Articles | Volume 22, issue 2
https://doi.org/10.5194/acp-22-1035-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-22-1035-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
21 Jan 2022
Research article |
| 21 Jan 2022
| 21 Jan 2022
Atmospheric measurements at Mt. Tai – Part II: HONO budget and radical (ROx + NO3) chemistry in the lower boundary layer
Chaoyang Xue
CORRESPONDING AUTHOR
Research Centre for Eco-Environmental Sciences, Chinese Academy of
Sciences, Beijing 100085, China
Laboratoire de Physique et Chimie de l'Environnement et de l'Espace
(LPC2E), CNRS–Université Orléans–CNES, CEDEX 2, Orléans 45071,
France
Research Centre for Eco-Environmental Sciences, Chinese Academy of
Sciences, Beijing 100085, China
State Key Joint Laboratory of Environment Simulation and Pollution
Control, College of Environmental Sciences and Engineering, Peking
University, Beijing 100871, China
Jörg Kleffmann
Physical and Theoretical Chemistry, University of Wuppertal,
Gaußstrasse 20, 42119 Wuppertal, Germany
Wenjin Zhang
Research Centre for Eco-Environmental Sciences, Chinese Academy of
Sciences, Beijing 100085, China
Xiaowei He
Research Centre for Eco-Environmental Sciences, Chinese Academy of
Sciences, Beijing 100085, China
College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China
Pengfei Liu
Research Centre for Eco-Environmental Sciences, Chinese Academy of
Sciences, Beijing 100085, China
Centre for Excellence in Regional Atmospheric Environment, Institute
of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China
Chenglong Zhang
Research Centre for Eco-Environmental Sciences, Chinese Academy of
Sciences, Beijing 100085, China
Centre for Excellence in Regional Atmospheric Environment, Institute
of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China
Xiaoxi Zhao
Research Centre for Eco-Environmental Sciences, Chinese Academy of
Sciences, Beijing 100085, China
College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China
Chengtang Liu
Research Centre for Eco-Environmental Sciences, Chinese Academy of
Sciences, Beijing 100085, China
Centre for Excellence in Regional Atmospheric Environment, Institute
of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China
Zhuobiao Ma
Research Centre for Eco-Environmental Sciences, Chinese Academy of
Sciences, Beijing 100085, China
Junfeng Liu
Research Centre for Eco-Environmental Sciences, Chinese Academy of
Sciences, Beijing 100085, China
Centre for Excellence in Regional Atmospheric Environment, Institute
of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China
Jinhe Wang
School of Municipal and Environmental Engineering, Co-Innovation
Centre for Green Building of Shandong Province, Shandong Jianzhu University,
Jinan 250101, China
Keding Lu
State Key Joint Laboratory of Environment Simulation and Pollution
Control, College of Environmental Sciences and Engineering, Peking
University, Beijing 100871, China
Valéry Catoire
Laboratoire de Physique et Chimie de l'Environnement et de l'Espace
(LPC2E), CNRS–Université Orléans–CNES, CEDEX 2, Orléans 45071,
France
Abdelwahid Mellouki
Institut de Combustion Aérothermique, Réactivité et
Environnement, Centre National de la Recherche Scientifique (ICARE-CNRS),
CEDEX 2, Orléans 45071, France
Environmental Research Institute, Shandong University, Qingdao,
Shandong 266237, China
Research Centre for Eco-Environmental Sciences, Chinese Academy of
Sciences, Beijing 100085, China
Centre for Excellence in Regional Atmospheric Environment, Institute
of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China
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Wenjie Wang, Bin Yuan, Hang Su, Yafang Cheng, Jipeng Qi, Sihang Wang, Wei Song, Xinming Wang, Chaoyang Xue, Chaoqun Ma, Fengxia Bao, Hongli Wang, Shengrong Lou, and Min Shao
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The formation of secondary sulfate needs to be further explored. In this work, we simultaneously measured sulfur and oxygen isotopic compositions to gain an increased understanding of specific sulfate formation processes. The results indicated that secondary sulfate was mainly ascribed to SO2 homogeneous oxidation by OH radicals and heterogeneous oxidation by H2O2 and Fe3+ / O2. This study is favourable for deeply investigating the sulfur cycle in the atmosphere.
