Articles | Volume 18, issue 11
https://doi.org/10.5194/amt-18-2509-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-18-2509-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
12 Jun 2025
Research article |
| 12 Jun 2025
| 12 Jun 2025
A comprehensive characterization of empirical parameterizations for OH exposure in the Aerodyne Potential Aerosol Mass Oxidation Flow Reactor (PAM-OFR)
Qianying Liu
Department of Civil and Environmental Engineering, Faculty of Science and Technology, University of Macau, Taipa, Macau SAR, 999078, China
Department of Ocean Science and Technology, Faculty of Science and Technology, University of Macau, Taipa, Macau SAR, 999078, China
State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex, Shanghai Academy of Environmental Sciences, Shanghai, 200233, China
State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex, Shanghai Academy of Environmental Sciences, Shanghai, 200233, China
Andrew T. Lambe
Aerodyne Research Inc., Billerica, Massachusetts, 01821, United States
Shengrong Lou
State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex, Shanghai Academy of Environmental Sciences, Shanghai, 200233, China
Lulu Zeng
Department of Civil and Environmental Engineering, Faculty of Science and Technology, University of Macau, Taipa, Macau SAR, 999078, China
Department of Ocean Science and Technology, Faculty of Science and Technology, University of Macau, Taipa, Macau SAR, 999078, China
Yuhang Wu
State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex, Shanghai Academy of Environmental Sciences, Shanghai, 200233, China
Congyan Huang
State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex, Shanghai Academy of Environmental Sciences, Shanghai, 200233, China
Shikang Tao
State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex, Shanghai Academy of Environmental Sciences, Shanghai, 200233, China
Xi Cheng
School of Chemical and Environmental Engineering, China University of Mining and Technology (Beijing), Beijing 100083, China
State Key Joint Laboratory of Environmental Simulation and Pollution Control, BIC-ESAT and IJRC, College of Environmental Sciences and Engineering, Peking University, Beijing, China
Ka In Hoi
Department of Civil and Environmental Engineering, Faculty of Science and Technology, University of Macau, Taipa, Macau SAR, 999078, China
Department of Ocean Science and Technology, Faculty of Science and Technology, University of Macau, Taipa, Macau SAR, 999078, China
Hongli Wang
State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex, Shanghai Academy of Environmental Sciences, Shanghai, 200233, China
Kai Meng Mok
Department of Civil and Environmental Engineering, Faculty of Science and Technology, University of Macau, Taipa, Macau SAR, 999078, China
Department of Ocean Science and Technology, Faculty of Science and Technology, University of Macau, Taipa, Macau SAR, 999078, China
Cheng Huang
State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex, Shanghai Academy of Environmental Sciences, Shanghai, 200233, China
Shanghai Environmental Monitoring Center, Shanghai, 200030, China
Yong Jie Li
CORRESPONDING AUTHOR
Department of Civil and Environmental Engineering, Faculty of Science and Technology, University of Macau, Taipa, Macau SAR, 999078, China
Department of Ocean Science and Technology, Faculty of Science and Technology, University of Macau, Taipa, Macau SAR, 999078, China
Related authors
Ya-Nan Zhan, Dan Dan Huang, Yaqin Gao, Sheng’ao Jing, Jun Pan, Yingjie Li, Juntao Huo, Yi Sun, Haobin Zhong, Wei Xu, Jing Duan, Ting Wang, Qianying Liu, Lulu Zeng, Yong Jie Li, Cheng Huang, Hongli Wang, Qingyan Fu, and Ru-Jin Huang
EGUsphere, https://doi.org/10.5194/egusphere-2026-6370, https://doi.org/10.5194/egusphere-2026-6370, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
This study investigates secondary organic aerosol formation in coastal air using a field-deployed oxidation flow reactor, quantitatively constrains its formation potential and the contributions of major precursors, reveals contrasting production from marine and continental air masses, and highlights the roles of high humidity and continental outflow in secondary organic aerosol formation. These results have implications for air pollution in nearby urban regions.
Ya-Nan Zhan, Dan Dan Huang, Yaqin Gao, Sheng’ao Jing, Jun Pan, Yingjie Li, Juntao Huo, Yi Sun, Haobin Zhong, Wei Xu, Jing Duan, Ting Wang, Qianying Liu, Lulu Zeng, Yong Jie Li, Cheng Huang, Hongli Wang, Qingyan Fu, and Ru-Jin Huang
EGUsphere, https://doi.org/10.5194/egusphere-2026-6370, https://doi.org/10.5194/egusphere-2026-6370, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
This study investigates secondary organic aerosol formation in coastal air using a field-deployed oxidation flow reactor, quantitatively constrains its formation potential and the contributions of major precursors, reveals contrasting production from marine and continental air masses, and highlights the roles of high humidity and continental outflow in secondary organic aerosol formation. These results have implications for air pollution in nearby urban regions.
Qiongqiong Wang, Zhongliang Huang, Zongjun Li, Shuihui Zhu, Liping Qiao, Min Zhou, Dandan Huang, Hongli Wang, Qingyan Fu, Kezheng Liao, and Jian Zhen Yu
EGUsphere, https://doi.org/10.5194/egusphere-2026-4766, https://doi.org/10.5194/egusphere-2026-4766, 2026
Short summary
Short summary
Brown carbon (BrC) is a poorly understood carbonaceous aerosol component that significantly affects climate and air quality. We examined the sources and secondary formation of BrC based on long-term field measurements of bihourly BrC and a suite of organic and elemental tracers in urban Shanghai. Seasonal contrast of source contributions and complexity of secondary formation and evolution was observed. This study offers a scientific basis for BrC mitigation and urban air quality improvement.
Wenfei Zhu, Qinghong Wang, Qingsong Wang, Jialin Shi, Yu Sun, Juntao Huo, Yi Sun, Jia Chen, Yue Zhao, Mei Li, Jun Chen, Shengrong Lou, and Hui Chen
EGUsphere, https://doi.org/10.5194/egusphere-2026-2447, https://doi.org/10.5194/egusphere-2026-2447, 2026
Short summary
Short summary
This study examines nitrate-containing particles during winter haze in eastern China. A framework combining single-particle mass spectrometry and statistical analysis was developed to better quantify nitrate sources. Results show that nitrate is mainly found in aged particles and strongly mixed with combustion and marine emissions. Pollution episodes are driven by stagnant conditions, high humidity, nighttime reactions, and regional transport.
Ruqian Miao, Ruochong Xu, Shan Huang, Sihan Xiao, Hao Wang, Yan Zheng, Siyi Liu, Jingxian Li, Guannan Geng, Manish Shrivastava, Xu Dao, Claire Granier, Guy Brasseur, Vlassis A. Karydis, Alexandra P. Tsimpidi, Jianhui Jiang, Kaspar R. Daellenbach, Imad El Haddad, André S. H. Prévôt, and Qi Chen
EGUsphere, https://doi.org/10.5194/egusphere-2026-3160, https://doi.org/10.5194/egusphere-2026-3160, 2026
Short summary
Short summary
Primary and secondary organic aerosols (POA and SOA) have distinct climate and human health impacts. We develop an OA simulation framework resolving the full volatility spectrum of organic precursor emissions, which improves global POA and SOA characterization. Reassessing their global distributions and budgets, this study shows greater POA and SOA burdens than previous estimates and presents region-dependent OA sources and variability to guide health-oriented pollution mitigation strategies.
Xun Li, Xuan Li, Rusha Yan, Yaqin Gao, Kangjia Gong, Hongli Wang, Momei Qin, Jianlin Hu, and Jingyi Li
Atmos. Chem. Phys., 26, 4901–4915, https://doi.org/10.5194/acp-26-4901-2026, https://doi.org/10.5194/acp-26-4901-2026, 2026
Short summary
Short summary
An updated emission inventory, incorporating source-specific OVOC (Oxygenated volatile organic compound) profiles derived from measurements and the literature, is applied in an air quality model to improve OVOC simulations in a heavily polluted region. A substantial fraction of key OVOCs originates from anthropogenic sources and enhances hydroperoxyl radical production, thereby contributing to ozone formation. The results highlight the importance of accurately representing OVOC emissions in models to support ozone control strategies.
