Articles | Volume 16, issue 18
https://doi.org/10.5194/acp-16-11773-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-11773-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
22 Sep 2016
Research article |
| 22 Sep 2016
Isotopic composition for source identification of mercury in atmospheric fine particles
Qiang Huang
SKLEG, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang
550081, China
SKLEG, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang
550081, China
Weilin Huang
Department of Environmental Sciences, Rutgers, The State University of
New Jersey, New Brunswick, NJ 08901, USA
Pingqing Fu
LAPC, Institute of Atmospheric Physics, Chinese Academy of Sciences,
Beijing 100029, China
Benjamin Guinot
Laboratoire d'Aérologie UMR5560 CNRS-Université Toulouse 3,
Toulouse, France
Xinbin Feng
SKLEG, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang
550081, China
Lihai Shang
SKLEG, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang
550081, China
Zhuhong Wang
SKLEG, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang
550081, China
Zhongwei Wang
SKLEG, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang
550081, China
Shengliu Yuan
SKLEG, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang
550081, China
Hongming Cai
SKLEG, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang
550081, China
Lianfang Wei
LAPC, Institute of Atmospheric Physics, Chinese Academy of Sciences,
Beijing 100029, China
Ben Yu
SKLEG, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang
550081, China
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Xueshun Chen, Fangqun Yu, Wenyi Yang, Yele Sun, Huansheng Chen, Wei Du, Jian Zhao, Ying Wei, Lianfang Wei, Huiyun Du, Zhe Wang, Qizhong Wu, Jie Li, Junling An, and Zifa Wang
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Atmospheric aerosol particles have significant climate and health effects that depend on aerosol size, composition, and mixing state. A new global-regional nested aerosol model with an advanced particle microphysics module and a volatility basis set organic aerosol module was developed to simulate aerosol microphysical processes. Simulations strongly suggest the important role of anthropogenic organic species in particle formation over the areas influenced by anthropogenic sources.
Siqi Hou, Di Liu, Jingsha Xu, Tuan V. Vu, Xuefang Wu, Deepchandra Srivastava, Pingqing Fu, Linjie Li, Yele Sun, Athanasia Vlachou, Vaios Moschos, Gary Salazar, Sönke Szidat, André S. H. Prévôt, Roy M. Harrison, and Zongbo Shi
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This study provides a newly developed method which combines radiocarbon (14C) with organic tracers to enable source apportionment of primary and secondary fossil vs. non-fossil sources of carbonaceous aerosols at an urban and a rural site of Beijing. The source apportionment results were compared with those by chemical mass balance and AMS/ACSM-PMF methods. Correlations of WINSOC and WSOC with different sources of OC were also performed to elucidate the formation mechanisms of SOC.
Jingsha Xu, Di Liu, Xuefang Wu, Tuan V. Vu, Yanli Zhang, Pingqing Fu, Yele Sun, Weiqi Xu, Bo Zheng, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 7321–7341, https://doi.org/10.5194/acp-21-7321-2021, https://doi.org/10.5194/acp-21-7321-2021, 2021
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Source apportionment of fine aerosols in an urban site of Beijing used a chemical mass balance (CMB) model. Seven primary sources (industrial/residential coal burning, biomass burning, gasoline/diesel vehicles, cooking and vegetative detritus) explained an average of 75.7 % and 56.1 % of fine OC in winter and summer, respectively. CMB was found to resolve more primary OA sources than AMS-PMF, but the latter apportioned more secondary OA sources.
Philippe Massicotte, Rainer M. W. Amon, David Antoine, Philippe Archambault, Sergio Balzano, Simon Bélanger, Ronald Benner, Dominique Boeuf, Annick Bricaud, Flavienne Bruyant, Gwenaëlle Chaillou, Malik Chami, Bruno Charrière, Jing Chen, Hervé Claustre, Pierre Coupel, Nicole Delsaut, David Doxaran, Jens Ehn, Cédric Fichot, Marie-Hélène Forget, Pingqing Fu, Jonathan Gagnon, Nicole Garcia, Beat Gasser, Jean-François Ghiglione, Gaby Gorsky, Michel Gosselin, Priscillia Gourvil, Yves Gratton, Pascal Guillot, Hermann J. Heipieper, Serge Heussner, Stanford B. Hooker, Yannick Huot, Christian Jeanthon, Wade Jeffrey, Fabien Joux, Kimitaka Kawamura, Bruno Lansard, Edouard Leymarie, Heike Link, Connie Lovejoy, Claudie Marec, Dominique Marie, Johannie Martin, Jacobo Martín, Guillaume Massé, Atsushi Matsuoka, Vanessa McKague, Alexandre Mignot, William L. Miller, Juan-Carlos Miquel, Alfonso Mucci, Kaori Ono, Eva Ortega-Retuerta, Christos Panagiotopoulos, Tim Papakyriakou, Marc Picheral, Louis Prieur, Patrick Raimbault, Joséphine Ras, Rick A. Reynolds, André Rochon, Jean-François Rontani, Catherine Schmechtig, Sabine Schmidt, Richard Sempéré, Yuan Shen, Guisheng Song, Dariusz Stramski, Eri Tachibana, Alexandre Thirouard, Imma Tolosa, Jean-Éric Tremblay, Mickael Vaïtilingom, Daniel Vaulot, Frédéric Vaultier, John K. Volkman, Huixiang Xie, Guangming Zheng, and Marcel Babin
Earth Syst. Sci. Data, 13, 1561–1592, https://doi.org/10.5194/essd-13-1561-2021, https://doi.org/10.5194/essd-13-1561-2021, 2021
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The MALINA oceanographic expedition was conducted in the Mackenzie River and the Beaufort Sea systems. The sampling was performed across seven shelf–basin transects to capture the meridional gradient between the estuary and the open ocean. The main goal of this research program was to better understand how processes such as primary production are influencing the fate of organic matter originating from the surrounding terrestrial landscape during its transition toward the Arctic Ocean.
Steven J. Campbell, Kate Wolfer, Battist Utinger, Joe Westwood, Zhi-Hui Zhang, Nicolas Bukowiecki, Sarah S. Steimer, Tuan V. Vu, Jingsha Xu, Nicholas Straw, Steven Thomson, Atallah Elzein, Yele Sun, Di Liu, Linjie Li, Pingqing Fu, Alastair C. Lewis, Roy M. Harrison, William J. Bloss, Miranda Loh, Mark R. Miller, Zongbo Shi, and Markus Kalberer
Atmos. Chem. Phys., 21, 5549–5573, https://doi.org/10.5194/acp-21-5549-2021, https://doi.org/10.5194/acp-21-5549-2021, 2021
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In this study, we quantify PM2.5 oxidative potential (OP), a metric widely suggested as a potential measure of particle toxicity, in Beijing in summer and winter using four acellular assays. We correlate PM2.5 OP with a comprehensive range of atmospheric and particle composition measurements, demonstrating inter-assay differences and seasonal variation of PM2.5 OP. Using multivariate statistical analysis, we highlight specific particle chemical components and sources that influence OP.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Santosh Kumar Verma, Kimitaka Kawamura, Fei Yang, Pingqing Fu, Yugo Kanaya, and Zifa Wang
Atmos. Chem. Phys., 21, 4959–4978, https://doi.org/10.5194/acp-21-4959-2021, https://doi.org/10.5194/acp-21-4959-2021, 2021
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We studied aerosol samples collected in autumn 2007 with day and night intervals in a rural site of Mangshan, north of Beijing, for sugar compounds (SCs) that are abundant organic aerosol components and can influence the air quality and climate. We found higher concentrations of biomass burning (BB) products at nighttime than daytime, whereas pollen tracers and other SCs showed an opposite diurnal trend, because this site is meteorologically characterized by a mountain/valley breeze.
Lei Liu, Jian Zhang, Yinxiao Zhang, Yuanyuan Wang, Liang Xu, Qi Yuan, Dantong Liu, Yele Sun, Pingqing Fu, Zongbo Shi, and Weijun Li
Atmos. Chem. Phys., 21, 2251–2265, https://doi.org/10.5194/acp-21-2251-2021, https://doi.org/10.5194/acp-21-2251-2021, 2021
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We found that large numbers of light-absorbing primary organic particles with high viscosity, especially tarballs, from domestic coal and biomass burning occurred in rural and even urban hazes in the winter of North China. For the first time, we characterized the atmospheric aging process of these burning-related primary organic particles by microscopic analysis and further evaluated their light absorption enhancement resulting from the “lensing effect” of secondary inorganic coatings.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
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To understand how emission controls will impact ozone, an understanding of the sources and sinks of OH and the chemical cycling between peroxy radicals is needed. This paper presents measurements of OH, HO2 and total RO2 taken in central Beijing. The radical observations are compared to a detailed chemistry model, which shows that under low NO conditions, there is a missing OH source. Under high NOx conditions, the model under-predicts RO2 and impacts our ability to model ozone.
Rutambhara Joshi, Dantong Liu, Eiko Nemitz, Ben Langford, Neil Mullinger, Freya Squires, James Lee, Yunfei Wu, Xiaole Pan, Pingqing Fu, Simone Kotthaus, Sue Grimmond, Qiang Zhang, Ruili Wu, Oliver Wild, Michael Flynn, Hugh Coe, and James Allan
Atmos. Chem. Phys., 21, 147–162, https://doi.org/10.5194/acp-21-147-2021, https://doi.org/10.5194/acp-21-147-2021, 2021
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Black carbon (BC) is a component of particulate matter which has significant effects on climate and human health. Sources of BC include biomass burning, transport, industry and domestic cooking and heating. In this study, we measured BC emissions in Beijing, finding a dominance of traffic emissions over all other sources. The quantitative method presented here has benefits for revising widely used emissions inventories and for understanding BC sources with impacts on air quality and climate.
W. Joe F. Acton, Zhonghui Huang, Brian Davison, Will S. Drysdale, Pingqing Fu, Michael Hollaway, Ben Langford, James Lee, Yanhui Liu, Stefan Metzger, Neil Mullinger, Eiko Nemitz, Claire E. Reeves, Freya A. Squires, Adam R. Vaughan, Xinming Wang, Zhaoyi Wang, Oliver Wild, Qiang Zhang, Yanli Zhang, and C. Nicholas Hewitt
Atmos. Chem. Phys., 20, 15101–15125, https://doi.org/10.5194/acp-20-15101-2020, https://doi.org/10.5194/acp-20-15101-2020, 2020
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Air quality in Beijing is of concern to both policy makers and the general public. In order to address concerns about air quality it is vital that the sources of atmospheric pollutants are understood. This work presents the first top-down measurement of volatile organic compound (VOC) emissions in Beijing. These measurements are used to evaluate the emissions inventory and assess the impact of VOC emission from the city centre on atmospheric chemistry.
