used to estimate the acidity of atmospheric particles, Atmos. Chem. Phys., 15, 2775–2790, https://doi.org/10.5194/acp-15-2775-2015, 2015.
Huang, R. J., Zhang, Y., Bozzetti, C., Ho, K. F., Cao, J. J., Han, Y.,
Daellenbach, K. R., Slowik, J. G., Platt, S. M., Canonaco, F., Zotter, P.,
Wolf, R., Pieber, S. M., Bruns, E. A., Crippa, M., Ciarelli, G.,
Piazzalunga, A., Schwikowski, M., Abbaszade, G., Schnelle-Kreis, J.,
Zimmermann, R., An, Z., Szidat, S., Baltensperger, U., El Haddad, I., and
Prevot, A. S.: High secondary aerosol contribution to particulate pollution
during haze events in China, Nature, 514, 218–222, https://doi.org/10.1038/nature13774,
2014.
Ibusuki, T. and Takeuchi, K.: Sulfur-dioxide oxidation by oxygen catalyzed
by mixtures of manganese(II) and iron(III) in aqueous-solutions at
environmental reaction conditions, Atmos. Environ., 21, 1555–1560,
https://doi.org/10.1016/0004-6981(87)90317-9, 1987.
Li, G., Bei, N., Cao, J., Huang, R., Wu, J., Feng, T., Wang, Y., Liu, S., Zhang, Q., Tie, X., and Molina, L. T.: A possible pathway for rapid growth of sulfate during haze days in China, Atmos. Chem. Phys., 17, 3301–3316, https://doi.org/10.5194/acp-17-3301-2017, 2017.
Li, J., Liao, H., Hu, J., and Li, N.: Severe particulate pollution days in
China during 2013–2018 and the associated typical weather patterns in
Beijing-Tianjin-Hebei and the Yangtze River Delta regions, Environ. Pollut.,
248, 74–81, https://doi.org/10.1016/j.envpol.2019.01.124, 2019.
Li, L., Hoffmann, M. R., and Colussi, A. J.: Role of nitrogen dioxide in the
production of sulfate during Chinese haze-aerosol episodes, Environ. Sci.
Technol., 52, 2686–2693, https://doi.org/10.1021/acs.est.7b05222, 2018.
Li, Q., Li, X., Jiang, J., Duan, L., Ge, S., Zhang, Q., Deng, J., Wang, S.,
and Hao, J.: Semi-coke briquettes: towards reducing emissions of primary
PM2.5, particulate carbon, and carbon monoxide from household coal
combustion in China, Sci. Rep.-UK, 6, 1–10, https://doi.org/10.1038/srep19306, 2016.
Liu, M., Song, Y., Zhou, T., Xu, Z., Yan, C., Zheng, M., Wu, Z., Hu, M., Wu,
Y., and Zhu, T.: Fine particle pH during severe haze episodes in northern
China, Geophys. Res. Lett., 44, 1–9, https://doi.org/10.1002/2017GL073210, 2017.
Liu, P., Zhang, C., Mu, Y., Liu, C., Xue, C., Ye, C., Liu, J., Zhang, Y., and Zhang, H.: The possible contribution of the periodic emissions from farmers' activities in the North China Plain to atmospheric water-soluble ions in Beijing, Atmos. Chem. Phys., 16, 10097–10109, https://doi.org/10.5194/acp-16-10097-2016, 2016.
Liu, P., Zhang, C., Xue, C., Mu, Y., Liu, J., Zhang, Y., Tian, D., Ye, C., Zhang, H., and Guan, J.: The contribution of residential coal combustion to atmospheric PM2.5 in northern China during winter, Atmos. Chem. Phys., 17, 11503–11520, https://doi.org/10.5194/acp-17-11503-2017, 2017.
Meng, Z. Y., Lin, W. L., Jiang, X. M., Yan, P., Wang, Y., Zhang, Y. M., Jia, X. F., and Yu, X. L.: Characteristics of atmospheric ammonia over Beijing, China, Atmos. Chem. Phys., 11, 6139–6151, https://doi.org/10.5194/acp-11-6139-2011, 2011.
Murphy, J. G., Gregoire, P. K., Tevlin, A. G., Wentworth, G. R., Ellis, R.
A., Markovic, M. Z., and VandenBoer, T. C.: Observational constraints on
particle acidity using measurements and modelling of particles and gases,
Faraday Discuss., 200, 379–395, https://doi.org/10.1039/c7fd00086c, 2017.
