Articles | Volume 23, issue 14
https://doi.org/10.5194/acp-23-8383-2023
© Author(s) 2023. 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-23-8383-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Large differences of highly oxygenated organic molecules (HOMs) and low-volatile species in secondary organic aerosols (SOAs) formed from ozonolysis of β-pinene and limonene
Dandan Liu
Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Yun Zhang
Innovation Center of Pesticide Research, Department of Applied Chemistry, College of Science, China Agricultural University, Beijing 100193, China
Institute of Chemistry, Johannes Gutenberg University, Mainz 55128, Germany
Shujun Zhong
Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Shuang Chen
Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Qiaorong Xie
Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Donghuan Zhang
Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Qiang Zhang
Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Junjun Deng
Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Libin Wu
Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Chao Ma
Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Multiphase Chemistry Department, Max Planck Institute for Chemistry, Mainz 55128, Germany
Institute of Surface Science, Helmholtz-Zentrum Hereon, Geesthacht 21502, Germany
Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Related authors
Rui Jin, Wei Hu, Peimin Duan, Ming Sheng, Dandan Liu, Ziye Huang, Mutong Niu, Libin Wu, Junjun Deng, and Pingqing Fu
Atmos. Chem. Phys., 25, 1805–1829, https://doi.org/10.5194/acp-25-1805-2025, https://doi.org/10.5194/acp-25-1805-2025, 2025
Short summary
Short summary
The metabolic capacity of atmospheric microorganisms after settling into habitats is poorly understood. We studied the molecular composition of exometabolites for cultured typical airborne microbes and traced their metabolic processes. Bacteria and fungi produce highly oxidized exometabolites and have significant variations in metabolism among different strains. These insights are pivotal for assessing the biogeochemical impacts of atmospheric microorganisms following their deposition.
Qinghao Guo, Haofei Zhang, Bo Long, Lehui Cui, Yiyang Sun, Hao Liu, Yaxin Liu, Yunting Xiao, Pingqing Fu, and Jialei Zhu
Atmos. Chem. Phys., 25, 9249–9262, https://doi.org/10.5194/acp-25-9249-2025, https://doi.org/10.5194/acp-25-9249-2025, 2025
Short summary
Short summary
Limonene, a natural compound from plants, reacts with pollutants to form airborne particles that influence air quality and climate. Using advanced models with explicit chemical mechanisms, we show how different reaction pathways shape organonitrate formation, with some increasing and others decreasing particle levels. This approach enhances predictions of pollution and climate impacts while deepening our understanding of how natural and human-made emissions interact in the atmosphere.
Shubin Li, Yujue Wang, Yiwen Zhang, Yizhe Yi, Yuchen Wang, Yuqi Guo, Chao Yu, Yue Jiang, Jinhui Shi, Chao Zhang, Jialei Zhu, Wei Hu, Jianzhen Yu, Xiaohong Yao, Huiwang Gao, and Min Hu
EGUsphere, https://doi.org/10.5194/egusphere-2025-2154, https://doi.org/10.5194/egusphere-2025-2154, 2025
Short summary
Short summary
Organosulfates (OSs) are an unrecognized and potentially important component in marine organic aerosols. In this study, we quantified and characterized the OSs over East Asian marginal seas. The chemical nature and spatiotemporal distribution of OSs were modified by the joint influence of marine emissions and transported terrestrial pollutants. The results highlight the vital roles of OSs in shaping organic aerosol formation and sulfur cycle during summer in marine boundary layer.
Wenxin Zhang, Wei Hu, Mutong Niu, Quanfei Zhu, Na An, Qiang Zhang, Rui Jin, Xiaoli Fu, Jian Hao, Jianbo Yang, Jingle Liu, Jing Shi, Suqin Han, Junjun Deng, Libin Wu, Yuqi Feng, Kimitaka Kawamura, and Pingqing Fu
EGUsphere, https://doi.org/10.5194/egusphere-2025-2269, https://doi.org/10.5194/egusphere-2025-2269, 2025
Short summary
Short summary
This study investigated airborne endotoxins varying with height and season in northern China. By analyzing specific hydroxy fatty acids in aerosols, we estimated endotoxins at ground level and higher altitudes. Higher concentrations were observed near the ground during winter, likely driven by microbial emissions and combustion sources. Our findings suggest that air pollution and meteorological factors can influence endotoxin concentrations, posing potential health risks in urban environments.
Hanzheng Zhu, Yaman Liu, Man Yue, Shihui Feng, Pingqing Fu, Kan Huang, Xinyi Dong, and Minghuai Wang
Atmos. Chem. Phys., 25, 5175–5197, https://doi.org/10.5194/acp-25-5175-2025, https://doi.org/10.5194/acp-25-5175-2025, 2025
Short summary
Short summary
Dust-soluble iron deposition from East Asia plays an important role in the marine ecology of the Northwest Pacific. Using the developed model, our findings highlight a dual trend: a decrease in the overall deposition of soluble iron from dust but an increase in the solubility of the iron itself due to the enhanced atmospheric processing. The study underscores the critical roles of both dust emission and atmospheric processing in soluble iron deposition and marine ecology.
Mingyu Li, Zhanjie Xu, Zhichao Dong, Junjun Deng, Pingqing Fu, and Chandra Mouli Pavuluri
EGUsphere, https://doi.org/10.5194/egusphere-2025-1335, https://doi.org/10.5194/egusphere-2025-1335, 2025
Short summary
Short summary
This study investigated the seasonal and diurnal variability of fine aerosol composition in two forest ecosystems in North and South China. Carbonaceous/nitrogenous compound concentrations were higher in winter than summer at both sites. The forest fine aerosols in high latitude exhibited significantly greater influence from fossil fuel combustion compared to that in low latitude.
Zhichao Dong, Subba Rao Devineni, Xiaoli Fu, Zhanjie Xu, Mingyu Li, Pingqing Fu, Cong-Qiang Liu, and Chandra Mouli Pavuluri
EGUsphere, https://doi.org/10.5194/egusphere-2025-899, https://doi.org/10.5194/egusphere-2025-899, 2025
Preprint archived
Short summary
Short summary
We developed new method to detect and measure organosulfates in PM2.5. By synthesizing organosulfates and combining them with commercial standards, we improved detection accuracy. Testing air samples from Tianjin, China, we found wintertime levels of organosulfates were much higher than in other regions. Our results show how human actions directly impact air quality and provide a tool to track pollution sources. This work helps scientists understand and address harmful aerosols in environments.
Yaxin Liu, Yunting Xiao, Lehui Cui, Qinghao Guo, Yiyang Sun, Pingqing Fu, Cong-Qiang Liu, and Jialei Zhu
EGUsphere, https://doi.org/10.5194/egusphere-2025-763, https://doi.org/10.5194/egusphere-2025-763, 2025
Short summary
Short summary
Dust carries iron deposits into the ocean, providing essential nutrients for the growth of marine phytoplankton, influencing their carbon uptake capacity. A model constrained by global datasets on dust iron content, ocean iron solubility, and dissolved iron concentrations was used to assess the contributions of 11 major dust sources to carbon uptake in 8 marine areas, enhancing understanding of the impact of global dust emissions on marine deposition and carbon cycle with decreased uncertainty.
Rui Jin, Wei Hu, Peimin Duan, Ming Sheng, Dandan Liu, Ziye Huang, Mutong Niu, Libin Wu, Junjun Deng, and Pingqing Fu
Atmos. Chem. Phys., 25, 1805–1829, https://doi.org/10.5194/acp-25-1805-2025, https://doi.org/10.5194/acp-25-1805-2025, 2025
Short summary
Short summary
The metabolic capacity of atmospheric microorganisms after settling into habitats is poorly understood. We studied the molecular composition of exometabolites for cultured typical airborne microbes and traced their metabolic processes. Bacteria and fungi produce highly oxidized exometabolites and have significant variations in metabolism among different strains. These insights are pivotal for assessing the biogeochemical impacts of atmospheric microorganisms following their deposition.
Hongyi Li, Ting Yang, Lars Nerger, Dawei Zhang, Di Zhang, Guigang Tang, Haibo Wang, Yele Sun, Pingqing Fu, Hang Su, and Zifa Wang
Geosci. Model Dev., 17, 8495–8519, https://doi.org/10.5194/gmd-17-8495-2024, https://doi.org/10.5194/gmd-17-8495-2024, 2024
Short summary
Short summary
To accurately characterize the spatiotemporal distribution of particulate matter <2.5 µm chemical components, we developed the Nested Air Quality Prediction Model System with the Parallel Data Assimilation Framework (NAQPMS-PDAF) v2.0 for chemical components with non-Gaussian and nonlinear properties. NAQPMS-PDAF v2.0 has better computing efficiency, excels when used with a small ensemble size, and can significantly improve the simulation performance of chemical components.
Xu Yang, Fobang Liu, Shuqi Yang, Yuling Yang, Yanan Wang, Jingjing Li, Mingyu Zhao, Zhao Wang, Kai Wang, Chi He, and Haijie Tong
Atmos. Chem. Phys., 24, 11029–11043, https://doi.org/10.5194/acp-24-11029-2024, https://doi.org/10.5194/acp-24-11029-2024, 2024
Short summary
Short summary
A study in the rural North China Plain showed environmentally persistent free radicals (EPFRs) in atmospheric particulate matter (PM), with a notable water-soluble fraction likely from atmospheric oxidation during transport. Significant positive correlations between EPFRs and the water-soluble oxidative potential of PM2.5 were found, primarily attributable to the water-soluble fractions of EPFRs. These findings emphasize understanding EPFRs' atmospheric evolution for climate and health impacts.