Eloise J. Slater, Lisa K. Whalley, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Leigh R. Crilley, Louisa Kramer, William Bloss, Tuan Vu, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 20, 14847–14871, https://doi.org/10.5194/acp-20-14847-2020, https://doi.org/10.5194/acp-20-14847-2020, 2020
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The paper details atmospheric chemistry in a megacity (Beijing), focussing on radicals which mediate the formation of secondary pollutants such as ozone and particles. Highly polluted conditions were experienced, including the highest ever levels of nitric oxide (NO), with simultaneous radical measurements. Radical concentrations were large during "haze" events, demonstrating active photochemistry. Modelling showed that our understanding of the chemistry at high NOx levels is incomplete.
Junjun Deng, Hao Guo, Hongliang Zhang, Jialei Zhu, Xin Wang, and Pingqing Fu
Atmos. Chem. Phys., 20, 14419–14435, https://doi.org/10.5194/acp-20-14419-2020, https://doi.org/10.5194/acp-20-14419-2020, 2020
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One-year source apportionment of BC aerosols in a coastal city in China was conducted with the light-absorption observation-based method and source-oriented model. Source contributions identified by the two source apportionment methods were compared. Temporal variability, potential sources and transport pathways of BC from fossil fuel and biomass burning were characterized. Significant influence of biomass burning in North and East–Central China on BC in the region was highlighted.
Jingsha Xu, Shaojie Song, Roy M. Harrison, Congbo Song, Lianfang Wei, Qiang Zhang, Yele Sun, Lu Lei, Chao Zhang, Xiaohong Yao, Dihui Chen, Weijun Li, Miaomiao Wu, Hezhong Tian, Lining Luo, Shengrui Tong, Weiran Li, Junling Wang, Guoliang Shi, Yanqi Huangfu, Yingze Tian, Baozhu Ge, Shaoli Su, Chao Peng, Yang Chen, Fumo Yang, Aleksandra Mihajlidi-Zelić, Dragana Đorđević, Stefan J. Swift, Imogen Andrews, Jacqueline F. Hamilton, Ye Sun, Agung Kramawijaya, Jinxiu Han, Supattarachai Saksakulkrai, Clarissa Baldo, Siqi Hou, Feixue Zheng, Kaspar R. Daellenbach, Chao Yan, Yongchun Liu, Markku Kulmala, Pingqing Fu, and Zongbo Shi
Atmos. Meas. Tech., 13, 6325–6341, https://doi.org/10.5194/amt-13-6325-2020, https://doi.org/10.5194/amt-13-6325-2020, 2020
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An interlaboratory comparison was conducted for the first time to examine differences in water-soluble inorganic ions (WSIIs) measured by 10 labs using ion chromatography (IC) and by two online aerosol chemical speciation monitor (ACSM) methods. Major ions including SO42−, NO3− and NH4+ agreed well in 10 IC labs and correlated well with ACSM data. WSII interlab variability strongly affected aerosol acidity results based on ion balance, but aerosol pH computed by ISORROPIA II was very similar.
Junfeng Wang, Jianhuai Ye, Dantong Liu, Yangzhou Wu, Jian Zhao, Weiqi Xu, Conghui Xie, Fuzhen Shen, Jie Zhang, Paul E. Ohno, Yiming Qin, Xiuyong Zhao, Scot T. Martin, Alex K. Y. Lee, Pingqing Fu, Daniel J. Jacob, Qi Zhang, Yele Sun, Mindong Chen, and Xinlei Ge
Atmos. Chem. Phys., 20, 14091–14102, https://doi.org/10.5194/acp-20-14091-2020, https://doi.org/10.5194/acp-20-14091-2020, 2020
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We compared the organics in total submicron matter and those coated on BC cores during summertime in Beijing and found large differences between them. Traffic-related OA was associated significantly with BC, while cooking-related OA did not coat BC. In addition, a factor likely originated from primary biomass burning OA was only identified in BC-containing particles. Such a unique BBOA requires further field and laboratory studies to verify its presence and elucidate its properties and impacts.
Jiawei Li, Zhiwei Han, Pingqing Fu, and Xiaohong Yao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1016, https://doi.org/10.5194/acp-2020-1016, 2020
Revised manuscript not accepted
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Organic aerosols of marine origin are so far poorly understood. An on-line coupled regional chemistry-climate model is developed to firstly explore and characterize the seasonality and annual feature of emission, distribution and radiative effects of marine organic aerosols specifically for the western Pacific over East Asia. This study reveals an important role of marine organic aerosols in radiation and cloud and would be valuable for climate research at both regional and global scales.
Wei Hu, Kotaro Murata, Chunlan Fan, Shu Huang, Hiromi Matsusaki, Pingqing Fu, and Daizhou Zhang
Biogeosciences, 17, 4477–4487, https://doi.org/10.5194/bg-17-4477-2020, https://doi.org/10.5194/bg-17-4477-2020, 2020
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This paper reports the first estimate of the status of bacteria in long-distance-transported Asian dust, demonstrating that airborne dust, which can carry viable and nonviable bacteria on particle surfaces, is an efficient medium for constantly spreading bacteria at regional and even global scales. Such data are essential to better model and understand the roles and activities of bioaerosols in environmental evolution and climate change and the potential risks of bioaerosols to human health.
Wanyu Zhao, Hong Ren, Kimitaka Kawamura, Huiyun Du, Xueshun Chen, Siyao Yue, Qiaorong Xie, Lianfang Wei, Ping Li, Xin Zeng, Shaofei Kong, Yele Sun, Zifa Wang, and Pingqing Fu
Atmos. Chem. Phys., 20, 10331–10350, https://doi.org/10.5194/acp-20-10331-2020, https://doi.org/10.5194/acp-20-10331-2020, 2020
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Our observations provide detailed information on the abundance and vertical distribution of dicarboxylic acids, oxoacids and α-dicarbonyls in PM2.5 collected at three heights based on a 325 m meteorological tower in Beijing in summer. Our results demonstrate that organic acids at the ground surface are largely associated with local traffic emissions, while long-range atmospheric transport followed by photochemical ageing contributes more in the urban boundary layer than the ground surface.
Freya A. Squires, Eiko Nemitz, Ben Langford, Oliver Wild, Will S. Drysdale, W. Joe F. Acton, Pingqing Fu, C. Sue B. Grimmond, Jacqueline F. Hamilton, C. Nicholas Hewitt, Michael Hollaway, Simone Kotthaus, James Lee, Stefan Metzger, Natchaya Pingintha-Durden, Marvin Shaw, Adam R. Vaughan, Xinming Wang, Ruili Wu, Qiang Zhang, and Yanli Zhang
Atmos. Chem. Phys., 20, 8737–8761, https://doi.org/10.5194/acp-20-8737-2020, https://doi.org/10.5194/acp-20-8737-2020, 2020
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Significant air quality problems exist in megacities like Beijing, China. To manage air pollution, legislators need a clear understanding of pollutant emissions. However, emissions inventories have large uncertainties, and reliable field measurements of pollutant emissions are required to constrain them. This work presents the first measurements of traffic-dominated emissions in Beijing which suggest that inventories overestimate these emissions in the region during both winter and summer.
Weiqi Xu, Yao He, Yanmei Qiu, Chun Chen, Conghui Xie, Lu Lei, Zhijie Li, Jiaxing Sun, Junyao Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Meas. Tech., 13, 3205–3219, https://doi.org/10.5194/amt-13-3205-2020, https://doi.org/10.5194/amt-13-3205-2020, 2020
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We characterized mass spectral features of organic aerosol (OA) and water-soluble OA (WSOA) from 21 cooking, crop straw, wood, and coal burning experiments using aerosol mass spectrometers with standard and capture vaporizers, and we demonstrated the applications of source spectral profiles in improving source apportionment of ambient OA at a highly polluted rural site in the North China Plain in winter.
Jing Yang, Wanyu Zhao, Lianfang Wei, Qiang Zhang, Yue Zhao, Wei Hu, Libin Wu, Xiaodong Li, Chandra Mouli Pavuluri, Xiaole Pan, Yele Sun, Zifa Wang, Cong-Qiang Liu, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 20, 6841–6860, https://doi.org/10.5194/acp-20-6841-2020, https://doi.org/10.5194/acp-20-6841-2020, 2020
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Our observations provide novel detailed information on the atmospheric abundances and spatial distributions of dicarboxylic acids, oxoacids, and α-dicarbonyls in marine aerosols collected from the South China Sea to the East Indian Ocean. Our results demonstrate that the continental outflow of both biogenic and anthropogenic precursors followed by photochemical aging is one of the main sources and formation processes of marine organic aerosols over the tropical oceanic regions.
Qiaorong Xie, Sihui Su, Shuang Chen, Yisheng Xu, Dong Cao, Jing Chen, Lujie Ren, Siyao Yue, Wanyu Zhao, Yele Sun, Zifa Wang, Haijie Tong, Hang Su, Yafang Cheng, Kimitaka Kawamura, Guibin Jiang, Cong-Qiang Liu, and Pingqing Fu
Atmos. Chem. Phys., 20, 6803–6820, https://doi.org/10.5194/acp-20-6803-2020, https://doi.org/10.5194/acp-20-6803-2020, 2020
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Current knowledge on firework-related organic aerosols is very limited. Here the detailed molecular composition of organics in urban aerosols was characterized using ultrahigh-resolution FT-ICR mass spectrometry. Our findings highlight that firework emission leads to a sharp increase in CHO, CHNO, and CHOS containing high-molecular-weight species, particularly aromatic-like substances, which affect the physicochemical properties such as the light absorption and health effects of urban aerosols.
Shengzhen Zhou, Luolin Wu, Junchen Guo, Weihua Chen, Xuemei Wang, Jun Zhao, Yafang Cheng, Zuzhao Huang, Jinpu Zhang, Yele Sun, Pingqing Fu, Shiguo Jia, Jun Tao, Yanning Chen, and Junxia Kuang
Atmos. Chem. Phys., 20, 6435–6453, https://doi.org/10.5194/acp-20-6435-2020, https://doi.org/10.5194/acp-20-6435-2020, 2020
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In this work, measurements of size-segregated aerosols were conducted at three altitudes (ground level, 118 m, and 488 m) on the 610 m high Canton Tower in southern China. Vertical variations of PM and size-segregated chemical compositions were investigated. The results indicated that meteorological parameters and atmospheric aqueous and heterogeneous reactions together led to aerosol formation and haze episodes in the Pearl River Delta region during the measurement periods.