Nie, W., Ding, A., Wang, T., Kerminen, V. M., George, C., Xue, L., Wang, W.,
Zhang, Q., Petaja, T., Qi, X., Gao, X., Wang, X., Yang, X., Fu, C., and
Kulmala, M.: Polluted dust promotes new particle formation and growth,
Sci. Rep.-UK, 4, 1–6, https://doi.org/10.1038/srep06634, 2014.
Pathak, R. K., Louie, P. K. K., and Chan, C. K.: Characteristics of aerosol
acidity in Hong kong, Atmos. Environ., 38, 2965–2974,
https://doi.org/10.1016/j.atmosenv.2004.02.044, 2004.
Ponczek, M., Hayeck, N., Emmelin, C., and George, C.: Heterogeneous
photochemistry of dicarboxylic acids on mineral dust, Atmos.
Environ., 212, 262–271, https://doi.org/10.1016/j.atmosenv.2019.05.032, 2019.
Ravishankara, A.: Heterogeneous and multiphase chemistry in the troposphere,
Science, 276, 1058–1065, 1997.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics, from
Air Pollution to Climate Change, John Wiley and Sons, Inc., 429–44, 2006.
Shao, J., Chen, Q., Wang, Y., Lu, X., He, P., Sun, Y., Shah, V., Martin, R. V., Philip, S., Song, S., Zhao, Y., Xie, Z., Zhang, L., and Alexander, B.: Heterogeneous sulfate aerosol formation mechanisms during wintertime Chinese haze events: air quality model assessment using observations of sulfate oxygen isotopes in Beijing, Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, 2019.
Shi, G., Xu, J., Peng, X., Xiao, Z., Chen, K., Tian, Y., Guan, X., Feng, Y.,
Yu, H., Nenes, A., and Russell, A. G.: pH of aerosols in a polluted
atmosphere: source contributions to highly acidic aerosol, Environ. Sci.
Technol., 51, 4289–4296, https://doi.org/10.1021/acs.est.6b05736, 2017.
Sun, Y., Wang, Z., Fu, P., Jiang, Q., Yang, T., Li, J., and Ge, X.: The
impact of relative humidity on aerosol composition and evolution processes
during wintertime in Beijing, China, Atmos. Environ., 77, 927–934,
https://doi.org/10.1016/j.atmosenv.2013.06.019, 2013.
Tang, M., Huang, X., Lu, K., Ge, M., Li, Y., Cheng, P., Zhu, T., Ding, A., Zhang, Y., Gligorovski, S., Song, W., Ding, X., Bi, X., and Wang, X.: Heterogeneous reactions of mineral dust aerosol: implications for tropospheric oxidation capacity, Atmos. Chem. Phys., 17, 11727–11777, https://doi.org/10.5194/acp-17-11727-2017, 2017.
Tham, Y. J., Wang, Z., Li, Q., Wang, W., Wang, X., Lu, K., Ma, N., Yan, C., Kecorius, S., Wiedensohler, A., Zhang, Y., and Wang, T.: Heterogeneous N2O5 uptake coefficient and production yield of ClNO2 in polluted northern China: roles of aerosol water content and chemical composition, Atmos. Chem. Phys., 18, 13155–13171, https://doi.org/10.5194/acp-18-13155-2018, 2018.
Tong, S. R., Hou, S. Q., Zhang, Y., Chu, B. W., Liu, Y. C., He, H., Zhao, P.
S., and Ge, M. F.: Exploring the nitrous acid (HONO) formation mechanism in
winter Beijing: direct emissions and heterogeneous production in urban and
suburban areas, Faraday Discuss., 189, 213–230, https://doi.org/10.1039/c5fd00163c, 2016.
Wang, G., Zhang, R., Gomez, M. E., Yang, L., Levy Zamora, M., Hu, M., Lin,
Y., Peng, J., Guo, S., Meng, J., Li, J., Cheng, C., Hu, T., Ren, Y., Wang,
Y., Gao, J., Cao, J., An, Z., Zhou, W., Li, G., Wang, J., Tian, P.,
Marrero-Ortiz, W., Secrest, J., Du, Z., Zheng, J., Shang, D., Zeng, L.,
Shao, M., Wang, W., Huang, Y., Wang, Y., Zhu, Y., Li, Y., Hu, J., Pan, B.,
Cai, L., Cheng, Y., Ji, Y., Zhang, F., Rosenfeld, D., Liss, P. S., Duce, R.
A., Kolb, C. E., and Molina, M. J.: Persistent sulfate formation from London
Fog to Chinese haze, P. Natl. Acad. Sci. USA, 113, 13630–13635, 2016.