Zhichao Dong, Chandra Mouli Pavuluri, Peisen Li, Zhanjie Xu, Junjun Deng, Xueyan Zhao, Xiaomai Zhao, Pingqing Fu, and Cong-Qiang Liu
Atmos. Chem. Phys., 24, 5887–5905, https://doi.org/10.5194/acp-24-5887-2024, https://doi.org/10.5194/acp-24-5887-2024, 2024
Short summary
Short summary
Comprehensive study of optical properties of brown carbon (BrC) in fine aerosols from Tianjin, China, implied that biological emissions are major sources of BrC in summer, whereas fossil fuel combustion and biomass burning emissions are in cold periods. The direct radiation absorption caused by BrC in short wavelengths contributed about 40 % to that caused by BrC in 300–700 nm. Water-insoluble but methanol-soluble BrC contains more protein-like chromophores (PLOM) than that of water-soluble BrC.
Jiawei Li, Zhiwei Han, Pingqing Fu, Xiaohong Yao, and Mingjie Liang
Atmos. Chem. Phys., 24, 3129–3161, https://doi.org/10.5194/acp-24-3129-2024, https://doi.org/10.5194/acp-24-3129-2024, 2024
Short summary
Short summary
Organic aerosols of marine origin are important for aerosol climatic effects but are poorly understood. For the first time, an online coupled regional chemistry–climate model is applied to explore the characteristics of emission, distribution, and direct and indirect radiative effects of marine organic aerosols over the western Pacific, which reveals an important role of marine organic aerosols in perturbing cloud and radiation and promotes understanding of global aerosol climatic impact.
Mutong Niu, Shu Huang, Wei Hu, Yajie Wang, Wanyun Xu, Wan Wei, Qiang Zhang, Zihan Wang, Donghuan Zhang, Rui Jin, Libin Wu, Junjun Deng, Fangxia Shen, and Pingqing Fu
Biogeosciences, 20, 4915–4930, https://doi.org/10.5194/bg-20-4915-2023, https://doi.org/10.5194/bg-20-4915-2023, 2023
Short summary
Short summary
Sugar compounds in air can trace the source of bioaerosols that affect public health and climate. In rural north China, we observed increased fungal activity at night and less variable bacterial community diversity. Certain night-increasing sugar compounds were more closely related to fungi than bacteria. The fungal community greatly influenced sugar compounds, while bacteria played a limited role. Caution is advised when using sugar compounds to trace airborne microbes, particularly bacteria.
Lehui Cui, Yunting Xiao, Wei Hu, Lei Song, Yujue Wang, Chao Zhang, Pingqing Fu, and Jialei Zhu
Earth Syst. Sci. Data, 15, 5403–5425, https://doi.org/10.5194/essd-15-5403-2023, https://doi.org/10.5194/essd-15-5403-2023, 2023
Short summary
Short summary
Isoprene is a crucial non-methane biogenic volatile organic compound with the largest global emissions, which has high chemical reactivity and serves as the primary source of natural secondary organic aerosols. This study built a module to present a 20-year global hourly dataset of marine phytoplankton-generated biological and photochemistry-generated isoprene emissions in the sea microlayers based on the latest advancements in biological, physical, and chemical processes.
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
Short summary
Short summary
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.
Li Wu, Hyo-Jin Eom, Hanjin Yoo, Dhrubajyoti Gupta, Hye-Rin Cho, Pingqing Fu, and Chul-Un Ro
Atmos. Chem. Phys., 23, 12571–12588, https://doi.org/10.5194/acp-23-12571-2023, https://doi.org/10.5194/acp-23-12571-2023, 2023
Short summary
Short summary
Hygroscopicity of ambient marine aerosols is of critical relevance to investigate their atmospheric impacts, which, however, remain uncertain due to their complex compositions and mixing states. Therefore, a study on the hygroscopic behavior of ambient marine aerosols for understanding the phase states when interacting with water vapor at different RH levels and their subsequent impacts on the heterogeneous chemical reactions, atmospheric environment, and human health is of vital importance.
Qi Yuan, Yuanyuan Wang, Yixin Chen, Siyao Yue, Jian Zhang, Yinxiao Zhang, Liang Xu, Wei Hu, Dantong Liu, Pingqing Fu, Huiwang Gao, and Weijun Li
Atmos. Chem. Phys., 23, 9385–9399, https://doi.org/10.5194/acp-23-9385-2023, https://doi.org/10.5194/acp-23-9385-2023, 2023
Short summary
Short summary
This study for the first time found large amounts of liquid–liquid phase separation particles with soot redistributing in organic coatings instead of sulfate cores in the eastern Tibetan Plateau atmosphere. The particle size and the ratio of the organic matter coating thickness to soot size are two of the major possible factors that likely affect the soot redistribution process. The soot redistribution process promoted the morphological compaction of soot particles.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Yele Sun, Pingqing Fu, Meng Gao, Huangjian Wu, Miaomiao Lu, Qian Wu, Shuyuan Huang, Wenxuan Sui, Jie Li, Xiaole Pan, Lin Wu, Hajime Akimoto, and Gregory R. Carmichael
Atmos. Chem. Phys., 23, 6217–6240, https://doi.org/10.5194/acp-23-6217-2023, https://doi.org/10.5194/acp-23-6217-2023, 2023
Short summary
Short summary
A multi-air-pollutant inversion system has been developed in this study to estimate emission changes in China during COVID-19 lockdown. The results demonstrate that the lockdown is largely a nationwide road traffic control measure with NOx emissions decreasing by ~40 %. Emissions of other species only decreased by ~10 % due to smaller effects of lockdown on other sectors. Assessment results further indicate that the lockdown only had limited effects on the control of PM2.5 and O3 in China.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
Short summary
Short summary
The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Zhichao Dong, Chandra Mouli Pavuluri, Zhanjie Xu, Yu Wang, Peisen Li, Pingqing Fu, and Cong-Qiang Liu
Atmos. Chem. Phys., 23, 2119–2143, https://doi.org/10.5194/acp-23-2119-2023, https://doi.org/10.5194/acp-23-2119-2023, 2023
Short summary
Short summary
This study has provided comprehensive baseline data of carbonaceous and inorganic aerosols as well as their isotope ratios in the Tianjin region, North China, found that Tianjin aerosols were derived from coal combustion, biomass burning and photochemical reactions of VOCs, and also implied that the Tianjin aerosols were more aged during long-range atmospheric transport in summer via carbonaceous and isotope data analysis.
Shujun Zhong, Shuang Chen, Junjun Deng, Yanbing Fan, Qiang Zhang, Qiaorong Xie, Yulin Qi, Wei Hu, Libin Wu, Xiaodong Li, Chandra Mouli Pavuluri, Jialei Zhu, Xin Wang, Di Liu, Xiaole Pan, Yele Sun, Zifa Wang, Yisheng Xu, Haijie Tong, Hang Su, Yafang Cheng, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 23, 2061–2077, https://doi.org/10.5194/acp-23-2061-2023, https://doi.org/10.5194/acp-23-2061-2023, 2023
Short summary
Short summary
This study investigated the role of the secondary organic aerosol (SOA) loading on the molecular composition of wintertime urban aerosols by ultrahigh-resolution mass spectrometry. Results demonstrate that the SOA loading is an important factor associated with the oxidation degree, nitrate group content, and chemodiversity of nitrooxy–organosulfates. Our study also found that the hydrolysis of nitrooxy–organosulfates is a possible pathway for the formation of organosulfates.
Xiaoying Niu, Wei Pu, Pingqing Fu, Yang Chen, Yuxuan Xing, Dongyou Wu, Ziqi Chen, Tenglong Shi, Yue Zhou, Hui Wen, and Xin Wang
Atmos. Chem. Phys., 22, 14075–14094, https://doi.org/10.5194/acp-22-14075-2022, https://doi.org/10.5194/acp-22-14075-2022, 2022
Short summary
Short summary
In this study, we do the first investigation of WSOC in seasonal snow of northeastern China. The results revealed the regional-specific compositions and sources of WSOC due to different natural environments and anthropogenic activities. The abundant concentrations of WSOC and its absorption properties contributed to a crucial impact on the snow albedo and radiative effect. We established that our study could raise awareness of carbon cycling processes, hydrological processes, and climate change.
Meng Wang, Yusen Duan, Wei Xu, Qiyuan Wang, Zhuozhi Zhang, Qi Yuan, Xinwei Li, Shuwen Han, Haijie Tong, Juntao Huo, Jia Chen, Shan Gao, Zhongbiao Wu, Long Cui, Yu Huang, Guangli Xiu, Junji Cao, Qingyan Fu, and Shun-cheng Lee
Atmos. Chem. Phys., 22, 12789–12802, https://doi.org/10.5194/acp-22-12789-2022, https://doi.org/10.5194/acp-22-12789-2022, 2022
Short summary
Short summary
In this study, we report the long-term measurement of organic carbon (OC) and elementary carbon (EC) in PM2.5 with hourly time resolution conducted at a regional site in Shanghai from 2016 to 2020. The results from this study provide critical information about the long-term trend of carbonaceous aerosol, in particular secondary OC, in one of the largest megacities in the world and are helpful for developing pollution control measures from a long-term planning perspective.