Hang Liu, Xiaole Pan, Dantong Liu, Xiaoyong Liu, Xueshun Chen, Yu Tian, Yele Sun, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 20, 5771–5785, https://doi.org/10.5194/acp-20-5771-2020, https://doi.org/10.5194/acp-20-5771-2020, 2020
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The bare black carbon (BC) was in a fractal structure. With coating thickness increasing, BC changed from a fractal structure to a core–shell structure. In the ambient atmosphere, plenty of BC particles were not in a perfect core–shell structure. This study brought attention to the combined effects of morphology and coating thickness on the absorption enhancement of BC-containing particles, which is helpful for determining the climatic effects of BC.
Aka Jacques Adon, Catherine Liousse, Elhadji Thierno Doumbia, Armelle Baeza-Squiban, Hélène Cachier, Jean-Francois Léon, Véronique Yoboué, Aristique Barthel Akpo, Corinne Galy-Lacaux, Benjamin Guinot, Cyril Zouiten, Hongmei Xu, Eric Gardrat, and Sekou Keita
Atmos. Chem. Phys., 20, 5327–5354, https://doi.org/10.5194/acp-20-5327-2020, https://doi.org/10.5194/acp-20-5327-2020, 2020
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It is our responsibility to establish a link between emissions, air pollution, and health impacts for urban combustion sources, typical of Africa.
Our results show that the particulate concentrations observed at all sites far exceed the recommendations of WHO. The site influenced by domestic fires is the most polluted site, dominated by a significant fraction of ultrafine particles. These studies will eventually lead to the implementation of emission reduction solutions to improve air quality.
Fanhao Meng, Min Qin, Ke Tang, Jun Duan, Wu Fang, Shuaixi Liang, Kaidi Ye, Pinhua Xie, Yele Sun, Conghui Xie, Chunxiang Ye, Pingqing Fu, Jianguo Liu, and Wenqing Liu
Atmos. Chem. Phys., 20, 5071–5092, https://doi.org/10.5194/acp-20-5071-2020, https://doi.org/10.5194/acp-20-5071-2020, 2020
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Nitrous acid (HONO), a major precursor of the OH radical, plays a key role in atmospheric chemistry, but its sources are still debated. The first high-resolution vertical measurements of HONO and NO2 were conducted in Beijing to investigate the nocturnal sources of HONO at different stages of pollution. The ground surface dominated HONO production by heterogeneous conversion of NO2 during clean episodes, but the aerosol production was an important nighttime HONO source during haze episodes.
Chenjie Yu, Dantong Liu, Kurtis Broda, Rutambhara Joshi, Jason Olfert, Yele Sun, Pingqing Fu, Hugh Coe, and James D. Allan
Atmos. Chem. Phys., 20, 3645–3661, https://doi.org/10.5194/acp-20-3645-2020, https://doi.org/10.5194/acp-20-3645-2020, 2020
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This study presents the first atmospheric application of a new morphology-independent measurement for the quantification of the mixing state of rBC-containing particles in urban Beijing as part of the UK–China APHH campaign. An inversion method has been applied for better quantification of rBC mixing state. The mass-resolved rBC mixing state information presented here has implications for detailed models of BC, its optical properties and its atmospheric life cycle.
Shaofeng Xu, Lujie Ren, Yunchao Lang, Shengjie Hou, Hong Ren, Lianfang Wei, Libin Wu, Junjun Deng, Wei Hu, Xiaole Pan, Yele Sun, Zifa Wang, Hang Su, Yafang Cheng, and Pingqing Fu
Atmos. Chem. Phys., 20, 3623–3644, https://doi.org/10.5194/acp-20-3623-2020, https://doi.org/10.5194/acp-20-3623-2020, 2020
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Current knowledge on the size distribution of biogenic primary organic aerosols in urban regions with heavy haze pollution is very limited. Here we performed a year-round study focusing on the organic molecular composition of size-segregated aerosol samples collected in urban Beijing during haze and non-haze days to elucidate the seasonal contributions of biomass burning, fungal spores, and plant debris to organic carbon as well as the influences from local emissions and long-range transport.
Leigh R. Crilley, Ajit Singh, Louisa J. Kramer, Marvin D. Shaw, Mohammed S. Alam, Joshua S. Apte, William J. Bloss, Lea Hildebrandt Ruiz, Pingqing Fu, Weiqi Fu, Shahzad Gani, Michael Gatari, Evgenia Ilyinskaya, Alastair C. Lewis, David Ng'ang'a, Yele Sun, Rachel C. W. Whitty, Siyao Yue, Stuart Young, and Francis D. Pope
Atmos. Meas. Tech., 13, 1181–1193, https://doi.org/10.5194/amt-13-1181-2020, https://doi.org/10.5194/amt-13-1181-2020, 2020
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There is considerable interest in using low-cost optical particle counters (OPCs) for particle mass measurements; however, there is no agreed upon method with respect to calibration. Here we exploit a number of datasets globally to demonstrate that particle composition and relative humidity are the key factors affecting measured concentrations from a low-cost OPC, and we present a simple correction methodology that corrects for this influence.
Lu Lei, Conghui Xie, Dawei Wang, Yao He, Qingqing Wang, Wei Zhou, Wei Hu, Pingqing Fu, Yong Chen, Xiaole Pan, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 20, 2877–2890, https://doi.org/10.5194/acp-20-2877-2020, https://doi.org/10.5194/acp-20-2877-2020, 2020
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We characterized aerosol composition and sources near two steel plants in a coastal region in fall and spring seasons. Our results showed substantially different aerosol composition and sources between the two seasons. We observed significant impacts of steel plant emissions on aerosol chemistry nearby, and we found that aerosol particles emitted from the steel plants were dominated by ammonium sulfate/bisulfate; NOx/CO and NOx/SO2 were distinct from those in the absence of industrial plumes.
Yanbing Fan, Cong-Qiang Liu, Linjie Li, Lujie Ren, Hong Ren, Zhimin Zhang, Qinkai Li, Shuang Wang, Wei Hu, Junjun Deng, Libin Wu, Shujun Zhong, Yue Zhao, Chandra Mouli Pavuluri, Xiaodong Li, Xiaole Pan, Yele Sun, Zifa Wang, Kimitaka Kawamura, Zongbo Shi, and Pingqing Fu
Atmos. Chem. Phys., 20, 117–137, https://doi.org/10.5194/acp-20-117-2020, https://doi.org/10.5194/acp-20-117-2020, 2020
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This study provides useful knowledge on the abundance, sources, and formation processes of organic aerosols in the coastal megacity of Tianjin, North China, based on the investigation of the molecular composition, diurnal variation, and winter/summer differences under the influence of land/sea breezes and the Asian summer monsoon.
Hang Liu, Xiaole Pan, Yu Wu, Dawei Wang, Yu Tian, Xiaoyong Liu, Lu Lei, Yele Sun, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 19, 14791–14804, https://doi.org/10.5194/acp-19-14791-2019, https://doi.org/10.5194/acp-19-14791-2019, 2019
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The relationship among the effective density, rBC's coating thickness, and rBC's morphology was investigated. rBC with larger effective density adopted a more regular shape due to more coating thickness. The effective density distribution of ambient rBC was also measured. From the information of effective density, the ambient rBC mainly adopts an irregular shape, which can cause large uncertainties in the rBC's optical properties.
Ruihe Lyu, Zongbo Shi, Mohammed Salim Alam, Xuefang Wu, Di Liu, Tuan V. Vu, Christopher Stark, Pingqing Fu, Yinchang Feng, and Roy M. Harrison
Atmos. Chem. Phys., 19, 10865–10881, https://doi.org/10.5194/acp-19-10865-2019, https://doi.org/10.5194/acp-19-10865-2019, 2019
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Severe pollution of the Beijing atmosphere is a frequent occurrence. The airborne particles which characterize the episodes of haze contain a wide range of chemical constituents but organic compounds make up a substantial proportion. In this study individual compounds are analysed under both haze and non-haze conditions, and the measurements are compared with samples collected in London, where the air pollution climate and sources are very different.
Weiqi Xu, Conghui Xie, Eleni Karnezi, Qi Zhang, Junfeng Wang, Spyros N. Pandis, Xinlei Ge, Jingwei Zhang, Junling An, Qingqing Wang, Jian Zhao, Wei Du, Yanmei Qiu, Wei Zhou, Yao He, Ying Li, Jie Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 19, 10205–10216, https://doi.org/10.5194/acp-19-10205-2019, https://doi.org/10.5194/acp-19-10205-2019, 2019
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We present the first aerosol volatility measurements in Beijing in summer using a thermodenuder coupled with aerosol mass spectrometers. Our results showed that organic aerosol (OA) comprised mainly semi-volatile organic compounds in summer, and the freshly oxidized secondary OA was the most volatile component. We also found quite different volatility distributions in black-carbon-containing primary and secondary OA, ambient OA, ambient secondary OA and the WRF-Chem model.
Huiyun Du, Jie Li, Xueshun Chen, Zifa Wang, Yele Sun, Pingqing Fu, Jianjun Li, Jian Gao, and Ying Wei
Atmos. Chem. Phys., 19, 9351–9370, https://doi.org/10.5194/acp-19-9351-2019, https://doi.org/10.5194/acp-19-9351-2019, 2019
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Regional transport and heterogeneous reactions play crucial roles in haze formation. Using a chemical transport model, we found that chemical transformation of SO2 along the transport pathway from source regions to Beijing was the major source of sulfate. Heterogeneous chemistry had a stronger effect under high humidity and high pollution levels. Aerosols underwent aging during transport which altered the aerosol size and the degree of aging.
Weijun Li, Lei Liu, Qi Yuan, Liang Xu, Yanhong Zhu, Bingbing Wang, Hua Yu, Xiaokun Ding, Jian Zhang, Dao Huang, Dantong Liu, Wei Hu, Daizhou Zhang, Pingqing Fu, Maosheng Yao, Min Hu, Xiaoye Zhang, and Zongbo Shi
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-539, https://doi.org/10.5194/acp-2019-539, 2019
Preprint withdrawn
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The real state of individual primary biological aerosol particles (PBAPs) derived from natural sources is under mystery, although many studies well evaluate the morphology, mixing state, and elemental composition of anthropogenic particles. It induces that some studies mislead some anthropogenic particles into biological particles through electron microscopy. Here we firstly estimate the full database of individual PBAPs through two microscopic instruments. The database is good for research.