Wang, G., Zhang, F., Peng, J., Duan, L., Ji, Y., Marrero-Ortiz, W., Wang, J., Li, J., Wu, C., Cao, C., Wang, Y., Zheng, J., Secrest, J., Li, Y., Wang, Y., Li, H., Li, N., and Zhang, R.: Particle acidity and sulfate production during severe haze events in China cannot be reliably inferred by assuming a mixture of inorganic salts, Atmos. Chem. Phys., 18, 10123–10132, https://doi.org/10.5194/acp-18-10123-2018, 2018.
Wang, H., Lu, K., Chen, X., Zhu, Q., Wu, Z., Wu, Y., and Sun, K.: Fast particulate nitrate formation via N2O5 uptake aloft in winter in Beijing, Atmos. Chem. Phys., 18, 10483–10495, https://doi.org/10.5194/acp-18-10483-2018, 2018a.
Wang, H., Lu, K., Guo, S., Wu, Z., Shang, D., Tan, Z., Wang, Y., Le Breton, M., Lou, S., Tang, M., Wu, Y., Zhu, W., Zheng, J., Zeng, L., Hallquist, M., Hu, M., and Zhang, Y.: Efficient N2O5 uptake and NO3 oxidation in the outflow of urban Beijing, Atmos. Chem. Phys., 18, 9705–9721, https://doi.org/10.5194/acp-18-9705-2018, 2018b.
Wang, J., Zhang, X., Guo, J., Wang, Z., and Zhang, M.: Observation of
nitrous acid (HONO) in Beijing, China: Seasonal variation, nocturnal
formation and daytime budget, Sci. Total Environ., 587–588,
350–359, https://doi.org/10.1016/j.scitotenv.2017.02.159, 2017.
Wang, Y., Yao, L., Wang, L., Liu, Z., Ji, D., Tang, G., Zhang, J., Sun, Y.,
Hu, B., and Xin, J.: Mechanism for the formation of the January 2013 heavy
haze pollution episode over central and eastern China, Sci. China Earth
Sci., 57, 14–25, https://doi.org/10.1007/s11430-013-4773-4, 2013.
Weber, R. J., Guo, H., Russell, A. G., and Nenes, A.: High aerosol acidity
despite declining atmospheric sulfate concentrations over the past 15 years,
Nat. Geosci., 9, 282–285, https://doi.org/10.1038/ngeo2665, 2016.
Wu, J., Bei, N., Hu, B., Liu, S., Zhou, M., Wang, Q., Li, X., Liu, L., Feng, T., Liu, Z., Wang, Y., Cao, J., Tie, X., Wang, J., Molina, L. T., and Li, G.: Is water vapor a key player of the wintertime haze in North China Plain?, Atmos. Chem. Phys., 19, 8721–8739, https://doi.org/10.5194/acp-19-8721-2019, 2019.
Xu, L., Duan, F., He, K., Ma, Y., Zhu, L., Zheng, Y., Huang, T., Kimoto, T.,
Ma, T., Li, H., Ye, S., Yang, S., Sun, Z., and Xu, B.: Characteristics of
the secondary water-soluble ions in a typical autumn haze in Beijing,
Environ. Pollut., 227, 296–305, https://doi.org/10.1016/j.envpol.2017.04.076, 2017.
Xu, W. Y., Zhao, C. S., Ran, L., Deng, Z. Z., Liu, P. F., Ma, N., Lin, W. L., Xu, X. B., Yan, P., He, X., Yu, J., Liang, W. D., and Chen, L. L.: Characteristics of pollutants and their correlation to meteorological conditions at a suburban site in the North China Plain, Atmos. Chem. Phys., 11, 4353–4369, https://doi.org/10.5194/acp-11-4353-2011, 2011.
Xue, C., Ye, C., Ma, Z., Liu, P., Zhang, Y., Zhang, C., Tang, K., Zhang, W.,
Zhao, X., Wang, Y., Song, M., Liu, J., Duan, J., Qin, M., Tong, S., Ge, M.,
and Mu, Y.: Development of stripping coil-ion chromatograph method and
intercomparison with CEAS and LOPAP to measure atmospheric HONO, Sci. Total Environ., 646, 187–195, https://doi.org/10.1016/j.scitotenv.2018.07.244,
2019a.