Zhiqiang Zhang, Yele Sun, Chun Chen, Bo You, Aodong Du, Weiqi Xu, Yan Li, Zhijie Li, Lu Lei, Wei Zhou, Jiaxing Sun, Yanmei Qiu, Lianfang Wei, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 22, 10409–10423, https://doi.org/10.5194/acp-22-10409-2022, https://doi.org/10.5194/acp-22-10409-2022, 2022
Short summary
Short summary
We present a comprehensive characterization of water-soluble organic aerosol and the first mass spectral characterization of water-insoluble organic aerosol in the cold season in Beijing by integrating online and offline aerosol mass spectrometer measurements. WSOA comprised dominantly secondary OA and showed large changes during the transition season from autumn to winter. WIOA was characterized by prominent hydrocarbon ions series, low oxidation states, and significant day–night differences.
Jiaxing Sun, Yele Sun, Conghui Xie, Weiqi Xu, Chun Chen, Zhe Wang, Lei Li, Xubing Du, Fugui Huang, Yan Li, Zhijie Li, Xiaole Pan, Nan Ma, Wanyun Xu, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 22, 7619–7630, https://doi.org/10.5194/acp-22-7619-2022, https://doi.org/10.5194/acp-22-7619-2022, 2022
Short summary
Short summary
We analyzed the chemical composition and mixing state of BC-containing particles at urban and rural sites in winter in the North China Plain and evaluated their impact on light absorption enhancement. BC was dominantly mixed with organic carbon, nitrate, and sulfate, and the mixing state evolved significantly as a function of relative humidity (RH) at both sites. The absorption enhancement depended strongly on coated secondary inorganic aerosol and was up to ~1.3–1.4 during aging processes.
Junjun Deng, Hao Ma, Xinfeng Wang, Shujun Zhong, Zhimin Zhang, Jialei Zhu, Yanbing Fan, Wei Hu, Libin Wu, Xiaodong Li, Lujie Ren, Chandra Mouli Pavuluri, Xiaole Pan, Yele Sun, Zifa Wang, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 22, 6449–6470, https://doi.org/10.5194/acp-22-6449-2022, https://doi.org/10.5194/acp-22-6449-2022, 2022
Short summary
Short summary
Light-absorbing brown carbon (BrC) plays an important role in climate change and atmospheric chemistry. Here we investigated the seasonal and diurnal variations in water-soluble BrC in PM2.5 in the megacity Tianjin in coastal China. Results of the source apportionments from the combination with organic molecular compositions and optical properties of water-soluble BrC reveal a large contribution from primary bioaerosol particles to BrC in the urban atmosphere.
Yanhong Zhu, Weijun Li, Yue Wang, Jian Zhang, Lei Liu, Liang Xu, Jingsha Xu, Jinhui Shi, Longyi Shao, Pingqing Fu, Daizhou Zhang, and Zongbo Shi
Atmos. Chem. Phys., 22, 2191–2202, https://doi.org/10.5194/acp-22-2191-2022, https://doi.org/10.5194/acp-22-2191-2022, 2022
Short summary
Short summary
The solubilities of iron in fine particles in a megacity in Eastern China were studied under haze, fog, dust, clear, and rain weather conditions. For the first time, a receptor model was used to quantify the sources of dissolved and total iron aerosol. Microscopic analysis further confirmed the aging of iron aerosol during haze and fog conditions that facilitated dissolution of insoluble iron.
Yaqing Zhou, Nan Ma, Qiaoqiao Wang, Zhibin Wang, Chunrong Chen, Jiangchuan Tao, Juan Hong, Long Peng, Yao He, Linhong Xie, Shaowen Zhu, Yuxuan Zhang, Guo Li, Wanyun Xu, Peng Cheng, Uwe Kuhn, Guangsheng Zhou, Pingqing Fu, Qiang Zhang, Hang Su, and Yafang Cheng
Atmos. Chem. Phys., 22, 2029–2047, https://doi.org/10.5194/acp-22-2029-2022, https://doi.org/10.5194/acp-22-2029-2022, 2022
Short summary
Short summary
This study characterizes size-resolved particle effective densities and their evolution associated with emissions and aging processes in a rural area of the North China Plain. Particle effective density exhibits a high-frequency bimodal distribution, and two density modes exhibit opposite trends with increasing particle size. SIA and BC mass fractions are key factors of particle effective density, and a value of 0.6 g cm−3 is appropriate to represent BC effective density in bulk particles.
Jiaxing Sun, Zhe Wang, Wei Zhou, Conghui Xie, Cheng Wu, Chun Chen, Tingting Han, Qingqing Wang, Zhijie Li, Jie Li, Pingqing Fu, Zifa Wang, and Yele Sun
Atmos. Chem. Phys., 22, 561–575, https://doi.org/10.5194/acp-22-561-2022, https://doi.org/10.5194/acp-22-561-2022, 2022
Short summary
Short summary
We analyzed 9-year measurements of BC and aerosol optical properties from 2012 to 2020 in Beijing, China. Our results showed large reductions in BC and light extinction coefficient due to the Clean Air Action Plan. As a response, both SSA and mass extinction efficiency (MEE) showed considerable increases, demonstrating a future challenge in visibility improvement. The primary and secondary BrC was also separated and quantified, and the changes in radiative forcing of BC and BrC were estimated.
Yuting Zhang, Hang Liu, Shandong Lei, Wanyun Xu, Yu Tian, Weijie Yao, Xiaoyong Liu, Qi Liao, Jie Li, Chun Chen, Yele Sun, Pingqing Fu, Jinyuan Xin, Junji Cao, Xiaole Pan, and Zifa Wang
Atmos. Chem. Phys., 21, 17631–17648, https://doi.org/10.5194/acp-21-17631-2021, https://doi.org/10.5194/acp-21-17631-2021, 2021
Short summary
Short summary
In this study, the authors used a single-particle soot photometer (SP2) to characterize the particle size, mixing state, and optical properties of black carbon aerosols in rural areas of the North China Plain in winter. Relatively warm and high-RH environments (RH > 50 %, −4° < T < 4 °) were more favorable to rBC aging than dry and cold environments (RH < 60 %, T < −8°). The paper emphasizes the importance of meteorological parameters in the mixing state of black carbon.
Deepchandra Srivastava, Jingsha Xu, Tuan V. Vu, Di Liu, Linjie Li, Pingqing Fu, Siqi Hou, Natalia Moreno Palmerola, Zongbo Shi, and Roy M. Harrison
Atmos. Chem. Phys., 21, 14703–14724, https://doi.org/10.5194/acp-21-14703-2021, https://doi.org/10.5194/acp-21-14703-2021, 2021
Short summary
Short summary
This study presents the source apportionment of PM2.5 performed by positive matrix factorization (PMF) at urban and rural sites in Beijing. These factors are interpreted as traffic emissions, biomass burning, road and soil dust, coal and oil combustion, and secondary inorganics. PMF failed to resolve some sources identified by CMB and AMS and appears to overestimate the dust sources. Comparison with earlier PMF studies from the Beijing area highlights inconsistent findings using this method.
Michael Biggart, Jenny Stocker, Ruth M. Doherty, Oliver Wild, David Carruthers, Sue Grimmond, Yiqun Han, Pingqing Fu, and Simone Kotthaus
Atmos. Chem. Phys., 21, 13687–13711, https://doi.org/10.5194/acp-21-13687-2021, https://doi.org/10.5194/acp-21-13687-2021, 2021
Short summary
Short summary
Heat-related illnesses are of increasing concern in China given its rapid urbanisation and our ever-warming climate. We examine the relative impacts that land surface properties and anthropogenic heat have on the urban heat island (UHI) in Beijing using ADMS-Urban. Air temperature measurements and satellite-derived land surface temperatures provide valuable means of evaluating modelled spatiotemporal variations. This work provides critical information for urban planners and UHI mitigation.
Hong Ren, Wei Hu, Lianfang Wei, Siyao Yue, Jian Zhao, Linjie Li, Libin Wu, Wanyu Zhao, Lujie Ren, Mingjie Kang, Qiaorong Xie, Sihui Su, Xiaole Pan, Zifa Wang, Yele Sun, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 21, 12949–12963, https://doi.org/10.5194/acp-21-12949-2021, https://doi.org/10.5194/acp-21-12949-2021, 2021
Short summary
Short summary
This study presents vertical profiles of biogenic and anthropogenic secondary organic aerosols (SOAs) in the urban boundary layer based on a 325 m tower in Beijing in late summer. The increases in the isoprene and toluene SOAs with height were found to be more related to regional transport, whereas the decrease in those from monoterpenes and sesquiterpene were more subject to local emissions. Such complicated vertical distributions of SOA should be considered in future modeling work.
Qiaorong Xie, Sihui Su, Jing Chen, Yuqing Dai, Siyao Yue, Hang Su, Haijie Tong, Wanyu Zhao, Lujie Ren, Yisheng Xu, Dong Cao, Ying Li, Yele Sun, Zifa Wang, Cong-Qiang Liu, Kimitaka Kawamura, Guibin Jiang, Yafang Cheng, and Pingqing Fu
Atmos. Chem. Phys., 21, 11453–11465, https://doi.org/10.5194/acp-21-11453-2021, https://doi.org/10.5194/acp-21-11453-2021, 2021
Short summary
Short summary
This study investigated the role of nighttime chemistry during Chinese New Year's Eve that enhances the formation of nitrooxy organosulfates in the aerosol phase. Results show that anthropogenic precursors, together with biogenic ones, considerably contribute to the formation of low-volatility nitrooxy OSs. Our study provides detailed molecular composition of firework-related aerosols, which gives new insights into the physicochemical properties and potential health effects of urban aerosols.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
Short summary
Short summary
We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Siqi Hou, Di Liu, Jingsha Xu, Tuan V. Vu, Xuefang Wu, Deepchandra Srivastava, Pingqing Fu, Linjie Li, Yele Sun, Athanasia Vlachou, Vaios Moschos, Gary Salazar, Sönke Szidat, André S. H. Prévôt, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 8273–8292, https://doi.org/10.5194/acp-21-8273-2021, https://doi.org/10.5194/acp-21-8273-2021, 2021
Short summary
Short summary
This study provides a newly developed method which combines radiocarbon (14C) with organic tracers to enable source apportionment of primary and secondary fossil vs. non-fossil sources of carbonaceous aerosols at an urban and a rural site of Beijing. The source apportionment results were compared with those by chemical mass balance and AMS/ACSM-PMF methods. Correlations of WINSOC and WSOC with different sources of OC were also performed to elucidate the formation mechanisms of SOC.