Zongbo Shi, Tuan Vu, Simone Kotthaus, Roy M. Harrison, Sue Grimmond, Siyao Yue, Tong Zhu, James Lee, Yiqun Han, Matthias Demuzere, Rachel E. Dunmore, Lujie Ren, Di Liu, Yuanlin Wang, Oliver Wild, James Allan, W. Joe Acton, Janet Barlow, Benjamin Barratt, David Beddows, William J. Bloss, Giulia Calzolai, David Carruthers, David C. Carslaw, Queenie Chan, Lia Chatzidiakou, Yang Chen, Leigh Crilley, Hugh Coe, Tie Dai, Ruth Doherty, Fengkui Duan, Pingqing Fu, Baozhu Ge, Maofa Ge, Daobo Guan, Jacqueline F. Hamilton, Kebin He, Mathew Heal, Dwayne Heard, C. Nicholas Hewitt, Michael Hollaway, Min Hu, Dongsheng Ji, Xujiang Jiang, Rod Jones, Markus Kalberer, Frank J. Kelly, Louisa Kramer, Ben Langford, Chun Lin, Alastair C. Lewis, Jie Li, Weijun Li, Huan Liu, Junfeng Liu, Miranda Loh, Keding Lu, Franco Lucarelli, Graham Mann, Gordon McFiggans, Mark R. Miller, Graham Mills, Paul Monk, Eiko Nemitz, Fionna O'Connor, Bin Ouyang, Paul I. Palmer, Carl Percival, Olalekan Popoola, Claire Reeves, Andrew R. Rickard, Longyi Shao, Guangyu Shi, Dominick Spracklen, David Stevenson, Yele Sun, Zhiwei Sun, Shu Tao, Shengrui Tong, Qingqing Wang, Wenhua Wang, Xinming Wang, Xuejun Wang, Zifang Wang, Lianfang Wei, Lisa Whalley, Xuefang Wu, Zhijun Wu, Pinhua Xie, Fumo Yang, Qiang Zhang, Yanli Zhang, Yuanhang Zhang, and Mei Zheng
Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, https://doi.org/10.5194/acp-19-7519-2019, 2019
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APHH-Beijing is a collaborative international research programme to study the sources, processes and health effects of air pollution in Beijing. This introduction to the special issue provides an overview of (i) the APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it and (iii) the air quality and meteorological conditions during joint intensive field campaigns as a core activity within APHH-Beijing.
Dantong Liu, Rutambhara Joshi, Junfeng Wang, Chenjie Yu, James D. Allan, Hugh Coe, Michael J. Flynn, Conghui Xie, James Lee, Freya Squires, Simone Kotthaus, Sue Grimmond, Xinlei Ge, Yele Sun, and Pingqing Fu
Atmos. Chem. Phys., 19, 6749–6769, https://doi.org/10.5194/acp-19-6749-2019, https://doi.org/10.5194/acp-19-6749-2019, 2019
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This study provides source attribution and characterization of BC in the Beijing urban environment in both winter and summer. For the first time, the physically and chemically based source apportionments are compared to evaluate the primary source contribution and secondary processing of BC-containing particles. A method is proposed to isolate the BC from the transportation sector and coal combustion sources.
Hongmei Xu, Jean-François Léon, Cathy Liousse, Benjamin Guinot, Véronique Yoboué, Aristide Barthélémy Akpo, Jacques Adon, Kin Fai Ho, Steven Sai Hang Ho, Lijuan Li, Eric Gardrat, Zhenxing Shen, and Junji Cao
Atmos. Chem. Phys., 19, 6637–6657, https://doi.org/10.5194/acp-19-6637-2019, https://doi.org/10.5194/acp-19-6637-2019, 2019
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This paper discusses the personal exposure characteristics and health implication of PM2.5 and bounded chemical species based on three anthropogenic sources and related populations (domestic fires for women, waste burning for students and motorcycle traffic for drivers) in Abidjan and Cotonou in dry and wet seasons of 2016. This work can be regarded as the first attempt at measuring personal exposure to PM2.5 and its related health risks in underdeveloped countries of Africa.
Junfeng Wang, Dantong Liu, Xinlei Ge, Yangzhou Wu, Fuzhen Shen, Mindong Chen, Jian Zhao, Conghui Xie, Qingqing Wang, Weiqi Xu, Jie Zhang, Jianlin Hu, James Allan, Rutambhara Joshi, Pingqing Fu, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 19, 447–458, https://doi.org/10.5194/acp-19-447-2019, https://doi.org/10.5194/acp-19-447-2019, 2019
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This work is part of the UK-China APHH campaign. We used a laser-only Aerodyne soot particle aerosol mass spectrometer, for the first time, to investigate the concentrations, size distributions and chemical compositions for those ambient submicron aerosol particles only with black carbon as cores. Our findings are valuable to understand the BC properties and processes in the densely populated megacities.
Qiang Huang, Jiubin Chen, Weilin Huang, John R. Reinfelder, Pingqing Fu, Shengliu Yuan, Zhongwei Wang, Wei Yuan, Hongming Cai, Hong Ren, Yele Sun, and Li He
Atmos. Chem. Phys., 19, 315–325, https://doi.org/10.5194/acp-19-315-2019, https://doi.org/10.5194/acp-19-315-2019, 2019
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Although the specific reactions and mechanisms in fine aerosols could not be explicitly determined from this field study, our results provide isotopic evidence that local daily photochemical reduction of divalent Hg is of critical importance to the fate of PM2.5-Hg in urban atmospheres and that, in addition to variation in sources, photochemical reduction appears to be an important process that affects both the particle mass-specific abundance and isotopic composition of PM2.5-Hg.
Xiaole Pan, Baozhu Ge, Zhe Wang, Yu Tian, Hang Liu, Lianfang Wei, Siyao Yue, Itsushi Uno, Hiroshi Kobayashi, Tomoaki Nishizawa, Atsushi Shimizu, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 19, 219–232, https://doi.org/10.5194/acp-19-219-2019, https://doi.org/10.5194/acp-19-219-2019, 2019
Conghui Xie, Weiqi Xu, Junfeng Wang, Qingqing Wang, Dantong Liu, Guiqian Tang, Ping Chen, Wei Du, Jian Zhao, Yingjie Zhang, Wei Zhou, Tingting Han, Qingyun Bian, Jie Li, Pingqing Fu, Zifa Wang, Xinlei Ge, James Allan, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 19, 165–179, https://doi.org/10.5194/acp-19-165-2019, https://doi.org/10.5194/acp-19-165-2019, 2019
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We present the first simultaneous real-time online measurements of aerosol optical properties at ground level and at 260 m on a meteorological tower in urban Beijing in winter. The vertical similarities and differences in scattering and absorption coefficients were characterized. The increases in MAC of BC were mainly associated with the coating materials on rBC. Coal combustion was the dominant source contribution of brown carbon followed by biomass burning and SOA in winter in Beijing.
Yingjie Zhang, Wei Du, Yuying Wang, Qingqing Wang, Haofei Wang, Haitao Zheng, Fang Zhang, Hongrong Shi, Yuxuan Bian, Yongxiang Han, Pingqing Fu, Francesco Canonaco, André S. H. Prévôt, Tong Zhu, Pucai Wang, Zhanqing Li, and Yele Sun
Atmos. Chem. Phys., 18, 14637–14651, https://doi.org/10.5194/acp-18-14637-2018, https://doi.org/10.5194/acp-18-14637-2018, 2018
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We have a comprehensive characterization of aerosol chemistry and particle growth events at a downwind site of a highly polluted city in the North China Plain. Aerosol particles at the urban downwind site were highly aged and mainly from secondary formation. New particle growth events were also frequently observed on both clean and polluted days. While both sulfate and SOA played important roles in particle growth during clean periods, SOA was more important than sulfate during polluted events.
Lei Liu, Jian Zhang, Liang Xu, Qi Yuan, Dao Huang, Jianmin Chen, Zongbo Shi, Yele Sun, Pingqing Fu, Zifa Wang, Daizhou Zhang, and Weijun Li
Atmos. Chem. Phys., 18, 14681–14693, https://doi.org/10.5194/acp-18-14681-2018, https://doi.org/10.5194/acp-18-14681-2018, 2018
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Using transmission electron microscopy, we studied individual cloud droplet residual and interstitial particles collected in cloud events at Mt. Tai in the polluted North China region. We found that individual cloud droplets were an extremely complicated mixture containing abundant refractory soot (i.e., black carbon), fly ash, and metals. The complicated cloud droplets have not been reported in clean continental or marine air before.
Mingjie Kang, Pingqing Fu, Kimitaka Kawamura, Fan Yang, Hongliang Zhang, Zhengchen Zang, Hong Ren, Lujie Ren, Ye Zhao, Yele Sun, and Zifa Wang
Atmos. Chem. Phys., 18, 13947–13967, https://doi.org/10.5194/acp-18-13947-2018, https://doi.org/10.5194/acp-18-13947-2018, 2018
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Molecular characterization and spatial distribution of biogenic primary organic aerosol (POA) and secondary organic aerosol (SOA) in the marine atmosphere are not well known. Here, we analysed the organic molecular composition of marine aerosols collected during a marine cruise in the East China Sea during May–June 2014. Our results suggest that the Asian continent can be a natural emitter of biogenic POA and SOA, which can be transported to the downwind marine atmosphere.
Wei Zhou, Jian Zhao, Bin Ouyang, Archit Mehra, Weiqi Xu, Yuying Wang, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Qi Chen, Conghui Xie, Qingqing Wang, Junfeng Wang, Wei Du, Yingjie Zhang, Xinlei Ge, Penglin Ye, James D. Lee, Pingqing Fu, Zifa Wang, Douglas Worsnop, Roderic Jones, Carl J. Percival, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 18, 11581–11597, https://doi.org/10.5194/acp-18-11581-2018, https://doi.org/10.5194/acp-18-11581-2018, 2018
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We present measurements of gas-phase N2O5 and ClNO2 by ToF-CIMS during summer in urban Beijing as part of the APHH campaign. High reactivity of N2O5 indicative of active nocturnal chemistry was observed. The lifetime of N2O5 as a function of aerosol surface area and relative humidity was characterized, and N2O5 uptake coefficients were estimated. We also found that the N2O5 loss in this study is mainly attributed to its indirect loss via reactions of NO3 with VOCs and NO.
Yele Sun, Weiqi Xu, Qi Zhang, Qi Jiang, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Jie Li, John Jayne, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 18, 8469–8489, https://doi.org/10.5194/acp-18-8469-2018, https://doi.org/10.5194/acp-18-8469-2018, 2018
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We present a 2–year analysis of organic aerosol (OA) from highly time–resolved measurements by an aerosol chemical speciation monitor in the megacity of Beijing. The sources of OA were analyzed with the advanced factor analysis of a multilinear engine (ME-2). Our results showed very different seasonal patterns, relative humidity and temperature dependence, and sources regions among different OA factors. The sources and processes of OA factors, and their roles in haze pollution are elucidated.