Yifei Song, Chaoyang Xue, Yuanyuan Zhang, Pengfei Liu, Fengxia Bao, Xuran Li, and Yujing Mu
Atmos. Chem. Phys., 23, 15733–15747, https://doi.org/10.5194/acp-23-15733-2023, https://doi.org/10.5194/acp-23-15733-2023, 2023
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We present measurements of HONO flux and related parameters over an agricultural field during a whole growing season of summer maize. This dataset allows studies on the characteristics and influencing factors of soil HONO emissions, determination of HONO emission factors, estimation of total HONO emissions at a national scale, and the discussion on future environmental policies in terms of mitigating regional air pollution.
Can Ye, Keding Lu, Xuefei Ma, Wanyi Qiu, Shule Li, Xinping Yang, Chaoyang Xue, Tianyu Zhai, Yuhan Liu, Xuan Li, Yang Li, Haichao Wang, Zhaofeng Tan, Xiaorui Chen, Huabin Dong, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 15455–15472, https://doi.org/10.5194/acp-23-15455-2023, https://doi.org/10.5194/acp-23-15455-2023, 2023
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In this study, combining comprehensive field measurements and a box model, we found NO2 conversion on the ground surface was the most important source for HONO production among the proposed heterogeneous and gas-phase HONO sources. In addition, HONO was found to evidently enhance O3 production and aggravate O3 pollution in summer in China. Our study improved our understanding of the relative importance of different HONO sources and the crucial role of HONO in O3 formation in polluted areas.
Jingjing Meng, Yachen Wang, Yuanyuan Li, Tonglin Huang, Zhifei Wang, Yiqiu Wang, Min Chen, Zhanfang Hou, Houhua Zhou, Keding Lu, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 23, 14481–14503, https://doi.org/10.5194/acp-23-14481-2023, https://doi.org/10.5194/acp-23-14481-2023, 2023
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This study investigated the effect of COVID-19 lockdown (LCD) measures on the formation and evolutionary process of diacids and related compounds from field observations. Results demonstrate that more aged organic aerosols are observed during the LCD due to the enhanced photochemical oxidation. Our study also found that the reactivity of 13C was higher than that of 12C in the gaseous photochemical oxidation, leading to higher δ13C values of C2 during the LCD than before the LCD.
Shasha Tian, Kexin Zu, Huabin Dong, Limin Zeng, Keding Lu, and Qi Chen
Atmos. Meas. Tech., 16, 5525–5535, https://doi.org/10.5194/amt-16-5525-2023, https://doi.org/10.5194/amt-16-5525-2023, 2023
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We developed an online NH3 monitoring system based on a selective colorimetric reaction and a long-path absorption photometer (SAC-LOPAP), which can run statically for a long time and be applied to the continuous online measurement of low concentrations of ambient air by optimizing the reaction conditions, adding a constant-temperature module and liquid flow controller. It is well suited for the investigation of the NH3 budget for urban to rural conditions in China.
Chaoyang Xue, Gisèle Krysztofiak, Vanessa Brocchi, Stéphane Chevrier, Michel Chartier, Patrick Jacquet, Claude Robert, and Valéry Catoire
Earth Syst. Sci. Data, 15, 4553–4569, https://doi.org/10.5194/essd-15-4553-2023, https://doi.org/10.5194/essd-15-4553-2023, 2023
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To understand tropospheric air pollution at regional and global scales, an infrared laser spectrometer called SPIRIT was used on aircraft to rapidly and accurately measure carbon monoxide (CO), an important indicator of air pollution, during the last decade. Measurements were taken for more than 200 flight hours over three continents. Levels of CO are mapped with 3D trajectories for each flight. Additionally, this can be used to validate model performance and satellite measurements.