Jingsha Xu, Di Liu, Xuefang Wu, Tuan V. Vu, Yanli Zhang, Pingqing Fu, Yele Sun, Weiqi Xu, Bo Zheng, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 7321–7341, https://doi.org/10.5194/acp-21-7321-2021, https://doi.org/10.5194/acp-21-7321-2021, 2021
Short summary
Short summary
Source apportionment of fine aerosols in an urban site of Beijing used a chemical mass balance (CMB) model. Seven primary sources (industrial/residential coal burning, biomass burning, gasoline/diesel vehicles, cooking and vegetative detritus) explained an average of 75.7 % and 56.1 % of fine OC in winter and summer, respectively. CMB was found to resolve more primary OA sources than AMS-PMF, but the latter apportioned more secondary OA sources.
Philippe Massicotte, Rainer M. W. Amon, David Antoine, Philippe Archambault, Sergio Balzano, Simon Bélanger, Ronald Benner, Dominique Boeuf, Annick Bricaud, Flavienne Bruyant, Gwenaëlle Chaillou, Malik Chami, Bruno Charrière, Jing Chen, Hervé Claustre, Pierre Coupel, Nicole Delsaut, David Doxaran, Jens Ehn, Cédric Fichot, Marie-Hélène Forget, Pingqing Fu, Jonathan Gagnon, Nicole Garcia, Beat Gasser, Jean-François Ghiglione, Gaby Gorsky, Michel Gosselin, Priscillia Gourvil, Yves Gratton, Pascal Guillot, Hermann J. Heipieper, Serge Heussner, Stanford B. Hooker, Yannick Huot, Christian Jeanthon, Wade Jeffrey, Fabien Joux, Kimitaka Kawamura, Bruno Lansard, Edouard Leymarie, Heike Link, Connie Lovejoy, Claudie Marec, Dominique Marie, Johannie Martin, Jacobo Martín, Guillaume Massé, Atsushi Matsuoka, Vanessa McKague, Alexandre Mignot, William L. Miller, Juan-Carlos Miquel, Alfonso Mucci, Kaori Ono, Eva Ortega-Retuerta, Christos Panagiotopoulos, Tim Papakyriakou, Marc Picheral, Louis Prieur, Patrick Raimbault, Joséphine Ras, Rick A. Reynolds, André Rochon, Jean-François Rontani, Catherine Schmechtig, Sabine Schmidt, Richard Sempéré, Yuan Shen, Guisheng Song, Dariusz Stramski, Eri Tachibana, Alexandre Thirouard, Imma Tolosa, Jean-Éric Tremblay, Mickael Vaïtilingom, Daniel Vaulot, Frédéric Vaultier, John K. Volkman, Huixiang Xie, Guangming Zheng, and Marcel Babin
Earth Syst. Sci. Data, 13, 1561–1592, https://doi.org/10.5194/essd-13-1561-2021, https://doi.org/10.5194/essd-13-1561-2021, 2021
Short summary
Short summary
The MALINA oceanographic expedition was conducted in the Mackenzie River and the Beaufort Sea systems. The sampling was performed across seven shelf–basin transects to capture the meridional gradient between the estuary and the open ocean. The main goal of this research program was to better understand how processes such as primary production are influencing the fate of organic matter originating from the surrounding terrestrial landscape during its transition toward the Arctic Ocean.
Steven J. Campbell, Kate Wolfer, Battist Utinger, Joe Westwood, Zhi-Hui Zhang, Nicolas Bukowiecki, Sarah S. Steimer, Tuan V. Vu, Jingsha Xu, Nicholas Straw, Steven Thomson, Atallah Elzein, Yele Sun, Di Liu, Linjie Li, Pingqing Fu, Alastair C. Lewis, Roy M. Harrison, William J. Bloss, Miranda Loh, Mark R. Miller, Zongbo Shi, and Markus Kalberer
Atmos. Chem. Phys., 21, 5549–5573, https://doi.org/10.5194/acp-21-5549-2021, https://doi.org/10.5194/acp-21-5549-2021, 2021
Short summary
Short summary
In this study, we quantify PM2.5 oxidative potential (OP), a metric widely suggested as a potential measure of particle toxicity, in Beijing in summer and winter using four acellular assays. We correlate PM2.5 OP with a comprehensive range of atmospheric and particle composition measurements, demonstrating inter-assay differences and seasonal variation of PM2.5 OP. Using multivariate statistical analysis, we highlight specific particle chemical components and sources that influence OP.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
Short summary
Short summary
Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Santosh Kumar Verma, Kimitaka Kawamura, Fei Yang, Pingqing Fu, Yugo Kanaya, and Zifa Wang
Atmos. Chem. Phys., 21, 4959–4978, https://doi.org/10.5194/acp-21-4959-2021, https://doi.org/10.5194/acp-21-4959-2021, 2021
Short summary
Short summary
We studied aerosol samples collected in autumn 2007 with day and night intervals in a rural site of Mangshan, north of Beijing, for sugar compounds (SCs) that are abundant organic aerosol components and can influence the air quality and climate. We found higher concentrations of biomass burning (BB) products at nighttime than daytime, whereas pollen tracers and other SCs showed an opposite diurnal trend, because this site is meteorologically characterized by a mountain/valley breeze.
Lei Liu, Jian Zhang, Yinxiao Zhang, Yuanyuan Wang, Liang Xu, Qi Yuan, Dantong Liu, Yele Sun, Pingqing Fu, Zongbo Shi, and Weijun Li
Atmos. Chem. Phys., 21, 2251–2265, https://doi.org/10.5194/acp-21-2251-2021, https://doi.org/10.5194/acp-21-2251-2021, 2021
Short summary
Short summary
We found that large numbers of light-absorbing primary organic particles with high viscosity, especially tarballs, from domestic coal and biomass burning occurred in rural and even urban hazes in the winter of North China. For the first time, we characterized the atmospheric aging process of these burning-related primary organic particles by microscopic analysis and further evaluated their light absorption enhancement resulting from the “lensing effect” of secondary inorganic coatings.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
Short summary
Short summary
To understand how emission controls will impact ozone, an understanding of the sources and sinks of OH and the chemical cycling between peroxy radicals is needed. This paper presents measurements of OH, HO2 and total RO2 taken in central Beijing. The radical observations are compared to a detailed chemistry model, which shows that under low NO conditions, there is a missing OH source. Under high NOx conditions, the model under-predicts RO2 and impacts our ability to model ozone.
Rutambhara Joshi, Dantong Liu, Eiko Nemitz, Ben Langford, Neil Mullinger, Freya Squires, James Lee, Yunfei Wu, Xiaole Pan, Pingqing Fu, Simone Kotthaus, Sue Grimmond, Qiang Zhang, Ruili Wu, Oliver Wild, Michael Flynn, Hugh Coe, and James Allan
Atmos. Chem. Phys., 21, 147–162, https://doi.org/10.5194/acp-21-147-2021, https://doi.org/10.5194/acp-21-147-2021, 2021
Short summary
Short summary
Black carbon (BC) is a component of particulate matter which has significant effects on climate and human health. Sources of BC include biomass burning, transport, industry and domestic cooking and heating. In this study, we measured BC emissions in Beijing, finding a dominance of traffic emissions over all other sources. The quantitative method presented here has benefits for revising widely used emissions inventories and for understanding BC sources with impacts on air quality and climate.
W. Joe F. Acton, Zhonghui Huang, Brian Davison, Will S. Drysdale, Pingqing Fu, Michael Hollaway, Ben Langford, James Lee, Yanhui Liu, Stefan Metzger, Neil Mullinger, Eiko Nemitz, Claire E. Reeves, Freya A. Squires, Adam R. Vaughan, Xinming Wang, Zhaoyi Wang, Oliver Wild, Qiang Zhang, Yanli Zhang, and C. Nicholas Hewitt
Atmos. Chem. Phys., 20, 15101–15125, https://doi.org/10.5194/acp-20-15101-2020, https://doi.org/10.5194/acp-20-15101-2020, 2020
Short summary
Short summary
Air quality in Beijing is of concern to both policy makers and the general public. In order to address concerns about air quality it is vital that the sources of atmospheric pollutants are understood. This work presents the first top-down measurement of volatile organic compound (VOC) emissions in Beijing. These measurements are used to evaluate the emissions inventory and assess the impact of VOC emission from the city centre on atmospheric chemistry.
Eloise J. Slater, Lisa K. Whalley, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Leigh R. Crilley, Louisa Kramer, William Bloss, Tuan Vu, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 20, 14847–14871, https://doi.org/10.5194/acp-20-14847-2020, https://doi.org/10.5194/acp-20-14847-2020, 2020
Short summary
Short summary
The paper details atmospheric chemistry in a megacity (Beijing), focussing on radicals which mediate the formation of secondary pollutants such as ozone and particles. Highly polluted conditions were experienced, including the highest ever levels of nitric oxide (NO), with simultaneous radical measurements. Radical concentrations were large during "haze" events, demonstrating active photochemistry. Modelling showed that our understanding of the chemistry at high NOx levels is incomplete.