Xue, C., Ye, C., Zhang, Y., Ma, Z., Liu, P., Zhang, C., Zhao, X., Liu, J.,
and Mu, Y.: Development and application of a twin open-top chambers method
to measure soil HONO emission in the North China Plain, Sci. Total Environ.,
659, 621–631, https://doi.org/10.1016/j.scitotenv.2018.12.245, 2019b.
Xue, J., Yuan, Z., Griffith, S. M., Yu, X., Lau, A. K., and Yu, J. Z.:
Sulfate Formation Enhanced by a Cocktail of High NOx, SO2,
Particulate Matter, and Droplet pH during Haze-Fog Events in Megacities in
China: An Observation-Based Modeling Investigation, Environ. Sci. Technol., 50,
7325–7334, https://doi.org/10.1021/acs.est.6b00768, 2016.
Yang, Y. R., Liu, X. G., Qu, Y., An, J. L., Jiang, R., Zhang, Y. H., Sun, Y. L., Wu, Z. J., Zhang, F., Xu, W. Q., and Ma, Q. X.: Characteristics and formation mechanism of continuous hazes in China: a case study during the autumn of 2014 in the North China Plain, Atmos. Chem. Phys., 15, 8165–8178, https://doi.org/10.5194/acp-15-8165-2015, 2015.
Ye, C., Liu, P., Ma, Z., Xue, C., Zhang, C., Zhang, Y., Liu, J., Liu, C.,
Sun, X., and Mu, Y.: High H2O2 Concentrations Observed during Haze
Periods during the Winter in Beijing: Importance of H2O2 Oxidation
in Sulfate Formation, Environ. Sci. Tech. Let., 5,
757–763, https://doi.org/10.1021/acs.estlett.8b00579, 2018.
Zhang, H., Chen, S., Zhong, J., Zhang, S., Zhang, Y., Zhang, X., Li, Z., and
Zeng, X. C.: Formation of aqueous-phase sulfate during the haze period in
China: Kinetics and atmospheric implications, Atmos. Environ., 177,
93–99, https://doi.org/10.1016/j.atmosenv.2018.01.017, 2018.
Zhang, Q., He, K. B., and Huo, H.: Cleaning China's air, Nature, 484,
161–162, 2012.
Zhang, R., Wang, G., Guo, S., Zamora, M. L., Ying, Q., Lin, Y., Wang, W.,
Hu, M., and Wang, Y.: Formation of urban fine particulate matter, Chem. Rev.,
115, 3803–3855, https://doi.org/10.1021/acs.chemrev.5b00067, 2015.
Zhao, M., Wang, S., Tan, J., Hua, Y., Wu, D., and Hao, J.: Variation of
Urban Atmospheric Ammonia Pollution and its Relation with PM2.5 Chemical
Property in Winter of Beijing, China, Aerosol Air Qual. Res., 16,
1390–1402, https://doi.org/10.4209/aaqr.2015.12.0699, 2016.
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, Atmos. Chem. Phys., 15, 2031–2049, https://doi.org/10.5194/acp-15-2031-2015, 2015a.
Zheng, G. J., Duan, F. K., Su, H., Ma, Y. L., Cheng, Y., Zheng, B., Zhang, Q., Huang, T., Kimoto, T., Chang, D., Pöschl, U., Cheng, Y. F., and He, K. B.: Exploring the severe winter haze in Beijing: the impact of synoptic weather, regional transport and heterogeneous reactions, Atmos. Chem. Phys., 15, 2969–2983, https://doi.org/10.5194/acp-15-2969-2015, 2015b.
Zhong, J., Zhang, X., Wang, Y., Wang, J., Shen, X., Zhang, H., Wang, T., Xie, Z., Liu, C., Zhang, H., Zhao, T., Sun, J., Fan, S., Gao, Z., Li, Y., and Wang, L.: The two-way feedback mechanism between unfavorable meteorological conditions and cumulative aerosol pollution in various haze regions of China, Atmos. Chem. Phys., 19, 3287–3306, https://doi.org/10.5194/acp-19-3287-2019, 2019.
Short summary
A vast area in China is currently going through severe haze episodes with drastically elevated concentrations of PM2.5 in winter. Nitrate and sulfate are main constituents of PM2.5, but their formations via NO2 and SO2 oxidation are still not comprehensively understood. Our results found that the gas-phase reaction of NO2 with OH and the heterogeneous hydrolysis of N2O5 play key roles in nitrate formation, and SO2 aqueous-phase oxidation with H2O2 rather than NO2 contributed greatly to sulfate.
A vast area in China is currently going through severe haze episodes with drastically elevated...
Altmetrics
Final-revised paper
Preprint