Yali Jin, Hao Luo, Siqi Tang, Shuhui Xue, Chengyu Nie, Xiaocong Peng, Yan Zheng, Weiqi Xu, Guohua Zhang, Xiaole Pan, Yele Sun, Qi Chen, Lanzhong Liu, and Defeng Zhao
Atmos. Chem. Phys., 26, 2813–2830, https://doi.org/10.5194/acp-26-2813-2026, https://doi.org/10.5194/acp-26-2813-2026, 2026
Short summary
Short summary
Cloud substantially changes the compositions organic aerosol. How cloud processing of organics occur on molecular level remains unclear. We found that compared with cloud free particles, organics in cloud contains more large molecules likely due to accretion reactions and has more nitrogen-containing compounds. We identify some new compounds formed in cloud. Such modifications of the organics in cloud can further change its physicochemical properties, and impact on climate and human health.
Chunshui Lin, Ru-Jin Huang, Jing Duan, Jing Qu, Jiahua Liu, Yi Liu, Yan Luo, Wei Huang, Wei Xu, Yanan Zhan, Zhitao Liu, Sihan Liu, Qingshuang Zhang, Quan Liu, Zirui Liu, Shengrong Lou, Huinan Yang, Dan Dan Huang, Cheng Huang, and Hongli Wang
Atmos. Chem. Phys., 26, 2635–2647, https://doi.org/10.5194/acp-26-2635-2026, https://doi.org/10.5194/acp-26-2635-2026, 2026
Short summary
Short summary
Since China's 2013 Clean Air Act cut PM2.5 by over half, winter haze in the North China Plain persists partly due to secondary organic aerosols now dominating primary organic aerosol, requiring urgent regional cooperation to address model-underestimated chemical transformations and cross-border pollution.
Song Liu, Xiaopu Lyu, Fumo Yang, Zongbo Shi, Xin Huang, Tengyu Liu, Hongli Wang, Mei Li, Jian Gao, Nan Chen, Guoliang Shi, Yu Zou, Chenglei Pei, Chengxu Tong, Xinyi Liu, Li Zhou, Alex B. Guenther, and Nan Wang
Atmos. Chem. Phys., 26, 635–646, https://doi.org/10.5194/acp-26-635-2026, https://doi.org/10.5194/acp-26-635-2026, 2026
Short summary
Short summary
We studied the invisible gas isoprene, which trees and vehicles release into the air and which can worsen urban smog. Using advanced computer learning trained on measurements from many cities, we uncovered how temperature, sunlight, and city greening shape isoprene levels. Comparing Hong Kong and London, we found climate warming boosts isoprene and future ozone pollution, but strong cuts in anthropogenic emission could limit this impact.
Ruiqi Man, Yishu Zhu, Zhijun Wu, Peter Aaron Alpert, Bingbing Wang, Jing Dou, Jie Chen, Yan Zheng, Yanli Ge, Qi Chen, Shiyi Chen, Xiangrui Kong, Markus Ammann, and Min Hu
Atmos. Chem. Phys., 26, 349–363, https://doi.org/10.5194/acp-26-349-2026, https://doi.org/10.5194/acp-26-349-2026, 2026
Short summary
Short summary
The particle chemical morphology is important to atmospheric multiphase and heterogeneous chemistry. This work directly observed the core-shell structure and water uptake behavior of individual submicron aerosol particles at an urban site and elucidated the potential impact on particle reactive uptake and heterogeneous reactions.
Yi Liu, Xin Li, Ying Liu, Shuyu He, Yuqing Qiu, Mengdi Song, Jiarong Ye, Shengrong Lou, Sihua Lu, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 25, 15819–15834, https://doi.org/10.5194/acp-25-15819-2025, https://doi.org/10.5194/acp-25-15819-2025, 2025
Short summary
Short summary
We developed a method for speciated and quantitative measurement of peroxy radicals formed during the breakdown of aromatic hydrocarbons. These measurements revealed missing reaction pathways in current chemical mechanisms. Our findings help improve predictions of air quality and deepen understanding of chemical processes in the atmosphere.
Liuwei Kong, Xin Li, Yu Wang, Sihua Lu, Ying Liu, Shengrong Lou, Wenxin Zhou, Xinping Yang, Yan Ding, Yi Liu, Mengdi Song, Shuyu He, Kai Wang, Feng Wang, Xiaocen Shi, Jian Wang, Yun Zou, Chaofan Lian, Hefan Liu, Miao Feng, Xiaoya Dou, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 25, 13311–13326, https://doi.org/10.5194/acp-25-13311-2025, https://doi.org/10.5194/acp-25-13311-2025, 2025
Short summary
Short summary
Our research investigates the volatile organic compounds evaporative emission characteristics of China's typical representative vehicle regulatory standards. The emission factors, chemical composition characteristics and source profiles of volatile organic compounds were determined. The hydroxyl radical total reactivity and compositions of evaporative emissions were quantified, and identified key volatile organic compounds reactive species contributing to atmospheric photochemical processes.
Donger Lai, Yanxin Bai, Zijing Zhang, Pui-Kin So, Yong Jie Li, Ying-Lung Steve Tse, Ying-Yeung Yeung, Thomas Schaefer, Hartmut Herrmann, Jian Zhen Yu, Yuchen Wang, and Man Nin Chan
Atmos. Chem. Phys., 25, 12569–12584, https://doi.org/10.5194/acp-25-12569-2025, https://doi.org/10.5194/acp-25-12569-2025, 2025
Short summary
Short summary
Aqueous-phase •OH oxidation can potentially act as an important atmospheric sink for α-pinene-derived organosulfates (OSs). Such oxidation can also generate a variety of new OS products, and can be as a potential source for some atmospheric OSs with previously unknown origins.
Guangyuan Yu, Yan Zhang, Qian Wang, Zimin Han, Shenglan Jiang, Fan Yang, Xin Yang, and Cheng Huang
Atmos. Chem. Phys., 25, 9497–9518, https://doi.org/10.5194/acp-25-9497-2025, https://doi.org/10.5194/acp-25-9497-2025, 2025
Short summary
Short summary
China has carried out staged low-sulfur fuel policies since 2017. This study simulated the changing spatiotemporal patterns of the impacts of ship emissions on PM2.5 from 2017 to 2021 based on the updated emission inventories and mapping of chemical species in the CMAQ (Community Multiscale Air Quality). Fuel policies caused evident relative changes in inorganic and organic components of the shipping-related PM2.5 over China’s port cities. The driving factors of the interannual, seasonal, and diurnal patterns were discussed.
Xu Yu, Min Zhou, Shuhui Zhu, Liping Qiao, Jinjian Li, Yingge Ma, Zijing Zhang, Kezheng Liao, Hongli Wang, and Jian Zhen Yu
Atmos. Chem. Phys., 25, 9061–9074, https://doi.org/10.5194/acp-25-9061-2025, https://doi.org/10.5194/acp-25-9061-2025, 2025
Short summary
Short summary
Online measurements of bulk aerosol organic nitrogen (ON), in conjunction with a comprehensive array of source markers, have revealed five emission sources and five potentially significant formation processes of nitrogenous organic aerosols. This study provides a first quantitative source analysis of ON aerosol and valuable observational evidence of secondary ON aerosol formation through NH3 and NOx chemistries.
Yu Huang, Xingru Li, Dan Dan Huang, Ruoyuan Lei, Binhuang Zhou, Yunjiang Zhang, and Xinlei Ge
Atmos. Chem. Phys., 25, 7619–7645, https://doi.org/10.5194/acp-25-7619-2025, https://doi.org/10.5194/acp-25-7619-2025, 2025
Short summary
Short summary
This work comprises a comprehensive investigation into the chemical and optical properties of brown carbon (BrC) in PM2.5 samples collected in Nanjing, China. In particular, we used a machine learning approach to identify a list of key BrC species, which can be a good reference for future studies. Our findings extend understanding of BrC properties and are valuable to the assessment of BrC's impact on air quality and radiative forcing.