Sekou Keita, Cathy Liousse, Véronique Yoboué, Pamela Dominutti, Benjamin Guinot, Eric-Michel Assamoi, Agnès Borbon, Sophie L. Haslett, Laetitia Bouvier, Aurélie Colomb, Hugh Coe, Aristide Akpo, Jacques Adon, Julien Bahino, Madina Doumbia, Julien Djossou, Corinne Galy-Lacaux, Eric Gardrat, Sylvain Gnamien, Jean F. Léon, Money Ossohou, E. Touré N'Datchoh, and Laurent Roblou
Atmos. Chem. Phys., 18, 7691–7708, https://doi.org/10.5194/acp-18-7691-2018, https://doi.org/10.5194/acp-18-7691-2018, 2018
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This study provides emission factor (EF) data for elemental and organic carbon, total particulate matter and 58 volatile organic compound species for combustion sources specific to Africa to establish emission inventories with less uncertainty. EFs obtained in this study are generally higher than those in the literature whose values are used in emissions inventories for Africa. This shows that particles and VOC emissions were sometimes underestimated and underlines this study's importance.
Di Liu, Matthias Vonwiller, Jun Li, Junwen Liu, Sönke Szidat, Yanlin Zhang, Chongguo Tian, Yinjun Chen, Zhineng Cheng, Guangcai Zhong, Pingqing Fu, and Gan Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-295, https://doi.org/10.5194/acp-2018-295, 2018
Revised manuscript not accepted
Wei Zhou, Qingqing Wang, Xiujuan Zhao, Weiqi Xu, Chen Chen, Wei Du, Jian Zhao, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 18, 3951–3968, https://doi.org/10.5194/acp-18-3951-2018, https://doi.org/10.5194/acp-18-3951-2018, 2018
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We present a 3-month analysis of submicron aerosols that were measured at 260 m on a meteorological tower in Beijing, China. The sources of organic aerosol (OA) were analyzed by using a multi-linear engine (ME-2). Our results showed significant changes in both primary and secondary OA composition from the non-heating season to the heating season. We also observed a considerable contribution (10–13%) of cooking OA at 260 m and very different OA composition between ground level and 260 m.
Wanyu Zhao, Kimitaka Kawamura, Siyao Yue, Lianfang Wei, Hong Ren, Yu Yan, Mingjie Kang, Linjie Li, Lujie Ren, Senchao Lai, Jie Li, Yele Sun, Zifa Wang, and Pingqing Fu
Atmos. Chem. Phys., 18, 2749–2767, https://doi.org/10.5194/acp-18-2749-2018, https://doi.org/10.5194/acp-18-2749-2018, 2018
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In this paper, we investigate the seasonal trends in concentrations and compound-specific stable carbon isotope ratios of low molecular weight dicarboxylic acids (C2–C12) and related compounds in fine aerosols (PM2.5) in Beijing. Our study demonstrates that, in addition to the production via photo-oxidation, high abundances of diacids and related compounds in Beijing are largely associated with anthropogenic primary emissions such as biomass burning, fossil fuel combustion and plastic burning.
Santosh Kumar Verma, Kimitaka Kawamura, Jing Chen, and Pingqing Fu
Atmos. Chem. Phys., 18, 81–101, https://doi.org/10.5194/acp-18-81-2018, https://doi.org/10.5194/acp-18-81-2018, 2018
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East Asia has experienced rapid economic development in the last several decades, of which activities emit bioaerosols. The atmospheric particles are transported to downwind regions in the Pacific. To understand the atmospheric transport of bioaerosols, we conducted long-term observations of sugar components over Chichijima Island from 2001 to 2013. We found that atmospheric circulations significantly affect the seasonal variation of bioaerosol distributions over the western North Pacific.
Wei Du, Jian Zhao, Yuying Wang, Yingjie Zhang, Qingqing Wang, Weiqi Xu, Chen Chen, Tingting Han, Fang Zhang, Zhanqing Li, Pingqing Fu, Jie Li, Zifa Wang, and Yele Sun
Atmos. Chem. Phys., 17, 6797–6811, https://doi.org/10.5194/acp-17-6797-2017, https://doi.org/10.5194/acp-17-6797-2017, 2017
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We conducted the first simultaneous measurements of size-resolved particle number concentrations at ground level and 260 m in urban Beijing. The vertical differences strongly depend on particle sizes, with accumulation-mode particles being highly correlated at the two heights. We further demonstrated that regional emission controls have a dominant impact on accumulation-mode particles, while the influences on Aitken particles were much smaller due to the enhanced NPF events.
Jian Zhao, Wei Du, Yingjie Zhang, Qingqing Wang, Chen Chen, Weiqi Xu, Tingting Han, Yuying Wang, Pingqing Fu, Zifa Wang, Zhanqing Li, and Yele Sun
Atmos. Chem. Phys., 17, 3215–3232, https://doi.org/10.5194/acp-17-3215-2017, https://doi.org/10.5194/acp-17-3215-2017, 2017
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We conducted aerosol particle composition measurements at ground level and 260 m with two aerosol mass spectrometers in Beijing during the 2015 China Victory Day parade. Our results showed a stronger impact of emission controls on inorganic aerosol than OA. A larger decrease in more oxidized SOA than the less oxidized one during the control period was also observed. Our results indicate that emission controls and the changes in meteorological conditions have affected SOA formation mechanisms.
Shurui Chen, Liang Xu, Yinxiao Zhang, Bing Chen, Xinfeng Wang, Xiaoye Zhang, Mei Zheng, Jianmin Chen, Wenxing Wang, Yele Sun, Pingqing Fu, Zifa Wang, and Weijun Li
Atmos. Chem. Phys., 17, 1259–1270, https://doi.org/10.5194/acp-17-1259-2017, https://doi.org/10.5194/acp-17-1259-2017, 2017
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Many studies have focused on the unusually severe hazes instead of the more frequent light and moderate hazes (22–63 %) in winter in the North China Plain (NCP). The morphology, mixing state, and size of organic aerosols in the L & M hazes were characterized. We conclude that the direct emissions from residential coal stoves without any pollution controls in rural and urban outskirts contribute large amounts of primary OM particles to the regional L & M hazes in winter in the NCP.
Hui Zhang, Xuewu Fu, Che-Jen Lin, Lihai Shang, Yiping Zhang, Xinbin Feng, and Cynthia Lin
Atmos. Chem. Phys., 16, 13131–13148, https://doi.org/10.5194/acp-16-13131-2016, https://doi.org/10.5194/acp-16-13131-2016, 2016
Xuewu Fu, Xu Yang, Xiaofang Lang, Jun Zhou, Hui Zhang, Ben Yu, Haiyu Yan, Che-Jen Lin, and Xinbin Feng
Atmos. Chem. Phys., 16, 11547–11562, https://doi.org/10.5194/acp-16-11547-2016, https://doi.org/10.5194/acp-16-11547-2016, 2016
Yele Sun, Wei Du, Pingqing Fu, Qingqing Wang, Jie Li, Xinlei Ge, Qi Zhang, Chunmao Zhu, Lujie Ren, Weiqi Xu, Jian Zhao, Tingting Han, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 16, 8309–8329, https://doi.org/10.5194/acp-16-8309-2016, https://doi.org/10.5194/acp-16-8309-2016, 2016
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We have a comprehensive characterization of the sources, variations and processes of submicron aerosols in Beijing in winter using HR-AMS and GC/MS measurements. The primary sources including traffic, cooking, biomass burning and coal combustion emissions, and secondary components were separated and quantified with PMF. Our results elucidated the important roles of primary emissions, particularly coal combustion, and aqueous-phase processing in the formation of severe air pollution in winter.
Yan-Lin Zhang, Kimitaka Kawamura, Ping Qing Fu, Suresh K. R. Boreddy, Tomomi Watanabe, Shiro Hatakeyama, Akinori Takami, and Wei Wang
Atmos. Chem. Phys., 16, 6407–6419, https://doi.org/10.5194/acp-16-6407-2016, https://doi.org/10.5194/acp-16-6407-2016, 2016
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Here, based on three aircraft measurements over East Asia, we demonstrate an aqueous-phase mechanism for enhanced SOA production in the troposphere following correlation analysis of oxalic acid in tropospheric aerosols with other measured chemical variables including its precursors and its intermediate as well as biogenic-derived SOA from isoprene, monoterpenes and β-caryophyllene.
Jonas Sommar, Wei Zhu, Lihai Shang, Che-Jen Lin, and Xinbin Feng
Biogeosciences, 13, 2029–2049, https://doi.org/10.5194/bg-13-2029-2016, https://doi.org/10.5194/bg-13-2029-2016, 2016
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A micrometeorological method (REA) has been implemented to assess the role of cereal crop fields in the North China Plain as a source or sink of elemental mercury vapor (Hg0) during the course of a full year. In combination with chamber measurements under the canopy, the above-canopy REA measurements provided evidence for a balance between Hg0 ground emissions and uptake of Hg0 by the crop foliage, with net emissions prevailing from the ecosystem during the majority of a year.
S. Kundu, K. Kawamura, M. Kobayashi, E. Tachibana, M. Lee, P. Q. Fu, and J. Jung
Atmos. Chem. Phys., 16, 585–596, https://doi.org/10.5194/acp-16-585-2016, https://doi.org/10.5194/acp-16-585-2016, 2016
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Chemistry-transport models have predicted a change in secondary organic aerosols (SOA) in the future atmosphere with a large uncertainty. This study measures diacids, major water-soluble surrogates of SOA, on a sub-decadal scale in atmospheric aerosols in eastern Asia. Diacids are observed to increase by 3.9–47.4 % per year. The increases in the water-soluble organic acid fraction could modify the aerosol organic composition and its sensitivity to climate-relevant physical properties.
W. Q. Xu, Y. L. Sun, C. Chen, W. Du, T. T. Han, Q. Q. Wang, P. Q. Fu, Z. F. Wang, X. J. Zhao, L. B. Zhou, D. S. Ji, P. C. Wang, and D. R. Worsnop
Atmos. Chem. Phys., 15, 13681–13698, https://doi.org/10.5194/acp-15-13681-2015, https://doi.org/10.5194/acp-15-13681-2015, 2015
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We have investigated the response of aerosol composition, size distributions, and oxidation properties to emission controls during the 2014 Asia- Pacific Economic Cooperation (APEC) summit in Beijing. Our results showed substantial changes of aerosol bulk composition during APEC with the most reductions in secondary aerosols in large accumulation modes, demonstrating that that emission controls over regional scales can substantially reduce secondary particulates.
C. Chen, Y. L. Sun, W. Q. Xu, W. Du, L. B. Zhou, T. T. Han, Q. Q. Wang, P. Q. Fu, Z. F. Wang, Z. Q. Gao, Q. Zhang, and D. R. Worsnop
Atmos. Chem. Phys., 15, 12879–12895, https://doi.org/10.5194/acp-15-12879-2015, https://doi.org/10.5194/acp-15-12879-2015, 2015
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A comprehensive characterization of submicron aerosol composition and sources at 260m in urban Beijing during APEC 2014 is presented. Aerosol species were shown to decrease substantially by 40–80% during APEC, whereas the bulk composition was relatively similar to the result of synergetic controls of secondary precursors. Our results elucidated that the good air quality during APEC was the combined result of emission controls and meteorological effects, with the former playing the dominant role.