Valerian Hahn, Ralf Meerkötter, Christiane Voigt, Sonja Gisinger, Daniel Sauer, Valéry Catoire, Volker Dreiling, Hugh Coe, Cyrille Flamant, Stefan Kaufmann, Jonas Kleine, Peter Knippertz, Manuel Moser, Philip Rosenberg, Hans Schlager, Alfons Schwarzenboeck, and Jonathan Taylor
Atmos. Chem. Phys., 23, 8515–8530, https://doi.org/10.5194/acp-23-8515-2023, https://doi.org/10.5194/acp-23-8515-2023, 2023
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During the DACCIWA campaign in West Africa, we found a 35 % increase in the cloud droplet concentration that formed in a polluted compared with a less polluted environment and a decrease of 17 % in effective droplet diameter. Radiative transfer simulations, based on the measured cloud properties, reveal that these low-level polluted clouds radiate only 2.6 % more energy back to space, compared with a less polluted cloud. The corresponding additional decrease in temperature is rather small.
Hejun Hu, Haichao Wang, Keding Lu, Jie Wang, Zelong Zheng, Xuezhen Xu, Tianyu Zhai, Xiaorui Chen, Xiao Lu, Wenxing Fu, Xin Li, Limin Zeng, Min Hu, Yuanhang Zhang, and Shaojia Fan
Atmos. Chem. Phys., 23, 8211–8223, https://doi.org/10.5194/acp-23-8211-2023, https://doi.org/10.5194/acp-23-8211-2023, 2023
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Nitrate radical chemistry is critical to the degradation of volatile organic compounds (VOCs) and secondary organic aerosol formation. This work investigated the level, seasonal variation, and trend of nitrate radical reactivity towards volatile organic compounds (kNO3) in Beijing. We show the key role of isoprene and styrene in regulating seasonal variation in kNO3 and rebuild a long-term record of kNO3 based on the reported VOC measurements.
Chengzhi Xing, Shiqi Xu, Yuhang Song, Cheng Liu, Yuhan Liu, Keding Lu, Wei Tan, Chengxin Zhang, Qihou Hu, Shanshan Wang, Hongyu Wu, and Hua Lin
Atmos. Chem. Phys., 23, 5815–5834, https://doi.org/10.5194/acp-23-5815-2023, https://doi.org/10.5194/acp-23-5815-2023, 2023
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High RH could contribute to the secondary formation of HONO in the sea atmosphere. High temperature could promote the formation of HONO from NO2 heterogeneous reactions in the sea and coastal atmosphere. The aerosol surface plays a more important role during the above process in coastal and sea cases. The generation rate of HONO from the NO2 heterogeneous reaction in the sea cases is larger than that in inland cases in higher atmospheric layers above 600 m.
Amelia M. H. Bond, Markus M. Frey, Jan Kaiser, Jörg Kleffmann, Anna E. Jones, and Freya A. Squires
Atmos. Chem. Phys., 23, 5533–5550, https://doi.org/10.5194/acp-23-5533-2023, https://doi.org/10.5194/acp-23-5533-2023, 2023
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Atmospheric nitrous acid (HONO) amount fractions measured at Halley Research Station, Antarctica, were found to be low. Vertical fluxes of HONO from the snow were also measured and agree with the estimated HONO production rate from photolysis of snow nitrate. In a simple box model of HONO sources and sinks, there was good agreement between the measured flux and amount fraction. HONO was found to be an important OH radical source at Halley.
Junhua Wang, Baozhu Ge, Xueshun Chen, Jie Li, Keding Lu, Yayuan Dong, Lei Kong, Zifa Wang, and Yuanhang Zhang
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2023-22, https://doi.org/10.5194/gmd-2023-22, 2023
Revised manuscript not accepted
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We developed a quantitative decoupling analysis (QDA) method to quantify the contributions of emissions, meteorology, chemical reactions, and their nonlinear interactions on PM2.5. We found the effects of adverse meteorological conditions and the importance of nonlinear interactions. This method can provide valuable information for understanding of key factors to heavy pollution, but also help the modelers to find out the sources of uncertainties in numerical models.