Chunmeng Li, Xiaorui Chen, Haichao Wang, Tianyu Zhai, Xuefei Ma, Xinping Yang, Shiyi Chen, Min Zhou, Shengrong Lou, Xin Li, Limin Zeng, and Keding Lu
Atmos. Chem. Phys., 25, 3905–3918, https://doi.org/10.5194/acp-25-3905-2025, https://doi.org/10.5194/acp-25-3905-2025, 2025
Short summary
Short summary
This study reports an observation of organic nitrate (including total peroxy nitrates and total alkyl nitrates) in Shanghai, China, during the summer of 2021, by homemade thermal dissociation cavity-enhanced absorption spectroscopy (TD-CEAS; Atmos. Meas. Tech., 14, 4033–4051, 2021). The distribution of organic nitrates and their effects on local ozone production are analyzed based on field observations in conjunction with model simulations.
Renzhi Hu, Guoxian Zhang, Haotian Cai, Jingyi Guo, Keding Lu, Xin Li, Shengrong Lou, Zhaofeng Tan, Changjin Hu, Pinhua Xie, and Wenqing Liu
Atmos. Chem. Phys., 25, 3011–3028, https://doi.org/10.5194/acp-25-3011-2025, https://doi.org/10.5194/acp-25-3011-2025, 2025
Short summary
Short summary
A full suite of radical measurements (OH, HO2, RO2, and kOH) was established to accurately elucidate the limitations of oxidation in a chemically complex atmosphere. Sensitivity tests revealed that the incorporation of complex processes enabled a balance in both radical concentrations and coordinate ratios, effectively addressing the deficiency in the ozone generation mechanism. The full-chain radical detection bridged the gap between the photochemistry and the intensive oxidation level.
Han Zang, Zekun Luo, Chenxi Li, Ziyue Li, Dandan Huang, and Yue Zhao
Atmos. Chem. Phys., 24, 11701–11716, https://doi.org/10.5194/acp-24-11701-2024, https://doi.org/10.5194/acp-24-11701-2024, 2024
Short summary
Short summary
Atmospheric organics are subject to synergistic oxidation by different oxidants, yet the mechanisms of such processes are poorly understood. Here, using direct measurements and kinetic modeling, we probe the nocturnal synergistic-oxidation mechanism of α-pinene by O3 and NO3 radicals and in particular the fate of peroxy radical intermediates of different origins, which will deepen our understanding of the monoterpene oxidation chemistry and its contribution to atmospheric particle formation.
Mengdi Song, Shuyu He, Xin Li, Ying Liu, Shengrong Lou, Sihua Lu, Limin Zeng, and Yuanhang Zhang
Atmos. Meas. Tech., 17, 5113–5127, https://doi.org/10.5194/amt-17-5113-2024, https://doi.org/10.5194/amt-17-5113-2024, 2024
Short summary
Short summary
We introduce detailed and improved quantitation and semi-quantitation methods of iodide-adduct time-of-flight chemical ionization mass spectrometry (I-CIMS) to measure toluene oxidation intermediates. We assess the experimental sensitivity of various functional group species and their binding energy with iodide ions in I-CIMS. A novel classification approach was introduced to significantly enhance the accuracy of semi-quantitative methods (improving R2 values from 0.52 to beyond 0.88).
Tianle Pan, Andrew T. Lambe, Weiwei Hu, Yicong He, Minghao Hu, Huaishan Zhou, Xinming Wang, Qingqing Hu, Hui Chen, Yue Zhao, Yuanlong Huang, Doug R. Worsnop, Zhe Peng, Melissa A. Morris, Douglas A. Day, Pedro Campuzano-Jost, Jose-Luis Jimenez, and Shantanu H. Jathar
Atmos. Meas. Tech., 17, 4915–4939, https://doi.org/10.5194/amt-17-4915-2024, https://doi.org/10.5194/amt-17-4915-2024, 2024
Short summary
Short summary
This study systematically characterizes the temperature enhancement in the lamp-enclosed oxidation flow reactor (OFR). The enhancement varied multiple dimensional factors, emphasizing the complexity of temperature inside of OFR. The effects of temperature on the flow field and gas- or particle-phase reaction inside OFR were also evaluated with experiments and model simulations. Finally, multiple mitigation strategies were demonstrated to minimize this temperature increase.
Fan Zhang, Binyu Xiao, Zeyu Liu, Yan Zhang, Chongguo Tian, Rui Li, Can Wu, Yali Lei, Si Zhang, Xinyi Wan, Yubao Chen, Yong Han, Min Cui, Cheng Huang, Hongli Wang, Yingjun Chen, and Gehui Wang
Atmos. Chem. Phys., 24, 8999–9017, https://doi.org/10.5194/acp-24-8999-2024, https://doi.org/10.5194/acp-24-8999-2024, 2024
Short summary
Short summary
Mandatory use of low-sulfur fuel due to global sulfur limit regulations means large uncertainties in volatile organic compound (VOC) emissions. On-board tests of VOCs from nine cargo ships in China were carried out. Results showed that switching from heavy-fuel oil to diesel increased emission factor VOCs by 48 % on average, enhancing O3 and the secondary organic aerosol formation potential. Thus, implementing a global ultra-low-sulfur oil policy needs to be optimized in the near future.
Fei Ye, Jingyi Li, Yaqin Gao, Hongli Wang, Jingyu An, Cheng Huang, Song Guo, Keding Lu, Kangjia Gong, Haowen Zhang, Momei Qin, and Jianlin Hu
Atmos. Chem. Phys., 24, 7467–7479, https://doi.org/10.5194/acp-24-7467-2024, https://doi.org/10.5194/acp-24-7467-2024, 2024
Short summary
Short summary
Naphthalene (Nap) and methylnaphthalene (MN) are key precursors of secondary organic aerosol (SOA), yet their sources and sinks are often inadequately represented in air quality models. In this study, we incorporated detailed emissions, gas-phase chemistry, and SOA parameterization of Nap and MN into CMAQ to address this issue. The findings revealed remarkably high SOA formation potentials for these compounds despite their low emissions in the Yangtze River Delta region during summer.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
Atmos. Chem. Phys., 24, 5625–5636, https://doi.org/10.5194/acp-24-5625-2024, https://doi.org/10.5194/acp-24-5625-2024, 2024
Short summary
Short summary
Cooking is a major source of particles in urban areas. Previous studies demonstrated that the chemical lifetimes of cooking organic aerosols (COAs) were much shorter (~minutes) than the values reported by field observations (~hours). We conducted laboratory experiments to resolve the discrepancy by considering suppressed reactivity under low temperature. The parameterized k2–T relationships and observed surface temperature data were used to estimate the chemical lifetimes of COA particles.
Liangbin Wu, Cheng Wu, Tao Deng, Dui Wu, Mei Li, Yong Jie Li, and Zhen Zhou
Atmos. Meas. Tech., 17, 2917–2936, https://doi.org/10.5194/amt-17-2917-2024, https://doi.org/10.5194/amt-17-2917-2024, 2024
Short summary
Short summary
Field comparison of dual-spot (AE33) and single-spot (AE31) Aethalometers by full-year collocated measurements suggests that site-specific correction factors are needed to ensure the long-term data continuity for AE31-to-AE33 transition in black carbon monitoring networks; babs agrees well between AE33 and AE31, with slight variations by wavelength (slope: 0.87–1.04; R2: 0.95–0.97). A ~ 20 % difference in secondary brown carbon light absorption was found between AE33 and AE31.