Y. L. Sun, Z. F. Wang, W. Du, Q. Zhang, Q. Q. Wang, P. Q. Fu, X. L. Pan, J. Li, J. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 10149–10165, https://doi.org/10.5194/acp-15-10149-2015, https://doi.org/10.5194/acp-15-10149-2015, 2015
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We conducted the first long-term real-time measurement of submicron aerosol composition in Beijing using an ACSM for 1 year. The seasonal variations of mass concentrations and chemical composition of submicron aerosol were investigated in detail, and the meteorological effects on aerosol chemistry, particularly temperature and relative humidity, were elucidated. Finally, the potential source areas of aerosol species during four seasons were identified.
C. M. Pavuluri, K. Kawamura, and P. Q. Fu
Atmos. Chem. Phys., 15, 9883–9896, https://doi.org/10.5194/acp-15-9883-2015, https://doi.org/10.5194/acp-15-9883-2015, 2015
Z. Cong, S. Kang, K. Kawamura, B. Liu, X. Wan, Z. Wang, S. Gao, and P. Fu
Atmos. Chem. Phys., 15, 1573–1584, https://doi.org/10.5194/acp-15-1573-2015, https://doi.org/10.5194/acp-15-1573-2015, 2015
P. Q. Fu, K. Kawamura, Y. F. Cheng, S. Hatakeyama, A. Takami, H. Li, and W. Wang
Atmos. Chem. Phys., 14, 4185–4199, https://doi.org/10.5194/acp-14-4185-2014, https://doi.org/10.5194/acp-14-4185-2014, 2014
Y. Kanaya, H. Akimoto, Z.-F. Wang, P. Pochanart, K. Kawamura, Y. Liu, J. Li, Y. Komazaki, H. Irie, X.-L. Pan, F. Taketani, K. Yamaji, H. Tanimoto, S. Inomata, S. Kato, J. Suthawaree, K. Okuzawa, G. Wang, S. G. Aggarwal, P. Q. Fu, T. Wang, J. Gao, Y. Wang, and G. Zhuang
Atmos. Chem. Phys., 13, 8265–8283, https://doi.org/10.5194/acp-13-8265-2013, https://doi.org/10.5194/acp-13-8265-2013, 2013
Y. L. Sun, Z. F. Wang, P. Q. Fu, T. Yang, Q. Jiang, H. B. Dong, J. Li, and J. J. Jia
Atmos. Chem. Phys., 13, 4577–4592, https://doi.org/10.5194/acp-13-4577-2013, https://doi.org/10.5194/acp-13-4577-2013, 2013
C. M. Pavuluri, K. Kawamura, N. Mihalopoulos, and P. Fu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-6589-2013, https://doi.org/10.5194/acpd-13-6589-2013, 2013
Revised manuscript not accepted
P. Q. Fu, K. Kawamura, J. Chen, B. Charrière, and R. Sempéré
Biogeosciences, 10, 653–667, https://doi.org/10.5194/bg-10-653-2013, https://doi.org/10.5194/bg-10-653-2013, 2013
G. H. Wang, B. H. Zhou, C. L. Cheng, J. J. Cao, J. J. Li, J. J. Meng, J. Tao, R. J. Zhang, and P. Q. Fu
Atmos. Chem. Phys., 13, 819–835, https://doi.org/10.5194/acp-13-819-2013, https://doi.org/10.5194/acp-13-819-2013, 2013
Related subject area
Subject: Isotopes | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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An improved estimate for the δ13C and δ18O signatures of carbon monoxide produced from atmospheric oxidation of volatile organic compounds
Seasonality in the Δ33S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO2
The Δ17O and δ18O values of atmospheric nitrates simultaneously collected downwind of anthropogenic sources – implications for polluted air masses
A very limited role of tropospheric chlorine as a sink of the greenhouse gas methane
Detection and variability of combustion-derived vapor in an urban basin
Stable sulfur isotope measurements to trace the fate of SO2 in the Athabasca oil sands region
Triple oxygen isotopes indicate urbanization affects sources of nitrate in wet and dry atmospheric deposition
Isotopic constraints on heterogeneous sulfate production in Beijing haze
Estimation of the fossil fuel component in atmospheric CO2 based on radiocarbon measurements at the Beromünster tall tower, Switzerland
Constraining N2O emissions since 1940 using firn air isotope measurements in both hemispheres
Seasonal variations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica
Carbon isotopic signature of coal-derived methane emissions to the atmosphere: from coalification to alteration
Isotopic constraints on the role of hypohalous acids in sulfate aerosol formation in the remote marine boundary layer
In situ observations of the isotopic composition of methane at the Cabauw tall tower site
Oxygen isotope mass balance of atmospheric nitrate at Dome C, East Antarctica, during the OPALE campaign
Isotopic effects of nitrate photochemistry in snow: a field study at Dome C, Antarctica
Stable carbon isotope ratios of ambient secondary organic aerosols in Toronto
WAIS Divide ice core suggests sustained changes in the atmospheric formation pathways of sulfate and nitrate since the 19th century in the extratropical Southern Hemisphere
Stable carbon isotope ratios of toluene in the boundary layer and the lower free troposphere
Emission ratio and isotopic signatures of molecular hydrogen emissions from tropical biomass burning
Can the carbon isotopic composition of methane be reconstructed from multi-site firn air measurements?
Air–snow transfer of nitrate on the East Antarctic Plateau – Part 1: Isotopic evidence for a photolytically driven dynamic equilibrium in summer
Chemical characterization and stable carbon isotopic composition of particulate Polycyclic Aromatic Hydrocarbons issued from combustion of 10 Mediterranean woods
Quantification of the carbonaceous matter origin in submicron marine aerosol by 13C and 14C isotope analysis
Temporal and spatial variability of the stable isotopic composition of atmospheric molecular hydrogen: observations at six EUROHYDROS stations
Continuous isotopic composition measurements of tropospheric CO2 at Jungfraujoch (3580 m a.s.l.), Switzerland: real-time observation of regional pollution events
Anthropogenic imprints on nitrogen and oxygen isotopic composition of precipitation nitrate in a nitrogen-polluted city in southern China
Analysis of 13C and 18O isotope data of CO2 in CARIBIC aircraft samples as tracers of upper troposphere/lower stratosphere mixing and the global carbon cycle
Tracing the fate of atmospheric nitrate deposited onto a forest ecosystem in Eastern Asia using Δ17O
Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling
Sources and transport of Δ14C in CO2 within the Mexico City Basin and vicinity
Jessica M. Burger, Emily Joyce, Meredith G. Hastings, Kurt A. M. Spence, and Katye E. Altieri
Atmos. Chem. Phys., 23, 5605–5622, https://doi.org/10.5194/acp-23-5605-2023, https://doi.org/10.5194/acp-23-5605-2023, 2023
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A seasonal analysis of the nitrogen isotopes of atmospheric nitrate over the remote Southern Ocean reveals that similar natural NOx sources dominate in spring and summer, while winter is representative of background-level conditions. The oxygen isotopes suggest that similar oxidation pathways involving more ozone occur in spring and winter, while the hydroxyl radical is the main oxidant in summer. This work helps to constrain NOx cycling and oxidant budgets in a data-sparse remote marine region.
Claire Bekker, Wendell W. Walters, Lee T. Murray, and Meredith G. Hastings
Atmos. Chem. Phys., 23, 4185–4201, https://doi.org/10.5194/acp-23-4185-2023, https://doi.org/10.5194/acp-23-4185-2023, 2023
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Nitrate is a critical component of the atmosphere that degrades air quality and ecosystem health. We have investigated the nitrogen isotope compositions of nitrate from deposition samples collected across the northeastern United States. Spatiotemporal variability in the nitrogen isotope compositions was found to track with nitrate formation chemistry. Our results highlight that nitrogen isotope compositions may be a robust tool for improving model representation of nitrate chemistry.
Heejeong Kim, Wendell W. Walters, Claire Bekker, Lee T. Murray, and Meredith G. Hastings
Atmos. Chem. Phys., 23, 4203–4219, https://doi.org/10.5194/acp-23-4203-2023, https://doi.org/10.5194/acp-23-4203-2023, 2023
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Atmospheric nitrate has an important impact on human and ecosystem health. We evaluated atmospheric nitrate formation pathways in the northeastern US utilizing oxygen isotope compositions, which indicated a significant difference between the phases of nitrate (i.e., gas vs. particle). Comparing the observations with model simulations indicated that N2O5 hydrolysis chemistry was overpredicted. Our study has important implications for improving atmospheric chemistry model representation.
Pete D. Akers, Joël Savarino, Nicolas Caillon, Olivier Magand, and Emmanuel Le Meur
Atmos. Chem. Phys., 22, 15637–15657, https://doi.org/10.5194/acp-22-15637-2022, https://doi.org/10.5194/acp-22-15637-2022, 2022
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Nitrate isotopes in Antarctic ice do not preserve the seasonal isotopic cycles of the atmosphere, which limits their use to study the past. We studied nitrate along an 850 km Antarctic transect to learn how these cycles are changed by sunlight-driven chemistry in the snow. Our findings suggest that the snow accumulation rate and other environmental signals can be extracted from nitrate with the right sampling and analytical approaches.
Bryce F. J. Kelly, Xinyi Lu, Stephen J. Harris, Bruno G. Neininger, Jorg M. Hacker, Stefan Schwietzke, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Carina van der Veen, Malika Menoud, and Thomas Röckmann
Atmos. Chem. Phys., 22, 15527–15558, https://doi.org/10.5194/acp-22-15527-2022, https://doi.org/10.5194/acp-22-15527-2022, 2022
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This study explores using the composition of methane of in-flight atmospheric air samples for greenhouse gas inventory verification. The air samples were collected above one of the largest coal seam gas production regions in the world. Adjacent to these gas fields are coal mines, Australia's largest cattle feedlot, and over 1 million grazing cattle. The results are also used to identify methane mitigation opportunities.
Malika Menoud, Carina van der Veen, Jaroslaw Necki, Jakub Bartyzel, Barbara Szénási, Mila Stanisavljević, Isabelle Pison, Philippe Bousquet, and Thomas Röckmann
Atmos. Chem. Phys., 21, 13167–13185, https://doi.org/10.5194/acp-21-13167-2021, https://doi.org/10.5194/acp-21-13167-2021, 2021
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Using measurements of methane isotopes in ambient air and a 3D atmospheric transport model, in Krakow, Poland, we mainly detected fossil-fuel-related sources, coming from coal mining in Silesia and from the use of natural gas in the city. Emission inventories report large emissions from coal mine activity in Silesia, which is in agreement with our measurements. However, methane sources in the urban area of Krakow related to the use of fossil fuels might be underestimated in the inventories.