Junjun Deng, Hao Guo, Hongliang Zhang, Jialei Zhu, Xin Wang, and Pingqing Fu
Atmos. Chem. Phys., 20, 14419–14435, https://doi.org/10.5194/acp-20-14419-2020, https://doi.org/10.5194/acp-20-14419-2020, 2020
Short summary
Short summary
One-year source apportionment of BC aerosols in a coastal city in China was conducted with the light-absorption observation-based method and source-oriented model. Source contributions identified by the two source apportionment methods were compared. Temporal variability, potential sources and transport pathways of BC from fossil fuel and biomass burning were characterized. Significant influence of biomass burning in North and East–Central China on BC in the region was highlighted.
Jingsha Xu, Shaojie Song, Roy M. Harrison, Congbo Song, Lianfang Wei, Qiang Zhang, Yele Sun, Lu Lei, Chao Zhang, Xiaohong Yao, Dihui Chen, Weijun Li, Miaomiao Wu, Hezhong Tian, Lining Luo, Shengrui Tong, Weiran Li, Junling Wang, Guoliang Shi, Yanqi Huangfu, Yingze Tian, Baozhu Ge, Shaoli Su, Chao Peng, Yang Chen, Fumo Yang, Aleksandra Mihajlidi-Zelić, Dragana Đorđević, Stefan J. Swift, Imogen Andrews, Jacqueline F. Hamilton, Ye Sun, Agung Kramawijaya, Jinxiu Han, Supattarachai Saksakulkrai, Clarissa Baldo, Siqi Hou, Feixue Zheng, Kaspar R. Daellenbach, Chao Yan, Yongchun Liu, Markku Kulmala, Pingqing Fu, and Zongbo Shi
Atmos. Meas. Tech., 13, 6325–6341, https://doi.org/10.5194/amt-13-6325-2020, https://doi.org/10.5194/amt-13-6325-2020, 2020
Short summary
Short summary
An interlaboratory comparison was conducted for the first time to examine differences in water-soluble inorganic ions (WSIIs) measured by 10 labs using ion chromatography (IC) and by two online aerosol chemical speciation monitor (ACSM) methods. Major ions including SO42−, NO3− and NH4+ agreed well in 10 IC labs and correlated well with ACSM data. WSII interlab variability strongly affected aerosol acidity results based on ion balance, but aerosol pH computed by ISORROPIA II was very similar.
Junfeng Wang, Jianhuai Ye, Dantong Liu, Yangzhou Wu, Jian Zhao, Weiqi Xu, Conghui Xie, Fuzhen Shen, Jie Zhang, Paul E. Ohno, Yiming Qin, Xiuyong Zhao, Scot T. Martin, Alex K. Y. Lee, Pingqing Fu, Daniel J. Jacob, Qi Zhang, Yele Sun, Mindong Chen, and Xinlei Ge
Atmos. Chem. Phys., 20, 14091–14102, https://doi.org/10.5194/acp-20-14091-2020, https://doi.org/10.5194/acp-20-14091-2020, 2020
Short summary
Short summary
We compared the organics in total submicron matter and those coated on BC cores during summertime in Beijing and found large differences between them. Traffic-related OA was associated significantly with BC, while cooking-related OA did not coat BC. In addition, a factor likely originated from primary biomass burning OA was only identified in BC-containing particles. Such a unique BBOA requires further field and laboratory studies to verify its presence and elucidate its properties and impacts.
Jiawei Li, Zhiwei Han, Pingqing Fu, and Xiaohong Yao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1016, https://doi.org/10.5194/acp-2020-1016, 2020
Revised manuscript not accepted
Short summary
Short summary
Organic aerosols of marine origin are so far poorly understood. An on-line coupled regional chemistry-climate model is developed to firstly explore and characterize the seasonality and annual feature of emission, distribution and radiative effects of marine organic aerosols specifically for the western Pacific over East Asia. This study reveals an important role of marine organic aerosols in radiation and cloud and would be valuable for climate research at both regional and global scales.
Wei Hu, Kotaro Murata, Chunlan Fan, Shu Huang, Hiromi Matsusaki, Pingqing Fu, and Daizhou Zhang
Biogeosciences, 17, 4477–4487, https://doi.org/10.5194/bg-17-4477-2020, https://doi.org/10.5194/bg-17-4477-2020, 2020
Short summary
Short summary
This paper reports the first estimate of the status of bacteria in long-distance-transported Asian dust, demonstrating that airborne dust, which can carry viable and nonviable bacteria on particle surfaces, is an efficient medium for constantly spreading bacteria at regional and even global scales. Such data are essential to better model and understand the roles and activities of bioaerosols in environmental evolution and climate change and the potential risks of bioaerosols to human health.
Wanyu Zhao, Hong Ren, Kimitaka Kawamura, Huiyun Du, Xueshun Chen, Siyao Yue, Qiaorong Xie, Lianfang Wei, Ping Li, Xin Zeng, Shaofei Kong, Yele Sun, Zifa Wang, and Pingqing Fu
Atmos. Chem. Phys., 20, 10331–10350, https://doi.org/10.5194/acp-20-10331-2020, https://doi.org/10.5194/acp-20-10331-2020, 2020
Short summary
Short summary
Our observations provide detailed information on the abundance and vertical distribution of dicarboxylic acids, oxoacids and α-dicarbonyls in PM2.5 collected at three heights based on a 325 m meteorological tower in Beijing in summer. Our results demonstrate that organic acids at the ground surface are largely associated with local traffic emissions, while long-range atmospheric transport followed by photochemical ageing contributes more in the urban boundary layer than the ground surface.
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., Aschmann, S. M., Arey, J., and Shorees, B.:
Formation of OH radicals in the gas phase reactions of O3 with a series of terpenes, J. Geophys. Res., 97, 6065–6073, https://doi.org/10.1029/92JD00062, 1992.
Badali, K. M., Zhou, S., Aljawhary, D., Antiñolo, M., Chen, W. J., Lok, A., Mungall, E., Wong, J. P. S., Zhao, R., and Abbatt, J. P. D.:
Formation of hydroxyl radicals from photolysis of secondary organic aerosol material, Atmos. Chem. Phys., 15, 7831–7840, https://doi.org/10.5194/acp-15-7831-2015, 2015.
Barsanti, K. C., Kroll, J. H., and Thornton, J. A.:
Formation of low-volatility organic compounds in the atmosphere: Recent advancements and insights, J. Phys. Chem. Lett., 8, 1503–1511, https://doi.org/10.1021/acs.jpclett.6b02969, 2017.
Berndt, T., Richters, S., Jokinen, T., Hyttinen, N., Kurtén, T., Otkjær, R. V., Kjaergaard, H. G., Stratmann, F., Herrmann, H., Sipilä, M., Kulmala, M., and Ehn, M.:
Hydroxyl radical-induced formation of highly oxidized organic compounds, Nat. Commun., 7, 13677, https://doi.org/10.1038/ncomms13677, 2016.
Berndt, T., Mentler, B., Scholz, W., Fischer, L., Herrmann, H., Kulmala, M., and Hansel, A.:
Accretion product formation from ozonolysis and OH radical reaction of α-pinene: Mechanistic insight and the influence of isoprene and ethylene, Environ. Sci. Technol., 52, 11069–11077, https://doi.org/10.1021/acs.est.8b02210, 2018a.
Berndt, T., Scholz, W., Mentler, B., Fischer, L., Herrmann, H., Kulmala, M., and Hansel, A.:
Accretion product formation from self- and cross-reactions of RO2 radicals in the atmosphere, Angew. Chem. Int. Edit., 57, 3820–3824, https://doi.org/10.1002/anie.201710989, 2018b.
Bianchi, F., Kurten, T., Riva, M., Mohr, C., Rissanen, M. P., Roldin, P., Berndt, T., Crounse, J. D., Wennberg, P. O., Mentel, T. F., Wildt, J., Junninen, H., Jokinen, T., Kulmala, M., Worsnop, D. R., Thornton, J. A., Donahue, N., Kjaergaard, H. G., and Ehn, M.:
Highly oxygenated organic molecules (HOM) from gas-phase autoxidation involving peroxy radicals: A key contributor to atmospheric aerosol, Chem. Rev., 119, 3472–3509, https://doi.org/10.1021/acs.chemrev.8b00395, 2019.
Bianco, A., Deguillaume, L., Vaitilingom, M., Nicol, E., Baray, J. L., Chaumerliac, N., and Bridoux, M.:
Molecular characterization of cloud water samples collected at the Puy de Dome (France) by Fourier transform ion cyclotron resonance mass spectrometry, Environ. Sci. Technol., 52, 10275–10285, https://doi.org/10.1021/acs.est.8b01964, 2018.
Brean, J., Harrison, R. M., Shi, Z., Beddows, D. C. S., Acton, W. J. F., Hewitt, C. N., Squires, F. A., and Lee, J.:
Observations of highly oxidized molecules and particle nucleation in the atmosphere of Beijing, Atmos. Chem. Phys., 19, 14933–14947, https://doi.org/10.5194/acp-19-14933-2019, 2019.