Fangbing Li, Dan Dan Huang, Linhui Tian, Bin Yuan, Wen Tan, Liang Zhu, Penglin Ye, Douglas Worsnop, Ka In Hoi, Kai Meng Mok, and Yong Jie Li
Atmos. Meas. Tech., 17, 2415–2427, https://doi.org/10.5194/amt-17-2415-2024, https://doi.org/10.5194/amt-17-2415-2024, 2024
Short summary
Short summary
The responses of protonated, adduct, and fragmented ions of 21 volatile organic compounds (VOCs) were investigated with varying instrument settings and relative humidity (RH) in a Vocus proton-transfer-reaction mass spectrometer (PTR-MS). The protonated ions of most VOCs studied show < 15 % variation in sensitivity, except for some long-chain aldehydes. The relationship between sensitivity and PTR rate constant is complicated by the influences from ion transmission and protonated ion fraction.
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
Atmos. Chem. Phys., 24, 4017–4027, https://doi.org/10.5194/acp-24-4017-2024, https://doi.org/10.5194/acp-24-4017-2024, 2024
Short summary
Short summary
This study investigates the important role of unmeasured volatile organic compounds (VOCs) in ozone formation. Based on results in a megacity of China, we show that unmeasured VOCs can contribute significantly to ozone fomation and also influence the determination of ozone control strategy. Our results show that these unmeasured VOCs are mainly from human sources.
Xi Cheng, Yong Jie Li, Yan Zheng, Keren Liao, Theodore K. Koenig, Yanli Ge, Tong Zhu, Chunxiang Ye, Xinghua Qiu, and Qi Chen
Atmos. Chem. Phys., 24, 2099–2112, https://doi.org/10.5194/acp-24-2099-2024, https://doi.org/10.5194/acp-24-2099-2024, 2024
Short summary
Short summary
In this study we conducted laboratory measurements to investigate the formation of gas-phase oxygenated organic molecules (OOMs) from six aromatic volatile organic compounds (VOCs). We provide a thorough analysis on the effects of precursor structure (substituents and ring numbers) on product distribution and highlight from a laboratory perspective that heavy (e.g., double-ring) aromatic VOCs are important in initial particle growth during secondary organic aerosol formation.
Qiongqiong Wang, Shuhui Zhu, Shan Wang, Cheng Huang, Yusen Duan, and Jian Zhen Yu
Atmos. Chem. Phys., 24, 475–486, https://doi.org/10.5194/acp-24-475-2024, https://doi.org/10.5194/acp-24-475-2024, 2024
Short summary
Short summary
We investigated short-term source apportionment of PM2.5 utilizing rolling positive matrix factorization (PMF) and online PM chemical speciation data, which included source-specific organic tracers collected over a period of 37 d during the winter of 2019–2020 in suburban Shanghai, China. The findings highlight that by imposing constraints on the primary source profiles, short-term PMF analysis successfully replicated both the individual primary sources and the total secondary sources.
Abd El Rahman El Mais, Barbara D'Anna, Luka Drinovec, Andrew T. Lambe, Zhe Peng, Jean-Eudes Petit, Olivier Favez, Selim Aït-Aïssa, and Alexandre Albinet
Atmos. Chem. Phys., 23, 15077–15096, https://doi.org/10.5194/acp-23-15077-2023, https://doi.org/10.5194/acp-23-15077-2023, 2023
Short summary
Short summary
Polycyclic aromatic hydrocarbons (PAHS) and furans are key precursors of secondary organic aerosols (SOAs) related to biomass burning emissions. We evaluated and compared the formation yields, and the physical and light absorption properties, of laboratory-generated SOAs from the oxidation of such compounds for both, day- and nighttime reactivities. The results illustrate that PAHs are large SOA precursors and may contribute significantly to the biomass burning brown carbon in the atmosphere.
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
Short summary
Short summary
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.
Andrew T. Lambe, Bin Bai, Masayuki Takeuchi, Nicole Orwat, Paul M. Zimmerman, Mitchell W. Alton, Nga L. Ng, Andrew Freedman, Megan S. Claflin, Drew R. Gentner, Douglas R. Worsnop, and Pengfei Liu
Atmos. Chem. Phys., 23, 13869–13882, https://doi.org/10.5194/acp-23-13869-2023, https://doi.org/10.5194/acp-23-13869-2023, 2023
Short summary
Short summary
We developed a new method to generate nitrate radicals (NO3) for atmospheric chemistry applications that works by irradiating mixtures containing ceric ammonium nitrate with a UV light at room temperature. It has several advantages over traditional NO3 sources. We characterized its performance over a range of mixture and reactor conditions as well as other irradiation products. Proof of concept was demonstrated by generating and characterizing oxidation products of the β-pinene + NO3 reaction.
Benjamin N. Murphy, Darrell Sonntag, Karl M. Seltzer, Havala O. T. Pye, Christine Allen, Evan Murray, Claudia Toro, Drew R. Gentner, Cheng Huang, Shantanu Jathar, Li Li, Andrew A. May, and Allen L. Robinson
Atmos. Chem. Phys., 23, 13469–13483, https://doi.org/10.5194/acp-23-13469-2023, https://doi.org/10.5194/acp-23-13469-2023, 2023
Short summary
Short summary
We update methods for calculating organic particle and vapor emissions from mobile sources in the USA. Conventionally, particulate matter (PM) and volatile organic carbon (VOC) are speciated without consideration of primary semivolatile emissions. Our methods integrate state-of-the-science speciation profiles and correct for common artifacts when sampling emissions in a laboratory. We quantify impacts of the emission updates on ambient pollution with the Community Multiscale Air Quality model.
Matthias Kohl, Jos Lelieveld, Sourangsu Chowdhury, Sebastian Ehrhart, Disha Sharma, Yafang Cheng, Sachchida Nand Tripathi, Mathew Sebastian, Govindan Pandithurai, Hongli Wang, and Andrea Pozzer
Atmos. Chem. Phys., 23, 13191–13215, https://doi.org/10.5194/acp-23-13191-2023, https://doi.org/10.5194/acp-23-13191-2023, 2023
Short summary
Short summary
Knowledge on atmospheric ultrafine particles (UFPs) with a diameter smaller than 100 nm is crucial for public health and the hydrological cycle. We present a new global dataset of UFP concentrations at the Earth's surface derived with a comprehensive chemistry–climate model and evaluated with ground-based observations. The evaluation results are combined with high-resolution primary emissions to downscale UFP concentrations to an unprecedented horizontal resolution of 0.1° × 0.1°.
Han Zang, Dandan Huang, Jiali Zhong, Ziyue Li, Chenxi Li, Huayun Xiao, and Yue Zhao
Atmos. Chem. Phys., 23, 12691–12705, https://doi.org/10.5194/acp-23-12691-2023, https://doi.org/10.5194/acp-23-12691-2023, 2023
Short summary
Short summary
Acylperoxy radicals (RO2) are key intermediates in the atmospheric oxidation of organic compounds, yet our knowledge of their identities and chemistry remains poor. Using direct measurements and kinetic modeling, we identify the composition and formation pathways of acyl RO2 and quantify their contribution to highly oxygenated organic molecules during α-pinene ozonolysis, which will help to understand oxidation chemistry of monoterpenes and sources of low-volatility organics in the atmosphere.
Xiaodong Xie, Jianlin Hu, Momei Qin, Song Guo, Min Hu, Dongsheng Ji, Hongli Wang, Shengrong Lou, Cheng Huang, Chong Liu, Hongliang Zhang, Qi Ying, Hong Liao, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 10563–10578, https://doi.org/10.5194/acp-23-10563-2023, https://doi.org/10.5194/acp-23-10563-2023, 2023
Short summary
Short summary
The atmospheric age of particles reflects how long particles have been formed and suspended in the atmosphere, which is closely associated with the evolution processes of particles. An analysis of the atmospheric age of PM2.5 provides a unique perspective on the evolution processes of different PM2.5 components. The results also shed lights on how to design effective emission control actions under unfavorable meteorological conditions.