Xinyi Lu, Stephen J. Harris, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Thomas Röckmann, Carina van der Veen, Malika Menoud, Stefan Schwietzke, and Bryce F. J. Kelly
Atmos. Chem. Phys., 21, 10527–10555, https://doi.org/10.5194/acp-21-10527-2021, https://doi.org/10.5194/acp-21-10527-2021, 2021
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Many coal seam gas (CSG) facilities in the Surat Basin, Australia, are adjacent to other sources of methane, including agricultural, urban, and natural seeps. This makes it challenging to estimate the amount of methane being emitted into the atmosphere from CSG facilities. This research demonstrates that measurements of the carbon and hydrogen stable isotopic composition of methane can distinguish between and apportion methane emissions from CSG facilities, cattle, and many other sources.
Sarah Albertin, Joël Savarino, Slimane Bekki, Albane Barbero, and Nicolas Caillon
Atmos. Chem. Phys., 21, 10477–10497, https://doi.org/10.5194/acp-21-10477-2021, https://doi.org/10.5194/acp-21-10477-2021, 2021
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We report an efficient method to collect atmospheric NO2 adapted for multi-isotopic analysis and present the first NO2 triple oxygen and double nitrogen isotope measurements. Atmospheric samplings carried out in Grenoble, France, highlight the NO2 isotopic signature sensitivity to the local NOx emissions and chemical regimes. These preliminary results are very promising for using the combination of Δ17O and δ15N of NO2 as a probe of the atmospheric NOx emissions and chemistry.
Ana Moreno, Miguel Iglesias, Cesar Azorin-Molina, Carlos Pérez-Mejías, Miguel Bartolomé, Carlos Sancho, Heather Stoll, Isabel Cacho, Jaime Frigola, Cinta Osácar, Arsenio Muñoz, Antonio Delgado-Huertas, Ileana Bladé, and Françoise Vimeux
Atmos. Chem. Phys., 21, 10159–10177, https://doi.org/10.5194/acp-21-10159-2021, https://doi.org/10.5194/acp-21-10159-2021, 2021
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We present a large and unique dataset of the rainfall isotopic composition at seven sites from northern Iberia to characterize their variability at daily and monthly timescales and to assess the role of climate and geographic factors in the modulation of δ18O values. We found that the origin, moisture uptake along the trajectory and type of precipitation play a key role. These results will help to improve the interpretation of δ18O paleorecords from lacustrine carbonates or speleothems.
Kun Wang, Shohei Hattori, Mang Lin, Sakiko Ishino, Becky Alexander, Kazuki Kamezaki, Naohiro Yoshida, and Shichang Kang
Atmos. Chem. Phys., 21, 8357–8376, https://doi.org/10.5194/acp-21-8357-2021, https://doi.org/10.5194/acp-21-8357-2021, 2021
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Sulfate aerosols play an important climatic role and exert adverse effects on the ecological environment and human health. In this study, we present the triple oxygen isotopic composition of sulfate from the Mt. Everest region, southern Tibetan Plateau, and decipher the formation mechanisms of atmospheric sulfate in this pristine environment. The results indicate the important role of the S(IV) + O3 pathway in atmospheric sulfate formation promoted by conditions of high cloud water pH.
Pete D. Akers, Ben G. Kopec, Kyle S. Mattingly, Eric S. Klein, Douglas Causey, and Jeffrey M. Welker
Atmos. Chem. Phys., 20, 13929–13955, https://doi.org/10.5194/acp-20-13929-2020, https://doi.org/10.5194/acp-20-13929-2020, 2020
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Water vapor isotopes recorded for 2 years in coastal northern Greenland largely reflect changes in sea ice cover, with distinct values when Baffin Bay is ice covered in winter vs. open in summer. Resulting changes in moisture transport, surface winds, and air temperature also modify the isotopes. Local glacial ice may thus preserve past changes in the Baffin Bay sea ice extent, and this will help us better understand how the Arctic environment and water cycle responds to global climate change.
Ben Yu, Lin Yang, Linlin Wang, Hongwei Liu, Cailing Xiao, Yong Liang, Qian Liu, Yongguang Yin, Ligang Hu, Jianbo Shi, and Guibin Jiang
Atmos. Chem. Phys., 20, 9713–9723, https://doi.org/10.5194/acp-20-9713-2020, https://doi.org/10.5194/acp-20-9713-2020, 2020
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We found that Br atoms in the marine boundary layer are the most probable oxidizer that transform gaseous elemental mercury into gaseous oxidized mercury, according to the mercury isotopes in the total gaseous mercury. On the other hand, Br or Cl atoms are not the primary oxidizers that produced oxidized mercury on particles. This study showed that mercury isotopes can provide new evidence that help us to fully understand the transformations of atmospheric mercury.
Longfei Yu, Eliza Harris, Stephan Henne, Sarah Eggleston, Martin Steinbacher, Lukas Emmenegger, Christoph Zellweger, and Joachim Mohn
Atmos. Chem. Phys., 20, 6495–6519, https://doi.org/10.5194/acp-20-6495-2020, https://doi.org/10.5194/acp-20-6495-2020, 2020
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We observed the isotopic composition of nitrous oxide in the unpolluted air at Jungfraujoch for 5 years. Our results indicate a clear seasonal pattern in the isotopic composition, corresponding with that in atmospheric nitrous oxide levels. This is most likely due to temporal variations in both emission processes and air mass sources for Jungfraujoch. Our findings are of importance to global nitrous oxide modelling and to better understanding of long-term trends in atmospheric nitrous oxide.
V. Holly L. Winton, Alison Ming, Nicolas Caillon, Lisa Hauge, Anna E. Jones, Joel Savarino, Xin Yang, and Markus M. Frey
Atmos. Chem. Phys., 20, 5861–5885, https://doi.org/10.5194/acp-20-5861-2020, https://doi.org/10.5194/acp-20-5861-2020, 2020
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The transfer of the nitrogen stable isotopic composition in nitrate between the air and snow at low accumulation sites in Antarctica leaves an UV imprint in the snow. Quantifying how nitrate isotope values change allows us to interpret longer ice core records. Based on nitrate observations and modelling at Kohnen, East Antarctica, the dominant factors controlling the nitrate isotope signature in deep snow layers are the depth of light penetration into the snowpack and the snow accumulation rate.
Isabelle Genot, David Au Yang, Erwan Martin, Pierre Cartigny, Erwann Legendre, and Marc De Rafelis
Atmos. Chem. Phys., 20, 4255–4273, https://doi.org/10.5194/acp-20-4255-2020, https://doi.org/10.5194/acp-20-4255-2020, 2020
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Given their critical impact on radiative forcing, sulfate aerosols have been extensively studied using their isotope signatures (δ34S, ∆33S, ∆36S, δ18O, and ∆17O). A striking observation is that ∆33S > 0 ‰, implying a missing reservoir in the sulfur cycle. Here, we measured ∆33S < 0 ‰ in black crust sulfates (i.e., formed on carbonate walls) that must therefore result from distinct chemical pathway(s) compared to sulfate aerosols, and they may well represent this complementary reservoir.
Angelina Wenger, Katherine Pugsley, Simon O'Doherty, Matt Rigby, Alistair J. Manning, Mark F. Lunt, and Emily D. White
Atmos. Chem. Phys., 19, 14057–14070, https://doi.org/10.5194/acp-19-14057-2019, https://doi.org/10.5194/acp-19-14057-2019, 2019
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We present 14CO2 observations at a background site in Ireland and a tall tower site in the UK. These data have been used to calculate the contribution of fossil fuel sources to atmospheric CO2 mole fractions from the UK and Ireland. 14CO2 emissions from nuclear industry sites in the UK cause a higher uncertainty in the results compared to observations in other locations. The observed ffCO2 at the site was not significantly different from simulated values based on the bottom-up inventory.
Isaac J. Vimont, Jocelyn C. Turnbull, Vasilii V. Petrenko, Philip F. Place, Colm Sweeney, Natasha Miles, Scott Richardson, Bruce H. Vaughn, and James W. C. White
Atmos. Chem. Phys., 19, 8547–8562, https://doi.org/10.5194/acp-19-8547-2019, https://doi.org/10.5194/acp-19-8547-2019, 2019
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Stable isotopes of Carbon Monoxide (CO) and radiocarbon carbon dioxide were measured over three summers at Indianapolis, Indiana, US, and for 1 year at a site thought to be strongly influenced by CO from oxidized volatile organic compounds (VOCs) in South Carolina, US. The Indianapolis results were used to provide an estimate of the carbon and oxygen isotopic signatures of CO produced from oxidized VOCs. This updated estimate agrees well with the data from South Carolina during the summer.
David Au Yang, Pierre Cartigny, Karine Desboeufs, and David Widory
Atmos. Chem. Phys., 19, 3779–3796, https://doi.org/10.5194/acp-19-3779-2019, https://doi.org/10.5194/acp-19-3779-2019, 2019
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Sulfates present in urban aerosols collected worldwide usually exhibit 33S-anomalies whose origin remains unclear. Besides, the sulfate concentration is not very well modelled nowadays, which, coupled with the isotopic composition anomaly on the 33S, would highlight the presence of at least an additional oxidation pathway, different from O2+TMI, O3, OH, H2O2 and NO2. We suggest here the implication of two other possible oxidation pathways.
Martine M. Savard, Amanda S. Cole, Robert Vet, and Anna Smirnoff
Atmos. Chem. Phys., 18, 10373–10389, https://doi.org/10.5194/acp-18-10373-2018, https://doi.org/10.5194/acp-18-10373-2018, 2018
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Improving air quality requires understanding of the atmospheric processes transforming nitrous oxides emitted by human activities into nitrates, an N form that may degrade natural ecosystems. Isotopes (∆17O, δ18O) are characterized in separate wet, particulate and gaseous nitrates for the first time. The gas ranges are distinct from those of the other nitrates, and the plume dynamics emerge as crucial in interpreting the results, which unravel key processes behind the distribution of nitrates.
Sergey Gromov, Carl A. M. Brenninkmeijer, and Patrick Jöckel
Atmos. Chem. Phys., 18, 9831–9843, https://doi.org/10.5194/acp-18-9831-2018, https://doi.org/10.5194/acp-18-9831-2018, 2018
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Using the observational data on 13C (CO) and 13C (CH4) from the extra-tropical Southern Hemisphere (ETSH) and EMAC model we (1) provide an independent, observation-based evaluation of Cl atom concentration variations in the ETSH throughout 1994–2000, (2) show that the role of tropospheric Cl as a sink of CH4 is seriously overestimated in the literature, (3) demonstrate that the 13C/12C ratio of CO is a sensitive indicator for the isotopic composition of reacted CH4 and therefore for its sources.