Brean, J., Beddows, D. C. S., Shi, Z., Temime-Roussel, B., Marchand, N., Querol, X., Alastuey, A., Minguillón, M. C., and Harrison, R. M.:
Molecular insights into new particle formation in Barcelona, Spain, Atmos. Chem. Phys., 20, 10029–10045, https://doi.org/10.5194/acp-20-10029-2020, 2020.
Cao, D., Lv, J., Geng, F., Rao, Z., Niu, H., Shi, Y., Cai, Y., and Kang, Y.:
Ion accumulation time dependent molecular characterization of natural organic matter using electrospray ionization-Fourier transform ion cyclotron resonance mass spectrometry, Anal. Chem., 88, 12210–12218, https://doi.org/10.1021/acs.analchem.6b03198, 2016.
Chen, Q., Liu, Y., Donahue, N. M., Shilling, J. E., and Martin, S. T.:
Particle-phase chemistry of secondary organic material: Modeled compared to measured O:C and H:C elemental ratios provide constraints, Environ. Sci. Technol., 45, 4763–4770, https://doi.org/10.1021/es104398s, 2011.
Claflin, M. S., Krechmer, J. E., Hu, W., Jimenez, J. L., and Ziemann, P. J.:
Functional group composition of secondary organic aerosol formed from ozonolysis of α-pinene under high VOC and autoxidation conditions, ACS Earth Space Chem., 2, 1196–1210, https://doi.org/10.1021/acsearthspacechem.8b00117, 2018.
Cohen, A. J., Brauer, M., Burnett, R., Anderson, H. R., Frostad, J., Estep, K., Balakrishnan, K., Brunekreef, B., Dandona, L., Dandona, R., Feigin, V., Freedman, G., Hubbell, B., Jobling, A., Kan, H., Knibbs, L., Liu, Y., Martin, R., Morawska, L., Pope, C. A., Shin, H., Straif, K., Shaddick, G., Thomas, M., van Dingenen, R., van Donkelaar, A., Vos, T., Murray, C. J. L., and Forouzanfar, M. H.:
Estimates and 25-year trends of the global burden of disease attributable to ambient air pollution: an analysis of data from the Global Burden of Diseases Study 2015, Lancet, 389, 1907–1918, https://doi.org/10.1016/S0140-6736(17)30505-6, 2017.
Crounse, J. D., Nielsen, L. B., Jørgensen, S., Kjaergaard, H. G., and Wennberg, P. O.:
Autoxidation of organic compounds in the atmosphere, J. Phys. Chem. Lett., 4, 3513–3520, https://doi.org/10.1021/jz4019207, 2013.
Donahue, N. M., Epstein, S. A., Pandis, S. N., and Robinson, A. L.:
A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics, Atmos. Chem. Phys., 11, 3303–3318, https://doi.org/10.5194/acp-11-3303-2011, 2011.
Donahue, N. M., Kroll, J. H., Pandis, S. N., and Robinson, A. L.:
A two-dimensional volatility basis set – Part 2: Diagnostics of organic-aerosol evolution, Atmos. Chem. Phys., 12, 615–634, https://doi.org/10.5194/acp-12-615-2012, 2012.
Ehn, M., Kleist, E., Junninen, H., Petäjä, T., Lönn, G., Schobesberger, S., Dal Maso, M., Trimborn, A., Kulmala, M., Worsnop, D. R., Wahner, A., Wildt, J., and Mentel, Th. F.:
Gas phase formation of extremely oxidized pinene reaction products in chamber and ambient air, Atmos. Chem. Phys., 12, 5113–5127, https://doi.org/10.5194/acp-12-5113-2012, 2012.
Ehn, M., Thornton, J. A., Kleist, E., Sipila, M., Junninen, H., Pullinen, I., Springer, M., Rubach, F., Tillmann, R., Lee, B., Lopez-Hilfiker, F., Andres, S., Acir, I. H., Rissanen, M., Jokinen, T., Schobesberger, S., Kangasluoma, J., Kontkanen, J., Nieminen, T., Kurten, T., Nielsen, L. B., Jorgensen, S., Kjaergaard, H. G., Canagaratna, M., Maso, M. D., Berndt, T., Petaja, T., Wahner, A., Kerminen, V. M., Kulmala, M., Worsnop, D. R., Wildt, J., and Mentel, T. F.:
A large source of low-volatility secondary organic aerosol, Nature, 506, 476–479, https://doi.org/10.1038/nature13032, 2014.
Fu, P., Kawamura, K., Chen, J., and Barrie, L. A.:
Isoprene, monoterpene, and sesquiterpene oxidation products in the high Arctic aerosols during late winter to early summer, Environ. Sci. Technol., 43, 4022–4028, https://doi.org/10.1021/es803669a, 2009.
Gallimore, P. J., Mahon, B. M., Wragg, F. P. H., Fuller, S. J., Giorio, C., Kourtchev, I., and Kalberer, M.:
Multiphase composition changes and reactive oxygen species formation during limonene oxidation in the new Cambridge Atmospheric Simulation Chamber (CASC), Atmos. Chem. Phys., 17, 9853–9868, https://doi.org/10.5194/acp-17-9853-2017, 2017.
Gong, Y., Chen, Z., and Li, H.:
The oxidation regime and SOA composition in limonene ozonolysis: roles of different double bonds, radicals, and water, Atmos. Chem. Phys., 18, 15105–15123, https://doi.org/10.5194/acp-18-15105-2018, 2018.
Grieshop, A. P., Donahue, N. M., and Robinson, A. L.:
Is the gas-particle partitioning in alpha-pinene secondary organic aerosol reversible?, Geophys. Res. Lett., 34, L14810, https://doi.org/10.1029/2007gl029987, 2007.
Griffin, R. J., Cocker, D. R., Flagan, R. C., and Seinfeld, J. H.:
Organic aerosol formation from the oxidation of biogenic hydrocarbons, J. Geophys. Res.-Atmos., 104, 3555–3567, https://doi.org/10.1029/1998jd100049, 1999.
Guenther, A. B., Jiang, X., Heald, C. L., Sakulyanontvittaya, T., Duhl, T., Emmons, L. K., and Wang, X.:
The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions, Geosci. Model Dev., 5, 1471–1492, https://doi.org/10.5194/gmd-5-1471-2012, 2012.
Guo, Y., Shen, H., Pullinen, I., Luo, H., Kang, S., Vereecken, L., Fuchs, H., Hallquist, M., Acir, I.-H., Tillmann, R., Rohrer, F., Wildt, J., Kiendler-Scharr, A., Wahner, A., Zhao, D., and Mentel, T. F.:
Identification of highly oxygenated organic molecules and their role in aerosol formation in the reaction of limonene with nitrate radical, Atmos. Chem. Phys., 22, 11323–11346, https://doi.org/10.5194/acp-22-11323-2022, 2022.
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.:
The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009.
Hammes, J., Lutz, A., Mentel, T., Faxon, C., and Hallquist, M.:
Carboxylic acids from limonene oxidation by ozone and hydroxyl radicals: insights into mechanisms derived using a FIGAERO-CIMS, Atmos. Chem. Phys., 19, 13037–13052, https://doi.org/10.5194/acp-19-13037-2019, 2019.
Iyer, S., Rissanen, M. P., Valiev, R., Barua, S., Krechmer, J. E., Thornton, J., Ehn, M., and Kurten, T.:
Molecular mechanism for rapid autoxidation in α-pinene ozonolysis, Nat. Commun., 12, 878, https://doi.org/10.1038/s41467-021-21172-w, 2021.
Jaoui, M. and Kamens, R. M.:
Gaseous and particulate oxidation products analysis of a mixture of α-pinene + β-pinene/O3/air in the absence of light and α-pinene + β-pinene/NOx/air in the presence of natural sunlight, J. Atmos. Chem., 44, 259–297, https://doi.org/10.1023/A:1022977427523, 2003.
Jokinen, T., Sipilä, M., Richters, S., Kerminen, V.-M., Paasonen, P., Stratmann, F., Worsnop, D., Kulmala, M., Ehn, M., Herrmann, H., and Berndt, T.:
Rapid autoxidation forms highly oxidized RO2 radicals in the atmosphere, Angew. Chem. Int. Edit., 53, 14596–14600, https://doi.org/10.1002/anie.201408566, 2014.
Jokinen, T., Berndt, T., Makkonen, R., Kerminen, V. M., Junninen, H., Paasonen, P., Stratmann, F., Herrmann, H., Guenther, A. B., Worsnop, D. R., Kulmala, M., Ehn, M., and Sipila, M.:
Production of extremely low volatile organic compounds from biogenic emissions: Measured yields and atmospheric implications, P. Natl. Acad. Sci. USA, 112, 7123–7128, https://doi.org/10.1073/pnas.1423977112, 2015.
Kahnt, A., Vermeylen, R., Iinuma, Y., Safi Shalamzari, M., Maenhaut, W., and Claeys, M.:
High-molecular-weight esters in α-pinene ozonolysis secondary organic aerosol: structural characterization and mechanistic proposal for their formation from highly oxygenated molecules, Atmos. Chem. Phys., 18, 8453–8467, https://doi.org/10.5194/acp-18-8453-2018, 2018.
Kamens, R., Jang, M., Chien, C.-J., and Leach, K.:
Aerosol formation from the reaction of α-pinene and ozone using a gas-phase kinetics-aerosol partitioning model, Environ. Sci. Technol., 33, 1430–1438, https://doi.org/10.1021/es980725r, 1999.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.:
Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, https://doi.org/10.5194/acp-5-1053-2005, 2005.