Shuhui Zhu, Min Zhou, Liping Qiao, Dan Dan Huang, Qiongqiong Wang, Shan Wang, Yaqin Gao, Shengao Jing, Qian Wang, Hongli Wang, Changhong Chen, Cheng Huang, and Jian Zhen Yu
Atmos. Chem. Phys., 23, 7551–7568, https://doi.org/10.5194/acp-23-7551-2023, https://doi.org/10.5194/acp-23-7551-2023, 2023
Short summary
Short summary
Organic aerosol (OA) is increasingly important in urban PM2.5 pollution as inorganic ions are becoming lower. We investigated the chemical characteristics of OA during nine episodes in Shanghai. The availability of bi-hourly measured molecular markers revealed that the control of local urban sources such as vehicular and cooking emissions lessened the severity of local episodes. Regional control of precursors and biomass burning would reduce PM2.5 episodes influenced by regional transport.
Yaqin Gao, Hongli Wang, Lingling Yuan, Shengao Jing, Bin Yuan, Guofeng Shen, Liang Zhu, Abigail Koss, Yingjie Li, Qian Wang, Dan Dan Huang, Shuhui Zhu, Shikang Tao, Shengrong Lou, and Cheng Huang
Atmos. Chem. Phys., 23, 6633–6646, https://doi.org/10.5194/acp-23-6633-2023, https://doi.org/10.5194/acp-23-6633-2023, 2023
Short summary
Short summary
A near-complete speciation of reactive organic gases from residential combustion was developed to get more insights into their atmospheric effects. Oxygenated species, higher hydrocarbons and nitrogen-containing species played larger roles in these emissions compared with common hydrocarbons. Based on the near-complete speciation, these emissions were largely underestimated, leading to more underestimation of their hydroxyl radical reactivity and secondary organic aerosol formation potential.
Yifang Gu, Ru-Jin Huang, Jing Duan, Wei Xu, Chunshui Lin, Haobin Zhong, Ying Wang, Haiyan Ni, Quan Liu, Ruiguang Xu, Litao Wang, and Yong Jie Li
Atmos. Chem. Phys., 23, 5419–5433, https://doi.org/10.5194/acp-23-5419-2023, https://doi.org/10.5194/acp-23-5419-2023, 2023
Short summary
Short summary
Secondary organic aerosol (SOA) can be produced by various pathways, but its formation mechanisms are unclear. Observations were conducted in the North China Plain during a highly oxidizing atmosphere in summer. We found that fast photochemistry dominated SOA formation during daytime. Two types of aqueous-phase chemistry (nocturnal and daytime processing) take place at high relative humidity. The potential transformation from primary organic aerosol (POA) to SOA was also an important pathway.
Yiqun Lu, Yingge Ma, Dan Dan Huang, Shengrong Lou, Sheng'ao Jing, Yaqin Gao, Hongli Wang, Yanjun Zhang, Hui Chen, Yunhua Chang, Naiqiang Yan, Jianmin Chen, Christian George, Matthieu Riva, and Cheng Huang
Atmos. Chem. Phys., 23, 3233–3245, https://doi.org/10.5194/acp-23-3233-2023, https://doi.org/10.5194/acp-23-3233-2023, 2023
Short summary
Short summary
N-containing oxygenated organic molecules have been identified as important precursors of aerosol particles. We used an ultra-high-resolution mass spectrometer coupled with an online sample inlet to accurately measure their molecular composition, concentration level and variation patterns. We show their formation process and influencing factors in a Chinese megacity involving various volatile organic compound precursors and atmospheric oxidants, and we highlight the influence of PM2.5 episodes.
Jing Cai, Kaspar R. Daellenbach, Cheng Wu, Yan Zheng, Feixue Zheng, Wei Du, Sophie L. Haslett, Qi Chen, Markku Kulmala, and Claudia Mohr
Atmos. Meas. Tech., 16, 1147–1165, https://doi.org/10.5194/amt-16-1147-2023, https://doi.org/10.5194/amt-16-1147-2023, 2023
Short summary
Short summary
We introduce the offline application of FIGAERO-CIMS by analyzing Teflon and quartz filter samples that were collected at a typical urban site in Beijing with the deposition time varying from 30 min to 24 h. This method provides a feasible, simple, and quantitative way to investigate the molecular composition and volatility of OA compounds by using FIGAERO-CIMS to analyze offline samples.
Brix Raphael Go, Yong Jie Li, Dan Dan Huang, Yalin Wang, and Chak K. Chan
Atmos. Chem. Phys., 23, 2859–2875, https://doi.org/10.5194/acp-23-2859-2023, https://doi.org/10.5194/acp-23-2859-2023, 2023
Short summary
Short summary
We compared non-phenolic and phenolic methoxybenzaldehydes as photosensitizers for aqueous secondary organic aerosol (aqSOA) formation under cloud and fog conditions. We showed that the structural features of photosensitizers affect aqSOA formation. We also elucidated potential interactions between photosensitization and ammonium nitrate photolysis. Our findings are useful for evaluating the importance of photosensitized reactions on aqSOA formation, which could improve aqSOA predictive 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
Short summary
Short summary
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.
Jingyu An, Cheng Huang, Dandan Huang, Momei Qin, Huan Liu, Rusha Yan, Liping Qiao, Min Zhou, Yingjie Li, Shuhui Zhu, Qian Wang, and Hongli Wang
Atmos. Chem. Phys., 23, 323–344, https://doi.org/10.5194/acp-23-323-2023, https://doi.org/10.5194/acp-23-323-2023, 2023
Short summary
Short summary
This paper aims to build up an approach to establish a high-resolution emission inventory of intermediate-volatility and semi-volatile organic compounds in city-scale and detailed source categories and incorporate it into the CMAQ model. We believe this approach can be widely applied to improve the simulation of secondary organic aerosol and its source contributions.
Yarong Peng, Hongli Wang, Yaqin Gao, Shengao Jing, Shuhui Zhu, Dandan Huang, Peizhi Hao, Shengrong Lou, Tiantao Cheng, Cheng Huang, and Xuan Zhang
Atmos. Meas. Tech., 16, 15–28, https://doi.org/10.5194/amt-16-15-2023, https://doi.org/10.5194/amt-16-15-2023, 2023
Short summary
Short summary
This work examined the phase partitioning behaviors of organic compounds at hourly resolution in ambient conditions with the use of the CHemical Analysis of aeRosols ONline (CHARON) inlet coupled to a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS). Properly accounting for the neutral losses of small moieties during the molecular feature extraction from PTR mass spectra could significantly reduce uncertainties associated with the gas–particle partitioning measurements.
Min Zhou, Guangjie Zheng, Hongli Wang, Liping Qiao, Shuhui Zhu, DanDan Huang, Jingyu An, Shengrong Lou, Shikang Tao, Qian Wang, Rusha Yan, Yingge Ma, Changhong Chen, Yafang Cheng, Hang Su, and Cheng Huang
Atmos. Chem. Phys., 22, 13833–13844, https://doi.org/10.5194/acp-22-13833-2022, https://doi.org/10.5194/acp-22-13833-2022, 2022
Short summary
Short summary
The trend of aerosol pH and its drivers is crucial in understanding the multiphase formation pathways of aerosols. We reported the first trend analysis of aerosol pH from 2011 to 2019 in eastern China. Although significant variations of aerosol compositions were observed from 2011 to 2019, the aerosol pH estimated by model only slightly declined by 0.24. Our work shows that the opposite effects of SO42− and non-volatile cation changes play key roles in determining the moderate pH trend.
Yishuo Guo, Chao Yan, Yuliang Liu, Xiaohui Qiao, Feixue Zheng, Ying Zhang, Ying Zhou, Chang Li, Xiaolong Fan, Zhuohui Lin, Zemin Feng, Yusheng Zhang, Penggang Zheng, Linhui Tian, Wei Nie, Zhe Wang, Dandan Huang, Kaspar R. Daellenbach, Lei Yao, Lubna Dada, Federico Bianchi, Jingkun Jiang, Yongchun Liu, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 22, 10077–10097, https://doi.org/10.5194/acp-22-10077-2022, https://doi.org/10.5194/acp-22-10077-2022, 2022
Short summary
Short summary
Gaseous oxygenated organic molecules (OOMs) are able to form atmospheric aerosols, which will impact on human health and climate change. Here, we find that OOMs in urban Beijing are dominated by anthropogenic sources, i.e. aromatic (29 %–41 %) and aliphatic (26 %–41 %) OOMs. They are also the main contributors to the condensational growth of secondary organic aerosols (SOAs). Therefore, the restriction on anthropogenic VOCs is crucial for the reduction of SOAs and haze formation.