Tianyu Zhai, Keding Lu, Haichao Wang, Shengrong Lou, Xiaorui Chen, Renzhi Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 2379–2391, https://doi.org/10.5194/acp-23-2379-2023, https://doi.org/10.5194/acp-23-2379-2023, 2023
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Particulate nitrate is a growing issue in air pollution. Based on comprehensive field measurement, we show heavy nitrate pollution in eastern China in summer. OH reacting with NO2 at daytime dominates nitrate formation on clean days, while N2O5 hydrolysis largely enhances and become comparable with that of OH reacting with O2 on polluted days (67.2 % and 30.2 %). Model simulation indicates that VOC : NOx = 2 : 1 is effective in mitigating the O3 and nitrate pollution coordinately.
Xiaorui Chen, Haichao Wang, Tianyu Zhai, Chunmeng Li, and Keding Lu
Atmos. Meas. Tech., 15, 7019–7037, https://doi.org/10.5194/amt-15-7019-2022, https://doi.org/10.5194/amt-15-7019-2022, 2022
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N2O5 is an important reservoir of atmospheric nitrogen, on whose interface reaction ambient particles can largely influence the fate of nitrogen oxides and air quality. In this study, we develop an approach to enable the reactions of N2O5 on ambient particles directly in a tube reactor, deriving the reaction rates with high accuracy by means of a chemistry model. Its successful application helps complement the data scarcity and to fill the knowledge gap between laboratory and field results.
Haichao Wang, Bin Yuan, E Zheng, Xiaoxiao Zhang, Jie Wang, Keding Lu, Chenshuo Ye, Lei Yang, Shan Huang, Weiwei Hu, Suxia Yang, Yuwen Peng, Jipeng Qi, Sihang Wang, Xianjun He, Yubin Chen, Tiange Li, Wenjie Wang, Yibo Huangfu, Xiaobing Li, Mingfu Cai, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 22, 14837–14858, https://doi.org/10.5194/acp-22-14837-2022, https://doi.org/10.5194/acp-22-14837-2022, 2022
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We present intensive field measurement of ClNO2 in the Pearl River Delta in 2019. Large variation in the level, formation, and atmospheric impacts of ClNO2 was found in different air masses. ClNO2 formation was limited by the particulate chloride (Cl−) and aerosol surface area. Our results reveal that Cl− originated from various anthropogenic emissions rather than sea sources and show minor contribution to the O3 pollution and photochemistry.
Xinping Yang, Keding Lu, Xuefei Ma, Yue Gao, Zhaofeng Tan, Haichao Wang, Xiaorui Chen, Xin Li, Xiaofeng Huang, Lingyan He, Mengxue Tang, Bo Zhu, Shiyi Chen, Huabin Dong, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 22, 12525–12542, https://doi.org/10.5194/acp-22-12525-2022, https://doi.org/10.5194/acp-22-12525-2022, 2022
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We present the OH and HO2 radical observations at the Shenzhen site (Pearl River Delta, China) in the autumn of 2018. The diurnal maxima were 4.5 × 106 cm−3 for OH and 4.2 × 108 cm−3 for HO2 (including an estimated interference of 23 %–28 % from RO2 radicals during the daytime). The OH underestimation was identified again, and it was attributable to the missing OH sources. HO2 heterogeneous uptake, ROx sources and sinks, and the atmospheric oxidation capacity were evaluated as well.
Xuefei Ma, Zhaofeng Tan, Keding Lu, Xinping Yang, Xiaorui Chen, Haichao Wang, Shiyi Chen, Xin Fang, Shule Li, Xin Li, Jingwei Liu, Ying Liu, Shengrong Lou, Wanyi Qiu, Hongli Wang, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 22, 7005–7028, https://doi.org/10.5194/acp-22-7005-2022, https://doi.org/10.5194/acp-22-7005-2022, 2022
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This paper presents the first OH and HO2 radical observations made in the Yangtze River Delta in China, and strong oxidation capacity is discovered based on direct measurements. The impacts of new OH regeneration mechanisms, monoterpene oxidation, and HO2 uptake processes are examined and discussed. The sources and the factors to sustain such strong oxidation are the key to understanding the ozone pollution formed in this area.