Richard P. Fiorella, Ryan Bares, John C. Lin, James R. Ehleringer, and Gabriel J. Bowen
Atmos. Chem. Phys., 18, 8529–8547, https://doi.org/10.5194/acp-18-8529-2018, https://doi.org/10.5194/acp-18-8529-2018, 2018
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Fossil fuel combustion produces water; where fossil fuel combustion is concentrated in urban areas, this humidity source may represent ~ 10 % of total humidity. In turn, this water vapor addition may alter urban meteorology, though the contribution of combustion vapor is difficult to measure. Using stable water isotopes, we estimate that up to 16 % of urban humidity may arise from combustion when the atmosphere is stable during winter, and develop recommendations for application in other cities.
Neda Amiri, Roya Ghahreman, Ofelia Rempillo, Travis W. Tokarek, Charles A. Odame-Ankrah, Hans D. Osthoff, and Ann-Lise Norman
Atmos. Chem. Phys., 18, 7757–7780, https://doi.org/10.5194/acp-18-7757-2018, https://doi.org/10.5194/acp-18-7757-2018, 2018
David M. Nelson, Urumu Tsunogai, Dong Ding, Takuya Ohyama, Daisuke D. Komatsu, Fumiko Nakagawa, Izumi Noguchi, and Takashi Yamaguchi
Atmos. Chem. Phys., 18, 6381–6392, https://doi.org/10.5194/acp-18-6381-2018, https://doi.org/10.5194/acp-18-6381-2018, 2018
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Atmospheric nitrate may be produced locally and/or come from upwind regions. To address this issue we measured oxygen and nitrogen isotopes of wet and dry nitrate deposition at nearby urban and rural sites. Our results suggest that, relative to nitrate in wet deposition in urban environments and wet and dry deposition in rural environments, nitrate in dry deposition in urban environments results from local NOx emissions more so than wet deposition, which is transported longer distances.
Pengzhen He, Becky Alexander, Lei Geng, Xiyuan Chi, Shidong Fan, Haicong Zhan, Hui Kang, Guangjie Zheng, Yafang Cheng, Hang Su, Cheng Liu, and Zhouqing Xie
Atmos. Chem. Phys., 18, 5515–5528, https://doi.org/10.5194/acp-18-5515-2018, https://doi.org/10.5194/acp-18-5515-2018, 2018
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We use observations of the oxygen isotopic composition of sulfate aerosol as a fingerprint to quantify various sulfate formation mechanisms during pollution events in Beijing, China. We found that heterogeneous reactions on aerosols dominated sulfate production in general; however, in-cloud reactions would dominate haze sulfate production when cloud liquid water content was high. The findings also suggest the heterogeneity of aerosol acidity should be parameterized in models.
Tesfaye A. Berhanu, Sönke Szidat, Dominik Brunner, Ece Satar, Rüdiger Schanda, Peter Nyfeler, Michael Battaglia, Martin Steinbacher, Samuel Hammer, and Markus Leuenberger
Atmos. Chem. Phys., 17, 10753–10766, https://doi.org/10.5194/acp-17-10753-2017, https://doi.org/10.5194/acp-17-10753-2017, 2017
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Fossil fuel CO2 is the major contributor of anthropogenic CO2 in the atmosphere, and accurate quantification is essential to better understand the carbon cycle. Such accurate quantification can be conducted based on radiocarbon measurements. In this study, we present radiocarbon measurements from a tall tower site in Switzerland. From these measurements, we have observed seasonally varying fossil fuel CO2 contributions and a biospheric CO2 component that varies diurnally and seasonally.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Atmos. Chem. Phys., 17, 4539–4564, https://doi.org/10.5194/acp-17-4539-2017, https://doi.org/10.5194/acp-17-4539-2017, 2017
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Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
Sakiko Ishino, Shohei Hattori, Joel Savarino, Bruno Jourdain, Susanne Preunkert, Michel Legrand, Nicolas Caillon, Albane Barbero, Kota Kuribayashi, and Naohiro Yoshida
Atmos. Chem. Phys., 17, 3713–3727, https://doi.org/10.5194/acp-17-3713-2017, https://doi.org/10.5194/acp-17-3713-2017, 2017
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We show the first simultaneous observations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica. The contrasting seasonal trends between oxygen isotopes of ozone and those of sulfate and nitrate indicate that these signatures in sulfate and nitrate are mainly controlled by changes in oxidation chemistry. We also discuss the specific oxidation chemistry induced by the unique phenomena at the site.
Giulia Zazzeri, Dave Lowry, Rebecca E. Fisher, James L. France, Mathias Lanoisellé, Bryce F. J. Kelly, Jaroslaw M. Necki, Charlotte P. Iverach, Elisa Ginty, Miroslaw Zimnoch, Alina Jasek, and Euan G. Nisbet
Atmos. Chem. Phys., 16, 13669–13680, https://doi.org/10.5194/acp-16-13669-2016, https://doi.org/10.5194/acp-16-13669-2016, 2016
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Methane emissions estimates from the coal sector are highly uncertain. Precise δ13C isotopic signatures of methane sources can be used in atmospheric models for a methane budget assessment. Emissions from both underground and opencast coal mines in the UK, Australia and Poland were sampled and isotopically characterised using high-precision measurements of δ13C values. Representative isotopic signatures were provided, taking into account specific ranks of coal and mine type.
Qianjie Chen, Lei Geng, Johan A. Schmidt, Zhouqing Xie, Hui Kang, Jordi Dachs, Jihong Cole-Dai, Andrew J. Schauer, Madeline G. Camp, and Becky Alexander
Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, https://doi.org/10.5194/acp-16-11433-2016, 2016
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The formation mechanisms of sulfate in the marine boundary layer are not well understood, which could result in large uncertainties in aerosol radiative forcing. We measure the oxygen isotopic composition (Δ17O) of sulfate collected in the MBL and analyze with a global transport model. Our results suggest that 33–50 % of MBL sulfate is formed via oxidation of S(IV) by hypohalous acids HOBr / HOCl in the aqueous phase, and the daily-mean HOBr/HOCl concentrations are on the order of 0.01–0.1 ppt.
Thomas Röckmann, Simon Eyer, Carina van der Veen, Maria E. Popa, Béla Tuzson, Guillaume Monteil, Sander Houweling, Eliza Harris, Dominik Brunner, Hubertus Fischer, Giulia Zazzeri, David Lowry, Euan G. Nisbet, Willi A. Brand, Jaroslav M. Necki, Lukas Emmenegger, and Joachim Mohn
Atmos. Chem. Phys., 16, 10469–10487, https://doi.org/10.5194/acp-16-10469-2016, https://doi.org/10.5194/acp-16-10469-2016, 2016
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A dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique were deployed at the Cabauw experimental site for atmospheric research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months, yielding a combined dataset with more than 2500 measurements of both δ13C and δD.
Joël Savarino, William C. Vicars, Michel Legrand, Suzanne Preunkert, Bruno Jourdain, Markus M. Frey, Alexandre Kukui, Nicolas Caillon, and Jaime Gil Roca
Atmos. Chem. Phys., 16, 2659–2673, https://doi.org/10.5194/acp-16-2659-2016, https://doi.org/10.5194/acp-16-2659-2016, 2016
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Atmospheric nitrate is collected on the East Antarctic ice sheet. Nitrogen and oxygen stable isotopes and concentrations of nitrate are measured. Using a box model, we show that there is s systematic discrepancy between observations and model results. We suggest that this discrepancy probably results from unknown NOx chemistry above the Antarctic ice sheet. However, possible misconception in the stable isotope mass balance is not completely excluded.
T. A. Berhanu, J. Savarino, J. Erbland, W. C. Vicars, S. Preunkert, J. F. Martins, and M. S. Johnson
Atmos. Chem. Phys., 15, 11243–11256, https://doi.org/10.5194/acp-15-11243-2015, https://doi.org/10.5194/acp-15-11243-2015, 2015
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In this field study at Dome C, Antarctica, we investigated the effect of solar UV photolysis on the stable isotopes of nitrate in snow via comparison of two identical snow pits while exposing only one to solar UV. From the difference between the average isotopic fractionations calculated for each pit, we determined a purely photolytic nitrogen isotopic fractionation of -55.8‰, in good agreement with what has been recently determined in a laboratory study.
M. Saccon, A. Kornilova, L. Huang, S. Moukhtar, and J. Rudolph
Atmos. Chem. Phys., 15, 10825–10838, https://doi.org/10.5194/acp-15-10825-2015, https://doi.org/10.5194/acp-15-10825-2015, 2015
E. D. Sofen, B. Alexander, E. J. Steig, M. H. Thiemens, S. A. Kunasek, H. M. Amos, A. J. Schauer, M. G. Hastings, J. Bautista, T. L. Jackson, L. E. Vogel, J. R. McConnell, D. R. Pasteris, and E. S. Saltzman
Atmos. Chem. Phys., 14, 5749–5769, https://doi.org/10.5194/acp-14-5749-2014, https://doi.org/10.5194/acp-14-5749-2014, 2014
J. Wintel, E. Hösen, R. Koppmann, M. Krebsbach, A. Hofzumahaus, and F. Rohrer
Atmos. Chem. Phys., 13, 11059–11071, https://doi.org/10.5194/acp-13-11059-2013, https://doi.org/10.5194/acp-13-11059-2013, 2013
F. A. Haumann, A. M. Batenburg, G. Pieterse, C. Gerbig, M. C. Krol, and T. Röckmann
Atmos. Chem. Phys., 13, 9401–9413, https://doi.org/10.5194/acp-13-9401-2013, https://doi.org/10.5194/acp-13-9401-2013, 2013
C. J. Sapart, P. Martinerie, E. Witrant, J. Chappellaz, R. S. W. van de Wal, P. Sperlich, C. van der Veen, S. Bernard, W. T. Sturges, T. Blunier, J. Schwander, D. Etheridge, and T. Röckmann
Atmos. Chem. Phys., 13, 6993–7005, https://doi.org/10.5194/acp-13-6993-2013, https://doi.org/10.5194/acp-13-6993-2013, 2013
J. Erbland, W. C. Vicars, J. Savarino, S. Morin, M. M. Frey, D. Frosini, E. Vince, and J. M. F. Martins
Atmos. Chem. Phys., 13, 6403–6419, https://doi.org/10.5194/acp-13-6403-2013, https://doi.org/10.5194/acp-13-6403-2013, 2013
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Short summary
Atmospheric airborne mercury is of particular concern because, once inhaled, both Hg and its vectors might have adverse effects on human beings. In this study, we attempted to identify the sources of PM2.5-Hg in Beijing, China, using Hg isotopic composition. Large range and seasonal variations in both mass-dependent and mass-independent fractionations of Hg isotopes in haze particles demonstrate the usefulness of Hg isotopes for directly tracing the sources and its vectors in the atmosphere.
Atmospheric airborne mercury is of particular concern because, once inhaled, both Hg and its...
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