Sihang Wang, Bin Yuan, Caihong Wu, Chaomin Wang, Tiange Li, Xianjun He, Yibo Huangfu, Jipeng Qi, Xiao-Bing Li, Qing'e Sha, Manni Zhu, Shengrong Lou, Hongli Wang, Thomas Karl, Martin Graus, Zibing Yuan, and Min Shao
Atmos. Chem. Phys., 22, 9703–9720, https://doi.org/10.5194/acp-22-9703-2022, https://doi.org/10.5194/acp-22-9703-2022, 2022
Short summary
Short summary
Volatile organic compound (VOC) emissions from vehicles are measured using online mass spectrometers. Differences between gasoline and diesel vehicles are observed with higher emission factors of most oxygenated VOCs (OVOCs) and heavier aromatics from diesel vehicles. A higher aromatics / toluene ratio could provide good indicators to distinguish emissions from both vehicle types. We show that OVOCs account for significant contributions to VOC emissions from vehicles, especially diesel vehicles.
Wenjie Wang, David D. Parrish, Siwen Wang, Fengxia Bao, Ruijing Ni, Xin Li, Suding Yang, Hongli Wang, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 8935–8949, https://doi.org/10.5194/acp-22-8935-2022, https://doi.org/10.5194/acp-22-8935-2022, 2022
Short summary
Short summary
Tropospheric ozone is an air pollutant that is detrimental to human health, vegetation and ecosystem productivity. A comprehensive characterisation of the spatial and temporal distribution of tropospheric ozone is critical to our understanding of these issues. Here we summarise this distribution over China from the available observational records to the extent possible. This study provides insights into efficient future ozone control strategies in China.
Shijie Cui, Dan Dan Huang, Yangzhou Wu, Junfeng Wang, Fuzhen Shen, Jiukun Xian, Yunjiang Zhang, Hongli Wang, Cheng Huang, Hong Liao, and Xinlei Ge
Atmos. Chem. Phys., 22, 8073–8096, https://doi.org/10.5194/acp-22-8073-2022, https://doi.org/10.5194/acp-22-8073-2022, 2022
Short summary
Short summary
Refractory black carbon (rBC) aerosols are important to air quality and climate change. rBC can mix with many other species, which can significantly change its properties and impacts. We used a specific set of techniques to exclusively characterize rBC-containing (rBCc) particles in Shanghai. We elucidated their composition, sources and size distributions and factors that affect their properties. Our findings are very valuable for advancing the understanding of BC and controlling BC pollution.
Reza Bashiri Khuzestani, Keren Liao, Ying Liu, Ruqian Miao, Yan Zheng, Xi Cheng, Tianjiao Jia, Xin Li, Shiyi Chen, Guancong Huang, and Qi Chen
Atmos. Chem. Phys., 22, 7389–7404, https://doi.org/10.5194/acp-22-7389-2022, https://doi.org/10.5194/acp-22-7389-2022, 2022
Short summary
Short summary
This work characterized the spatial variabilities of air pollutants in a megacity by advanced mobile measurements. The results show a large spatial heterogeneity in the distributions of PM2.5 composition and volatile organic compounds under non-haze conditions, and relatively uniform spatial distributions under haze conditions that may indicate a chemical homogeneity on an intracity scale. The findings improve our understanding of urban air pollution.
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
Short summary
Short summary
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.
Haoran Zhang, Nan Li, Keqin Tang, Hong Liao, Chong Shi, Cheng Huang, Hongli Wang, Song Guo, Min Hu, Xinlei Ge, Mindong Chen, Zhenxin Liu, Huan Yu, and Jianlin Hu
Atmos. Chem. Phys., 22, 5495–5514, https://doi.org/10.5194/acp-22-5495-2022, https://doi.org/10.5194/acp-22-5495-2022, 2022
Short summary
Short summary
We developed a new algorithm with low economic/technique costs to identify primary and secondary components of PM2.5. Our model was shown to be reliable by comparison with different observation datasets. We systematically explored the patterns and changes in the secondary PM2.5 pollution in China at large spatial and time scales. We believe that this method is a promising tool for efficiently estimating primary and secondary PM2.5, and has huge potential for future PM mitigation.
Han Zang, Yue Zhao, Juntao Huo, Qianbiao Zhao, Qingyan Fu, Yusen Duan, Jingyuan Shao, Cheng Huang, Jingyu An, Likun Xue, Ziyue Li, Chenxi Li, and Huayun Xiao
Atmos. Chem. Phys., 22, 4355–4374, https://doi.org/10.5194/acp-22-4355-2022, https://doi.org/10.5194/acp-22-4355-2022, 2022
Short summary
Short summary
Particulate nitrate plays an important role in wintertime haze pollution in eastern China, yet quantitative constraints on detailed nitrate formation mechanisms remain limited. Here we quantified the contributions of the heterogeneous N2O5 hydrolysis (66 %) and gas-phase OH + NO2 reaction (32 %) to nitrate formation in this region and identified the atmospheric oxidation capacity (i.e., availability of O3 and OH radicals) as the driving factor of nitrate formation from both processes.
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
Short summary
Short summary
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.
Brix Raphael Go, Yan Lyu, Yan Ji, Yong Jie Li, Dan Dan Huang, Xue Li, Theodora Nah, Chun Ho Lam, and Chak K. Chan
Atmos. Chem. Phys., 22, 273–293, https://doi.org/10.5194/acp-22-273-2022, https://doi.org/10.5194/acp-22-273-2022, 2022
Short summary
Short summary
Biomass burning (BB) is a global phenomenon that releases large quantities of pollutants such as phenols and aromatic carbonyls into the atmosphere. These compounds can form secondary organic aerosols (SOAs) which play an important role in the Earth’s energy budget. In this work, we demonstrated that the direct irradiation of vanillin (VL) could generate aqueous SOA (aqSOA) such as oligomers. In the presence of nitrate, VL photo-oxidation can also form nitrated compounds.
Shijie Liu, Dandan Huang, Yiqian Wang, Si Zhang, Xiaodi Liu, Can Wu, Wei Du, and Gehui Wang
Atmos. Chem. Phys., 21, 17759–17773, https://doi.org/10.5194/acp-21-17759-2021, https://doi.org/10.5194/acp-21-17759-2021, 2021
Short summary
Short summary
A series of chamber experiments was performed to probe the individual and common effects of NH3 and NOx on toluene secondary organic aerosol (SOA) formation through OH photooxidation. The synergetic effects of NH3 and NOx on the toluene SOA concentration and optical absorption were observed. The higher-volatility products formed in the presence of NOx could precipitate into the particle phase when NH3 was added. The formation pathways of N-containing OAs through NOx or NH3 are also discussed.
Ruqian Miao, Qi Chen, Manish Shrivastava, Youfan Chen, Lin Zhang, Jianlin Hu, Yan Zheng, and Keren Liao
Atmos. Chem. Phys., 21, 16183–16201, https://doi.org/10.5194/acp-21-16183-2021, https://doi.org/10.5194/acp-21-16183-2021, 2021
Short summary
Short summary
We apply process-based and observation-constrained schemes to simulate organic aerosol in China and conduct comprehensive model–observation comparisons. The results show that anthropogenic semivolatile and intermediate-volatility organic compounds (SVOCs and IVOCs) are the main sources of secondary organic aerosol (SOA) in polluted regions, for which the residential sector is perhaps the predominant contributor. The hydroxyl radical level is also important for SOA modeling in polluted regions.
Cited articles
Atkinson, R. and Arey, J.: Atmospheric degradation of volatile organic compounds, Chem. Rev., 103, 4605–4638, https://doi.org/10.1021/cr0206420, 2003.
Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., Troe, J., and IUPAC Subcommittee: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume II – gas phase reactions of organic species, Atmos. Chem. Phys., 6, 3625–4055, https://doi.org/10.5194/acp-6-3625-2006, 2006.