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.
Lisa von der Heyden, Walter Wißdorf, Ralf Kurtenbach, and Jörg Kleffmann
Atmos. Meas. Tech., 15, 1983–2000, https://doi.org/10.5194/amt-15-1983-2022, https://doi.org/10.5194/amt-15-1983-2022, 2022
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A relaxed eddy accumulation (REA) system based on the LOPAP technique for the quantification of vertical fluxes of nitrous acid (HONO) was developed and tested in a field campaign. Typical diurnal variations of the HONO fluxes were observed with low, partly negative fluxes during night-time and higher positive fluxes around noon. The highest correlation of the HONO flux was observed with the product of the NO2 photolysis frequency and the NO2 concentration.
Xiaorui Chen, Haichao Wang, and Keding Lu
Atmos. Chem. Phys., 22, 3525–3533, https://doi.org/10.5194/acp-22-3525-2022, https://doi.org/10.5194/acp-22-3525-2022, 2022
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We use a complete set of simulations to evaluate whether equilibrium and steady state are appropriate for a chemical system involving several reactive nitrogen-containing species (NO2, NO3, and N2O5) under various conditions. A previously neglected bias for the coefficient applied for interpreting their effects is disclosed, and the relevant ambient factors are examined. We therefore provide a good solution to an accurate representation of nighttime chemistry in high-aerosol areas.
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.
Haichao Wang, Chao Peng, Xuan Wang, Shengrong Lou, Keding Lu, Guicheng Gan, Xiaohong Jia, Xiaorui Chen, Jun Chen, Hongli Wang, Shaojia Fan, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 22, 1845–1859, https://doi.org/10.5194/acp-22-1845-2022, https://doi.org/10.5194/acp-22-1845-2022, 2022
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Via combining laboratory and modeling work, we found that heterogeneous reaction of N2O5 with saline mineral dust aerosol could be an important source of tropospheric ClNO2 in inland regions.
Guillermo Villena and Jörg Kleffmann
Atmos. Meas. Tech., 15, 627–637, https://doi.org/10.5194/amt-15-627-2022, https://doi.org/10.5194/amt-15-627-2022, 2022
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A continuous source for the generation of pure HONO mixtures was developed and characterized, which is based on the Henry's law solubility of HONO in acidic aqueous solutions. The source shows a fast time response and an excellent long-term stability and can be easily adjusted to HONO mixing ratios in the range 0.05–500 ppb. A general equation based on Henry's law is developed, whereby the HONO concentration of the source can be absolutely calculated with an accuracy of better than 10 %.
Mike J. Newland, Yangang Ren, Max R. McGillen, Lisa Michelat, Véronique Daële, and Abdelwahid Mellouki
Atmos. Chem. Phys., 22, 1761–1772, https://doi.org/10.5194/acp-22-1761-2022, https://doi.org/10.5194/acp-22-1761-2022, 2022
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Wildfires are increasing in extent and severity, driven by climate change. Such fires emit large amounts of volatile organic compounds (VOCs) to the atmosphere. Many of these, such as the furans studied here, are very reactive and are rapidly converted to other VOCs, which are expected to have negative health effects and to further impact the climate. Here, we establish the importance of the nitrate radical for removing these compounds both during the night and during the day.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
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
Atmos. Chem. Phys., 21, 15985–16000, https://doi.org/10.5194/acp-21-15985-2021, https://doi.org/10.5194/acp-21-15985-2021, 2021
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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.
Shuping Zhang, Golam Sarwar, Jia Xing, Biwu Chu, Chaoyang Xue, Arunachalam Sarav, Dian Ding, Haotian Zheng, Yujing Mu, Fengkui Duan, Tao Ma, and Hong He
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.