Kenseth, C. M., Huang, Y., Zhao, R., Dalleska, N. F., Hethcox, J. C., Stoltz, B. M., and Seinfeld, J. H.:
Synergistic O3 + OH oxidation pathway to extremely low-volatility dimers revealed in β-pinene secondary organic aerosol, P. Natl. Acad. Sci. USA, 115, 8301–8306, https://doi.org/10.1073/pnas.1804671115, 2018.
Kerminen, V.-M., Paramonov, M., Anttila, T., Riipinen, I., Fountoukis, C., Korhonen, H., Asmi, E., Laakso, L., Lihavainen, H., Swietlicki, E., Svenningsson, B., Asmi, A., Pandis, S. N., Kulmala, M., and Petäjä, T.:
Cloud condensation nuclei production associated with atmospheric nucleation: a synthesis based on existing literature and new results, Atmos. Chem. Phys., 12, 12037–12059, https://doi.org/10.5194/acp-12-12037-2012, 2012.
Kirkby, J., Duplissy, J., Sengupta, K., Frege, C., Gordon, H., Williamson, C., Heinritzi, M., Simon, M., Yan, C., Almeida, J., Trostl, J., Nieminen, T., Ortega, I. K., Wagner, R., Adamov, A., Amorim, A., Bernhammer, A. K., Bianchi, F., Breitenlechner, M., Brilke, S., Chen, X., Craven, J., Dias, A., Ehrhart, S., Flagan, R. C., Franchin, A., Fuchs, C., Guida, R., Hakala, J., Hoyle, C. R., Jokinen, T., Junninen, H., Kangasluoma, J., Kim, J., Krapf, M., Kurten, A., Laaksonen, A., Lehtipalo, K., Makhmutov, V., Mathot, S., Molteni, U., Onnela, A., Perakyla, O., Piel, F., Petaja, T., Praplan, A. P., Pringle, K., Rap, A., Richards, N. A., Riipinen, I., Rissanen, M. P., Rondo, L., Sarnela, N., Schobesberger, S., Scott, C. E., Seinfeld, J. H., Sipila, M., Steiner, G., Stozhkov, Y., Stratmann, F., Tome, A., Virtanen, A., Vogel, A. L., Wagner, A. C., Wagner, P. E., Weingartner, E., Wimmer, D., Winkler, P. M., Ye, P., Zhang, X., Hansel, A., Dommen, J., Donahue, N. M., Worsnop, D. R., Baltensperger, U., Kulmala, M., Carslaw, K. S., and Curtius, J.:
Ion-induced nucleation of pure biogenic particles, Nature, 533, 521–526, https://doi.org/10.1038/nature17953, 2016.
Koch, B. P., Witt, M., Engbrodt, R., Dittmar, T., and Kattner, G.:
Molecular formulae of marine and terrigenous dissolved organic matter detected by electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry, Geochim. Cosmochim. Ac., 69, 3299–3308, https://doi.org/10.1016/j.gca.2005.02.027, 2005.
Koch, B. P., Dittmar, T., Witt, M., and Kattner, G.:
Fundamentals of molecular formula assignment to ultrahigh resolution mass data of natural organic matter, Anal. Chem., 79, 1758–1763, https://doi.org/10.1021/ac061949s, 2007.
Kourtchev, I., Giorio, C., Manninen, A., Wilson, E., Mahon, B., Aalto, J., Kajos, M., Venables, D., Ruuskanen, T., Levula, J., Loponen, M., Connors, S., Harris, N., Zhao, D., Kiendler-Scharr, A., Mentel, T., Rudich, Y., Hallquist, M., Doussin, J.-F., Maenhaut, W., Bäck, J., Petäjä, T., Wenger, J., Kulmala, M., and Kalberer, M.:
Enhanced Volatile Organic Compounds emissions and organic aerosol mass increase the oligomer content of atmospheric aerosols, Sci. Rep.-UK, 6, 35038, https://doi.org/10.1038/srep35038, 2016.
Kristensen, K., Watne, Å. K., Hammes, J., Lutz, A., Petäjä, T., Hallquist, M., Bilde, M., and Glasius, M.:
High-molecular weight dimer esters are major products in aerosols from α-pinene ozonolysis and the boreal forest, Environ. Sci. Technol. Lett., 3, 280–285, https://doi.org/10.1021/acs.estlett.6b00152, 2016.
Kroll, J. H. and Seinfeld, J. H.:
Chemistry of secondary organic aerosol: Formation and evolution of low-volatility organics in the atmosphere, Atmos. Environ., 42, 3593–3624, https://doi.org/10.1016/j.atmosenv.2008.01.003, 2008.
Kroll, J. H., Chan, A. W. H., Ng, N. L., Flagan, R. C., and Seinfeld, J. H.:
Reactions of semivolatile organics and their effects on secondary organic aerosol formation, Environ. Sci. Technol., 41, 3545–3550, https://doi.org/10.1021/es062059x, 2007.
Kroll, J. H., Donahue, N. M., Jimenez, J. L., Kessler, S. H., Canagaratna, M. R., Wilson, K. R., Altieri, K. E., Mazzoleni, L. R., Wozniak, A. S., Bluhm, H., Mysak, E. R., Smith, J. D., Kolb, C. E., and Worsnop, D. R.:
Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol, Nat. Chem., 3, 133–139, https://doi.org/10.1038/nchem.948, 2011.
Kundu, S., Fisseha, R., Putman, A. L., Rahn, T. A., and Mazzoleni, L. R.:
High molecular weight SOA formation during limonene ozonolysis: insights from ultrahigh-resolution FT-ICR mass spectrometry characterization, Atmos. Chem. Phys., 12, 5523–5536, https://doi.org/10.5194/acp-12-5523-2012, 2012.
Laden, F., Schwartz, J., Speizer, F. E., and Dockery, D. W.:
Reduction in fine particulate air pollution and mortality, Am. J. Resp. Crit. Care, 173, 667–672, https://doi.org/10.1164/rccm.200503-443OC, 2006.
Lee, R., Gryn'ova, G., Ingold, K. U., and Coote, M. L.:
Why are sec-alkylperoxyl bimolecular self-reactions orders of magnitude faster than the analogous reactions of tert-alkylperoxyls? The unanticipated role of CH hydrogen bond donation, Phys. Chem. Chem. Phys., 18, 23673–23679, https://doi.org/10.1039/c6cp04670c, 2016.
Li, H., Yang, Y., Jin, J., Wang, H., Li, K., Wang, P., and Liao, H.:
Climate-driven deterioration of future ozone pollution in Asia predicted by machine learning with multi-source data, Atmos. Chem. Phys., 23, 1131–1145, https://doi.org/10.5194/acp-23-1131-2023, 2023.
Li, M., Li, J., Zhu, Y., Chen, J., Andreae, M. O., Pöschl, U., Su, H., Kulmala, M., Chen, C., Cheng, Y., and Zhao, J.:
Highly oxygenated organic molecules with high unsaturation formed upon photochemical aging of soot, Chem, 8, 2688–2699, https://doi.org/10.1016/j.chempr.2022.06.011, 2022.
Li, X., Chee, S., Hao, J., Abbatt, J. P. D., Jiang, J., and Smith, J. N.:
Relative humidity effect on the formation of highly oxidized molecules and new particles during monoterpene oxidation, Atmos. Chem. Phys., 19, 1555–1570, https://doi.org/10.5194/acp-19-1555-2019, 2019.
Li, Y., Pöschl, U., and Shiraiwa, M.:
Molecular corridors and parameterizations of volatility in the chemical evolution of organic aerosols, Atmos. Chem. Phys., 16, 3327–3344, https://doi.org/10.5194/acp-16-3327-2016, 2016.
Liu, P., Li, Y. J., Wang, Y., Gilles, M. K., Zaveri, R. A., Bertram, A. K., and Martin, S. T.:
Lability of secondary organic particulate matter, P. Natl. Acad. Sci. USA, 113, 12643–12648, https://doi.org/10.1073/pnas.1603138113, 2016.
Ma, Y. and Marston, G.:
Multifunctional acid formation from the gas-phase ozonolysis of β-pinene, Phys. Chem. Chem. Phys., 10, 6115–6126, https://doi.org/10.1039/b807863g, 2008.
Mahilang, M., Deb, M. K., and Pervez, S.:
Biogenic secondary organic aerosols: A review on formation mechanism, analytical challenges and environmental impacts, Chemosphere, 262, 127771, https://doi.org/10.1016/j.chemosphere.2020.127771, 2021.
Molteni, U., Bianchi, F., Klein, F., El Haddad, I., Frege, C., Rossi, M. J., Dommen, J., and Baltensperger, U.:
Formation of highly oxygenated organic molecules from aromatic compounds, Atmos. Chem. Phys., 18, 1909–1921, https://doi.org/10.5194/acp-18-1909-2018, 2018.
Mutzel, A., Rodigast, M., Iinuma, Y., Böge, O., and Herrmann, H.:
Monoterpene SOA – contribution of first-generation oxidation products to formation and chemical composition, Atmos. Environ., 130, 136–144, https://doi.org/10.1016/j.atmosenv.2015.10.080, 2016.
Noziere, B., Kalberer, M., Claeys, M., Allan, J., D'Anna, B., Decesari, S., Finessi, E., Glasius, M., Grgic, I., Hamilton, J. F., Hoffmann, T., Iinuma, Y., Jaoui, M., Kahnt, A., Kampf, C. J., Kourtchev, I., Maenhaut, W., Marsden, N., Saarikoski, S., Schnelle-Kreis, J., Surratt, J. D., Szidat, S., Szmigielski, R., and Wisthaler, A.:
The molecular identification of organic compounds in the atmosphere: state of the art and challenges, Chem. Rev., 115, 3919–3983, https://doi.org/10.1021/cr5003485, 2015.