Barmet, P., Dommen, J., DeCarlo, P. F., Tritscher, T., Praplan, A. P., Platt, S. M., Prévôt, A. S. H., Donahue, N. M., and Baltensperger, U.: OH clock determination by proton transfer reaction mass spectrometry at an environmental chamber, Atmos. Meas. Tech., 5, 647–656, https://doi.org/10.5194/amt-5-647-2012, 2012.
Burkholder, J. B., Sander, S. P., Abbatt, J. P. D., Barker, J. R., Cappa, C., Crounse, J. D., Dibble, T. S., Huie, R. E., Kolb, C. E., Kurylo, M. J., Orkin, V. L., Percival, C. J., Wilmouth, D. M., and Wine, P. H.: Chemical kinetics and photochemical data for use in atmospheric studies, Evaluation Number 19, Jet Propulsion Laboratory, National Aeronautics and Space Administration, Pasadena, CA, http://jpldataeval.jpl.nasa.gov (last access: 7 December 2024), 2020.
Cao, J., Wang, Q., Li, L., Zhang, Y., Tian, J., Chen, L. A., Ho, S. S. H., Wang, X., Chow, J. C., and Watson, J. G.: Evaluation of the oxidation flow reactor for particulate matter emission limit certification, Atmos. Environ., 224, 117086, https://doi.org/10.1016/j.atmosenv.2019.117086, 2020.
Cheng, X., Chen, Q., Jie Li, Y., Zheng, Y., Liao, K., and Huang, G.: Highly oxygenated organic molecules produced by the oxidation of benzene and toluene in a wide range of OH exposure and NOx conditions, Atmos. Chem. Phys., 21, 12005–12019, https://doi.org/10.5194/acp-21-12005-2021, 2021.
Cheng, X., Li, Y. J., Zheng, Y., Liao, K., Koenig, T. K., Ge, Y., Zhu, T., Ye, C., Qiu, X., and Chen, Q.: Oxygenated organic molecules produced by low-NOx photooxidation of aromatic compounds: contributions to secondary organic aerosol and steric hindrance, Atmos. Chem. Phys., 24, 2099–2112, https://doi.org/10.5194/acp-24-2099-2024, 2024.
Clerc, M. and Barat, F.: Kinetics of CO formation studied by far-UV flash photolysis of CO2, J. Chem. Phys., 46, 107–110, https://doi.org/10.1063/1.1840358, 1967.
Cocker, D. R., Flagan, R. C., and Seinfeld, J. H.: State-of-the-art chamber facility for studying atmospheric aerosol chemistry, Environ. Sci. Technol., 35, 2594–2601, https://doi.org/10.1021/es0019169, 2001.
Cohen, N. and Heicklen, J.: The Oxidation of Inorganic Non-metallic Compounds, in: Reactions of Non-Metallic Inorganic Compounds, Compr. Chem. Kinet., Elsevier, 1–137, https://doi.org/10.1016/s0069-8040(08)70303-0, 1972.
Ehhalt, D. H.: Photooxidation of trace gases in the troposphere Plenary Lecture, Phys. Chem. Chem. Phys., 1, 5401–5408, https://doi.org/10.1039/A905097C, 1999.
Friedman, B. and Farmer, D. K.: SOA and gas phase organic acid yields from the sequential photooxidation of seven monoterpenes, Atmos. Environ., 187, 335–345, https://doi.org/10.1016/j.atmosenv.2018.06.003, 2018.
Fuchs, H., Tan, Z., Lu, K., Bohn, B., Broch, S., Brown, S. S., Dong, H., Gomm, S., Häseler, R., He, L., Hofzumahaus, A., Holland, F., Li, X., Liu, Y., Lu, S., Min, K.-E., Rohrer, F., Shao, M., Wang, B., Wang, M., Wu, Y., Zeng, L., Zhang, Y., Wahner, A., and Zhang, Y.: OH reactivity at a rural site (Wangdu) in the North China Plain: contributions from OH reactants and experimental OH budget, Atmos. Chem. Phys., 17, 645–661, https://doi.org/10.5194/acp-17-645-2017, 2017.
George, I. J., Vlasenko, A., Slowik, J. G., Broekhuizen, K., and Abbatt, J. P. D.: Heterogeneous oxidation of saturated organic aerosols by hydroxyl radicals: uptake kinetics, condensed-phase products, and particle size change, Atmos. Chem. Phys., 7, 4187–4201, https://doi.org/10.5194/acp-7-4187-2007, 2007.
Hildebrandt, L., Donahue, N. M., and Pandis, S. N.: High formation of secondary organic aerosol from the photo-oxidation of toluene, Atmos. Chem. Phys., 9, 2973–2986, https://doi.org/10.5194/acp-9-2973-2009, 2009.
Kang, E., Root, M. J., Toohey, D. W., and Brune, W. H.: Introducing the concept of Potential Aerosol Mass (PAM), Atmos. Chem. Phys., 7, 5727–5744, https://doi.org/10.5194/acp-7-5727-2007, 2007.
Lambe, A. T., Ahern, A. T., Williams, L. R., Slowik, J. G., Wong, J. P. S., Abbatt, J. P. D., Brune, W. H., Ng, N. L., Wright, J. P., Croasdale, D. R., Worsnop, D. R., Davidovits, P., and Onasch, T. B.: Characterization of aerosol photooxidation flow reactors: heterogeneous oxidation, secondary organic aerosol formation and cloud condensation nuclei activity measurements, Atmos. Meas. Tech., 4, 445–461, https://doi.org/10.5194/amt-4-445-2011, 2011.
Li, R., Palm, B. B., Ortega, A. M., Hlywiak, J., Hu, W., Peng, Z., Day, D. A., Knote, C., Brune, W. H., and De Gouw, J. A.: Modeling the radical chemistry in an oxidation flow reactor: Radical formation and recycling, sensitivities, and the OH exposure estimation equation, J. Phys. Chem. A, 119, 4418–4432, https://doi.org/10.1021/jp509534k, 2015.
Liao, K., Chen, Q., Liu, Y., Li, Y. J., Lambe, A. T., Zhu, T., Huang, R.-J., Zheng, Y., Cheng, X., and Miao, R.: Secondary organic aerosol formation of fleet vehicle emissions in China: Potential seasonality of spatial distributions, Environ. Sci. Technol., 55, 7276–7286, https://doi.org/10.1021/acs.est.0c08591, 2021.
Liu, J., Chu, B., Chen, T., Liu, C., Wang, L., Bao, X., and He, H.: Secondary organic aerosol formation from ambient air at an urban site in Beijing: effects of OH exposure and precursor concentrations, Environ. Sci. Technol., 52, 6834–6841, https://doi.org/10.1021/acs.est.7b05701, 2018.
Liu, T., Clegg, S. L., and Abbatt, J. P.: Fast oxidation of sulfur dioxide by hydrogen peroxide in deliquesced aerosol particles, P. Natl. Acad. Sci. USA, 117, 1354–1359, 2020.
Lou, S., Holland, F., Rohrer, F., Lu, K., Bohn, B., Brauers, T., Chang, C. C., Fuchs, H., Häseler, R., Kita, K., Kondo, Y., Li, X., Shao, M., Zeng, L., Wahner, A., Zhang, Y., Wang, W., and Hofzumahaus, A.: Atmospheric OH reactivities in the Pearl River Delta – China in summer 2006: measurement and model results, Atmos. Chem. Phys., 10, 11243–11260, https://doi.org/10.5194/acp-10-11243-2010, 2010.
Lu, K., Zhang, Y., Su, H., Brauers, T., Chou, C. C., Hofzumahaus, A., Liu, S. C., Kita, K., Kondo, Y., and Shao, M.: Oxidant (O3 + NO2) production processes and formation regimes in Beijing, J. Geohys. Res.-Atmos., 115, D07303, https://doi.org/10.1029/2009JD012714, 2010.