Yangang Ren, Li Zhou, Abdelwahid Mellouki, Véronique Daële, Mahmoud Idir, Steven S. Brown, Branko Ruscic, Robert S. Paton, Max R. McGillen, and A. R. Ravishankara
Atmos. Chem. Phys., 21, 13537–13551, https://doi.org/10.5194/acp-21-13537-2021, https://doi.org/10.5194/acp-21-13537-2021, 2021
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Aromatic aldehydes are a family of compounds emitted into the atmosphere from both anthropogenic and biogenic sources that are formed from the degradation of aromatic hydrocarbons. Their atmospheric degradation may impact air quality. We report on their atmospheric degradation through reaction with NO3, which is useful to estimate their atmospheric lifetimes. We have also attempted to elucidate the mechanism of these reactions via studies of isotopic substitution and quantum chemistry.
Alexandre Kukui, Michel Chartier, Jinhe Wang, Hui Chen, Sébastien Dusanter, Stéphane Sauvage, Vincent Michoud, Nadine Locoge, Valérie Gros, Thierry Bourrianne, Karine Sellegri, and Jean-Marc Pichon
Atmos. Chem. Phys., 21, 13333–13351, https://doi.org/10.5194/acp-21-13333-2021, https://doi.org/10.5194/acp-21-13333-2021, 2021
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Sulfuric acid, H2SO4, plays a key role in formation of secondary atmospheric aerosol particles. It is generally accepted that the major atmospheric source of H2SO4 is the reaction of OH radicals with SO2. In this study, importance of an additional H2SO4 source via oxidation of SO2 by stabilized Criegee intermediates was estimated based on measurements at a remote site on Cape Corsica. It was found that the oxidation of SO2 by SCI may be an important source of H2SO4, especially during nighttime.
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.
Junhua Wang, Baozhu Ge, Xueshun Chen, Jie Li, Keding Lu, Yayuan Dong, Lei Kong, Zifa Wang, and Yuanhang Zhang
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-259, https://doi.org/10.5194/gmd-2021-259, 2021
Revised manuscript not accepted
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This paper developed a novel quantitative decoupling analysis (QDA) method to quantify the contributions of emission, meteorology, chemical reaction, and their nonlinear interactions on PM2.5 and applied it to a pollution episode in Beijing. This method can provides the researchers and policy makers with valuable information for understanding of key factors to heavy pollution, but also help the modelers to find out the sources of uncertainties among numerical models.
Gang Zhao, Yishu Zhu, Zhijun Wu, Taomou Zong, Jingchuan Chen, Tianyi Tan, Haichao Wang, Xin Fang, Keding Lu, Chunsheng Zhao, and Min Hu
Atmos. Chem. Phys., 21, 9995–10004, https://doi.org/10.5194/acp-21-9995-2021, https://doi.org/10.5194/acp-21-9995-2021, 2021
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New particle formation is thought to contribute half of the global cloud condensation nuclei. We find that the new particle formation is more likely to happen in the upper boundary layer than that at the ground, which can be partially explained by the aerosol–radiation interaction. Our study emphasizes the influence of aerosol–radiation interaction on the NPF.
Chunmeng Li, Haichao Wang, Xiaorui Chen, Tianyu Zhai, Shiyi Chen, Xin Li, Limin Zeng, and Keding Lu
Atmos. Meas. Tech., 14, 4033–4051, https://doi.org/10.5194/amt-14-4033-2021, https://doi.org/10.5194/amt-14-4033-2021, 2021
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We present a feasible instrument for the measurement of NO2, total peroxy nitrates (PNs, RO2NO2), and total alkyl nitrates (ANs, RONO2) in the atmosphere. The instrument samples sequentially from three channels at different temperature settings and then measures spectra using one cavity-enhanced absorption spectrometer. The concentrations are determined by spectral fitting and corrected using the lookup table method conveniently. The instrument will promote the study of PNs and ANs.
Mengdi Song, Xin Li, Suding Yang, Xuena Yu, Songxiu Zhou, Yiming Yang, Shiyi Chen, Huabin Dong, Keren Liao, Qi Chen, Keding Lu, Ningning Zhang, Junji Cao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 4939–4958, https://doi.org/10.5194/acp-21-4939-2021, https://doi.org/10.5194/acp-21-4939-2021, 2021
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Due to their lower diffusion capacities and higher conversion capacities, urban areas in Xi’an experienced severe ozone pollution in the summer. In this study, a campaign of comprehensive field observations and VOC grid sampling was conducted in Xi’an from 20 June to 20 July 2019. We found that Xi'an has a strong local emission source of VOCs, and vehicle exhaust was the primary VOC source. In addition, alkenes, aromatics, and oxygenated VOCs played a dominant role in secondary transformations.
Abdelwahid Mellouki, Markus Ammann, R. Anthony Cox, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 4797–4808, https://doi.org/10.5194/acp-21-4797-2021, https://doi.org/10.5194/acp-21-4797-2021, 2021
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Volatile organic compounds play an important role in atmospheric chemistry. This article, the eighth in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers the gas-phase reactions of organic species with four, or more, carbon atoms (≥ C4) including thermal reactions of closed-shell organic species with HO and NO3 radicals and their photolysis. These data are important for atmospheric models.
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.
Huan Song, Xiaorui Chen, Keding Lu, Qi Zou, Zhaofeng Tan, Hendrik Fuchs, Alfred Wiedensohler, Daniel R. Moon, Dwayne E. Heard, María-Teresa Baeza-Romero, Mei Zheng, Andreas Wahner, Astrid Kiendler-Scharr, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 15835–15850, https://doi.org/10.5194/acp-20-15835-2020, https://doi.org/10.5194/acp-20-15835-2020, 2020
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Accurate calculation of the HO2 uptake coefficient is one of the key parameters to quantify the co-reduction of both aerosol and ozone pollution. We modelled various lab measurements of γHO2 based on a gas-liquid phase kinetic model and developed a state-of-the-art parameterized equation. Based on a dataset from a comprehensive field campaign in the North China Plain, we proposed that the determination of the heterogeneous uptake process for HO2 should be included in future field campaigns.
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.
R. Anthony Cox, Markus Ammann, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 20, 13497–13519, https://doi.org/10.5194/acp-20-13497-2020, https://doi.org/10.5194/acp-20-13497-2020, 2020
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Criegee intermediates, formed from alkene–ozone reactions, play a potentially important role as tropospheric oxidants. Evaluated kinetic data are provided for reactions governing their formation and removal for use in atmospheric models. These include their formation from reactions of simple and complex alkenes and removal by decomposition and reaction with a number of atmospheric species (e.g. H2O, SO2). An overview of the tropospheric chemistry of Criegee intermediates is also provided.
Yangang Ren, Bastian Stieger, Gerald Spindler, Benoit Grosselin, Abdelwahid Mellouki, Thomas Tuch, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 20, 13069–13089, https://doi.org/10.5194/acp-20-13069-2020, https://doi.org/10.5194/acp-20-13069-2020, 2020
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We present HONO measurements from the TROPOS research site in Melpitz, Germany. Investigations of HONO sources and sinks revealed the nighttime formation by heterogeneous conversion of NO2 to HONO followed by a significant surface deposition at night. The evaporation of dew was identified as the main HONO source in the morning. In the following, dew measurements with a self-made dew collector were performed to estimate the amount of evaporated HONO from dew in the atmospheric HONO distribution.
Ruqian Miao, Qi Chen, Yan Zheng, Xi Cheng, Yele Sun, Paul I. Palmer, Manish Shrivastava, Jianping Guo, Qiang Zhang, Yuhan Liu, Zhaofeng Tan, Xuefei Ma, Shiyi Chen, Limin Zeng, Keding Lu, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 12265–12284, https://doi.org/10.5194/acp-20-12265-2020, https://doi.org/10.5194/acp-20-12265-2020, 2020
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In this study we evaluated the model performances for simulating secondary inorganic aerosol (SIA) and organic aerosol (OA) in PM2.5 in China against comprehensive datasets. The potential biases from factors related to meteorology, emission, chemistry, and atmospheric removal are systematically investigated. This study provides a comprehensive understanding of modeling PM2.5, which is important for studies on the effectiveness of emission control strategies.
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Short summary
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.
Nitrous acid (HONO) and related parameters were measured at the foot and the summit of Mt. Tai...
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