Mao, J., Ren, X., Brune, W. H., Olson, J. R., Crawford, J. H., Fried, A., Huey, L. G., Cohen, R. C., Heikes, B., Singh, H. B., Blake, D. R., Sachse, G. W., Diskin, G. S., Hall, S. R., and Shetter, R. E.: Airborne measurement of OH reactivity during INTEX-B, Atmos. Chem. Phys., 9, 163–173, https://doi.org/10.5194/acp-9-163-2009, 2009.
Nakashima, Y., Kamei, N., Kobayashi, S., and Kajii, Y.: Total OH reactivity and VOC analyses for gasoline vehicular exhaust with a chassis dynamometer, Atmos. Environ., 44, 468–475, https://doi.org/10.1016/j.atmosenv.2009.11.006, 2010.
Ono, R., Nakagawa, Y., Tokumitsu, Y., Matsumoto, H., and Oda, T.: Effect of humidity on the production of ozone and other radicals by low-pressure mercury lamps, J. Photochem. Photobiol. A, 274, 13–19, https://doi.org/10.1016/j.jphotochem.2013.09.012, 2014.
Palm, B. B., de Sá, S. S., Day, D. A., Campuzano-Jost, P., Hu, W., Seco, R., Sjostedt, S. J., Park, J.-H., Guenther, A. B., Kim, S., Brito, J., Wurm, F., Artaxo, P., Thalman, R., Wang, J., Yee, L. D., Wernis, R., Isaacman-VanWertz, G., Goldstein, A. H., Liu, Y., Springston, S. R., Souza, R., Newburn, M. K., Alexander, M. L., Martin, S. T., and Jimenez, J. L.: Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia, Atmos. Chem. Phys., 18, 467–493, https://doi.org/10.5194/acp-18-467-2018, 2018.
Pan, T., Lambe, A. T., Hu, W., He, Y., Hu, M., Zhou, H., Wang, X., Hu, Q., Chen, H., Zhao, Y., Huang, Y., Worsnop, D. R., Peng, Z., Morris, M. A., Day, D. A., Campuzano-Jost, P., Jimenez, J.-L., and Jathar, S. H.: A comprehensive evaluation of enhanced temperature influence on gas and aerosol chemistry in the lamp-enclosed oxidation flow reactor (OFR) system, Atmos. Meas. Tech., 17, 4915–4939, https://doi.org/10.5194/amt-17-4915-2024, 2024.
Peng, Z. and Jimenez, J. L.: KinSim: a research-grade, user-friendly, visual kinetics simulator for chemical-kinetics and environmental-chemistry teaching, J. Chem. Educ, 96, 806–811, https://doi.org/10.1021/acs.jchemed.9b00033, 2019.
Peng, Z. and Jimenez, J. L.: Radical chemistry in oxidation flow reactors for atmospheric chemistry research, Chem. Soc. Rev., 49, 2570–2616, https://doi.org/10.1039/C9CS00766K, 2020.
Peng, Z., Day, D. A., Stark, H., Li, R., Lee-Taylor, J., Palm, B. B., Brune, W. H., and Jimenez, J. L.: HOx radical chemistry in oxidation flow reactors with low-pressure mercury lamps systematically examined by modeling, Atmos. Meas. Tech., 8, 4863–4890, https://doi.org/10.5194/amt-8-4863-2015, 2015.
Peng, Z., Day, D. A., Ortega, A. M., Palm, B. B., Hu, W., Stark, H., Li, R., Tsigaridis, K., Brune, W. H., and Jimenez, J. L.: Non-OH chemistry in oxidation flow reactors for the study of atmospheric chemistry systematically examined by modeling, Atmos. Chem. Phys., 16, 4283–4305, https://doi.org/10.5194/acp-16-4283-2016, 2016.
Rowe, J. P., Lambe, A. T., and Brune, W. H.: Technical Note: Effect of varying the λ= 185 and 254 nm photon flux ratio on radical generation in oxidation flow reactors, Atmos. Chem. Phys., 20, 13417–13424, https://doi.org/10.5194/acp-20-13417-2020, 2020.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics: from air pollution to climate change, John Wiley & Sons, Inc., ISBN 9781119221166, 2016.
Stone, D., Whalley, L. K., and Heard, D. E.: Tropospheric OH and HO2 radicals: field measurements and model comparisons, Chem. Soc. Rev., 41, 6348–6404, https://doi.org/10.1039/C2CS35140D, 2012.
Tan, Z., Fuchs, H., Lu, K., Hofzumahaus, A., Bohn, B., Broch, S., Dong, H., Gomm, S., Häseler, R., He, L., Holland, F., Li, X., Liu, Y., Lu, S., Rohrer, F., Shao, M., Wang, B., Wang, M., Wu, Y., Zeng, L., Zhang, Y., Wahner, A., and Zhang, Y.: Radical chemistry at a rural site (Wangdu) in the North China Plain: observation and model calculations of OH, HO2 and RO2 radicals, Atmos. Chem. Phys., 17, 663–690, https://doi.org/10.5194/acp-17-663-2017, 2017.
Tan, Z., Rohrer, F., Lu, K., Ma, X., Bohn, B., Broch, S., Dong, H., Fuchs, H., Gkatzelis, G. I., Hofzumahaus, A., Holland, F., Li, X., Liu, Y., Liu, Y., Novelli, A., Shao, M., Wang, H., Wu, Y., Zeng, L., Hu, M., Kiendler-Scharr, A., Wahner, A., and Zhang, Y.: Wintertime photochemistry in Beijing: observations of ROx radical concentrations in the North China Plain during the BEST-ONE campaign, Atmos. Chem. Phys., 18, 12391–12411, https://doi.org/10.5194/acp-18-12391-2018, 2018.
Wang, N., Zannoni, N., Ernle, L., Bekö, G., Wargocki, P., Li, M., Weschler, C. J., and Williams, J.: Total OH reactivity of emissions from humans: in situ measurement and budget analysis, Environ. Sci. Technol., 55, 149–159, https://doi.org/10.1021/acs.est.0c04206, 2020.
Wang, X., Liu, T., Bernard, F., Ding, X., Wen, S., Zhang, Y., Zhang, Z., He, Q., Lü, S., Chen, J., Saunders, S., and Yu, J.: Design and characterization of a smog chamber for studying gas-phase chemical mechanisms and aerosol formation, Atmos. Meas. Tech., 7, 301–313, https://doi.org/10.5194/amt-7-301-2014, 2014.
Yang, Y., Shao, M., Keßel, S., Li, Y., Lu, K., Lu, S., Williams, J., Zhang, Y., Zeng, L., Nölscher, A. C., Wu, Y., Wang, X., and Zheng, J.: How the OH reactivity affects the ozone production efficiency: case studies in Beijing and Heshan, China, Atmos. Chem. Phys., 17, 7127–7142, https://doi.org/10.5194/acp-17-7127-2017, 2017.
You, X., Wang, H., Goos, E., Sung, C.-J., and Klippenstein, S. J.: Reaction kinetics of CO + HO2 → products: ab initio transition state theory study with master equation modeling, J. Phys. Chem. A, 111, 4031–4042, https://doi.org/10.1021/jp067597a, 2007.
Zhang, Z., Xu, W., Lambe, A. T., Hu, W., Liu, T., and Sun, Y.: Insights Into Formation and Aging of Secondary Organic Aerosol From Oxidation Flow Reactors: A Review, Curr. Pollut. Rep., 10, 1–14, https://doi.org/10.1007/s40726-024-00309-7, 2024.
Short summary
We evaluate the applicability of empirical equations to estimate OH exposure (OHexp) in an oxidative flow reactor (OFR). The fitting parameters obtained within a narrow range of conditions can generally be extended to estimate the OHexp for wide ranges of conditions in the OFR, except for external OH reactivity, which requires new fitting. At least 20–30 data points from SO2 or CO decay with varying conditions are required to fit a set of empirical parameters that can accurately estimate OHexp.
We evaluate the applicability of empirical equations to estimate OH exposure (OHexp) in an...
Altmetrics
Final-revised paper
Preprint