Pathak, R., Donahue, N. M., and Pandis, S. N.:
Ozonolysis of β-Pinene: Temperature dependence of secondary organic aerosol mass fraction, Environ. Sci. Technol., 42, 5081–5086, https://doi.org/10.1021/es070721z, 2008.
Pathak, R. K., Salo, K., Emanuelsson, E. U., Cai, C., Lutz, A., Hallquist, A. M., and Hallquist, M.:
Influence of ozone and radical chemistry on limonene organic aerosol production and thermal characteristics, Environ. Sci. Technol., 46, 11660–11669, https://doi.org/10.1021/es301750r, 2012.
Peräkylä, O., Riva, M., Heikkinen, L., Quéléver, L., Roldin, P., and Ehn, M.:
Experimental investigation into the volatilities of highly oxygenated organic molecules (HOMs) , Atmos. Chem. Phys., 20, 649–669, https://doi.org/10.5194/acp-20-649-2020, 2020.
Perraud, V., Bruns, E. A., Ezell, M. J., Johnson, S. N., Yu, Y., Alexander, M. L., Zelenyuk, A., Imre, D., Chang, W. L., Dabdub, D., Pankow, J. F., and Finlayson-Pitts, B. J.:
Nonequilibrium atmospheric secondary organic aerosol formation and growth, P. Natl. Acad. Sci. USA, 109, 2836–2841, https://doi.org/10.1073/pnas.1119909109, 2012.
Pullinen, I., Schmitt, S., Kang, S., Sarrafzadeh, M., Schlag, P., Andres, S., Kleist, E., Mentel, T. F., Rohrer, F., Springer, M., Tillmann, R., Wildt, J., Wu, C., Zhao, D., Wahner, A., and Kiendler-Scharr, A.:
Impact of NOx on secondary organic aerosol (SOA) formation from α-pinene and β-pinene photooxidation: the role of highly oxygenated organic nitrates, Atmos. Chem. Phys., 20, 10125–10147, https://doi.org/10.5194/acp-20-10125-2020, 2020.
Ramanathan, V., Crutzen, P. J., Kiehl, J. T., and Rosenfeld, D.:
Aerosols, climate, and the hydrological cycle, Science, 294, 2119–2124, https://doi.org/10.1126/science.1064034, 2001.
Rissanen, M. P.:
NO2 suppression of autoxidation–inhibition of gas-phase highly oxidized dimer product formation, ACS Earth Space Chem., 2, 1211–1219, https://doi.org/10.1021/acsearthspacechem.8b00123, 2018.
Rissanen, M. P., Kurtén, T., Sipilä, M., Thornton, J. A., Kangasluoma, J., Sarnela, N., Junninen, H., Jørgensen, S., Schallhart, S., Kajos, M. K., Taipale, R., Springer, M., Mentel, T. F., Ruuskanen, T., Petäjä, T., Worsnop, D. R., Kjaergaard, H. G., and Ehn, M.:
The formation of highly oxidized multifunctional products in the ozonolysis of cyclohexene, J. Am. Chem. Soc., 136, 15596–15606, https://doi.org/10.1021/ja507146s, 2014.
Rohr, A. C., Weschler, C. J., Koutrakis, P., and Spengler, J. D.:
Generation and quantification of ultrafine particles through terpene/ozone reaction in a chamber setting, Aerosol Sci. Technol., 37, 65–78, https://doi.org/10.1080/02786820300892, 2003.
Roldin, P., Ehn, M., Kurten, T., Olenius, T., Rissanen, M. P., Sarnela, N., Elm, J., Rantala, P., Hao, L., Hyttinen, N., Heikkinen, L., Worsnop, D. R., Pichelstorfer, L., Xavier, C., Clusius, P., Ostrom, E., Petaja, T., Kulmala, M., Vehkamaki, H., Virtanen, A., Riipinen, I., and Boy, M.:
The role of highly oxygenated organic molecules in the boreal aerosol-cloud-climate system, Nat. Commun., 10, 4370, https://doi.org/10.1038/s41467-019-12338-8, 2019.
Saukko, E., Lambe, A. T., Massoli, P., Koop, T., Wright, J. P., Croasdale, D. R., Pedernera, D. A., Onasch, T. B., Laaksonen, A., Davidovits, P., Worsnop, D. R., and Virtanen, A.:
Humidity-dependent phase state of SOA particles from biogenic and anthropogenic precursors, Atmos. Chem. Phys., 12, 7517–7529, https://doi.org/10.5194/acp-12-7517-2012, 2012.
Schervish, M. and Donahue, N. M.:
Peroxy radical chemistry and the volatility basis set, Atmos. Chem. Phys., 20, 1183–1199, https://doi.org/10.5194/acp-20-1183-2020, 2020.
Shah, R. U., Coggon, M. M., Gkatzelis, G. I., McDonald, B. C., Tasoglou, A., Huber, H., Gilman, J., Warneke, C., Robinson, A. L., and Presto, A. A.:
Urban oxidation flow reactor measurements reveal significant secondary organic aerosol contributions from volatile emissions of emerging importance, Environ. Sci. Technol., 54, 714–725, https://doi.org/10.1021/acs.est.9b06531, 2019.
Shen, H., Zhao, D., Pullinen, I., Kang, S., Vereecken, L., Fuchs, H., Acir, I. H., Tillmann, R., Rohrer, F., Wildt, J., Kiendler-Scharr, A., Wahner, A., and Mentel, T. F.:
Highly oxygenated organic nitrates formed from NO3 radical-initiated oxidation of β-pinene, Environ. Sci. Technol., 55, 15658–15671, https://doi.org/10.1021/acs.est.1c03978, 2021.
Shi, X., Tang, R., Dong, Z., Liu, H., Xu, F., Zhang, Q., Zong, W., and Cheng, J.:
A neglected pathway for the accretion products formation in the atmosphere, Sci. Total Environ., 848, 157494, https://doi.org/10.1016/j.scitotenv.2022.157494, 2022.
Shiraiwa, M., Berkemeier, T., Schilling-Fahnestock, K. A., Seinfeld, J. H., and Pöschl, U.:
Molecular corridors and kinetic regimes in the multiphase chemical evolution of secondary organic aerosol, Atmos. Chem. Phys., 14, 8323–8341, https://doi.org/10.5194/acp-14-8323-2014, 2014.
Shrivastava, M., Cappa, C. D., Fan, J., Goldstein, A. H., Guenther, A. B., Jimenez, J. L., Kuang, C., Laskin, A., Martin, S. T., Ng, N. L., Petaja, T., Pierce, J. R., Rasch, P. J., Roldin, P., Seinfeld, J. H., Shilling, J., Smith, J. N., Thornton, J. A., Volkamer, R., Wang, J., Worsnop, D. R., Zaveri, R. A., Zelenyuk, A., and Zhang, Q.:
Recent advances in understanding secondary organic aerosol: Implications for global climate forcing, Rev. Geophys., 55, 509–559, https://doi.org/10.1002/2016rg000540, 2017.
Simon, M., Dada, L., Heinritzi, M., Scholz, W., Stolzenburg, D., Fischer, L., Wagner, A. C., Kürten, A., Rörup, B., He, X.-C., Almeida, J., Baalbaki, R., Baccarini, A., Bauer, P. S., Beck, L., Bergen, A., Bianchi, F., Bräkling, S., Brilke, S., Caudillo, L., Chen, D., Chu, B., Dias, A., Draper, D. C., Duplissy, J., El-Haddad, I., Finkenzeller, H., Frege, C., Gonzalez-Carracedo, L., Gordon, H., Granzin, M., Hakala, J., Hofbauer, V., Hoyle, C. R., Kim, C., Kong, W., Lamkaddam, H., Lee, C. P., Lehtipalo, K., Leiminger, M., Mai, H., Manninen, H. E., Marie, G., Marten, R., Mentler, B., Molteni, U., Nichman, L., Nie, W., Ojdanic, A., Onnela, A., Partoll, E., Petäjä, T., Pfeifer, J., Philippov, M., Quéléver, L. L. J., Ranjithkumar, A., Rissanen, M. P., Schallhart, S., Schobesberger, S., Schuchmann, S., Shen, J., Sipilä, M., Steiner, G., Stozhkov, Y., Tauber, C., Tham, Y. J., Tomé, A. R., Vazquez-Pufleau, M., Vogel, A. L., Wagner, R., Wang, M., Wang, D. S., Wang, Y., Weber, S. K., Wu, Y., Xiao, M., Yan, C., Ye, P., Ye, Q., Zauner-Wieczorek, M., Zhou, X., Baltensperger, U., Dommen, J., Flagan, R. C., Hansel, A., Kulmala, M., Volkamer, R., Winkler, P. M., Worsnop, D. R., Donahue, N. M., Kirkby, J., and Curtius, J.:
Molecular understanding of new-particle formation from α-pinene between −50 and +25 ∘C, Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, 2020.
Song, C., Zaveri, R. A., Shilling, J. E., Alexander, M. L., and Newburn, M.:
Effect of hydrophilic organic seed aerosols on secondary organic aerosol formation from ozonolysis of α-pinene, Environ. Sci. Technol., 45, 7323–7329, https://doi.org/10.1021/es201225c, 2011.
Takekawa, H., Minoura, H., and Yamazaki, S.:
Temperature dependence of secondary organic aerosol formation by photo-oxidation of hydrocarbons, Atmos. Environ., 37, 3413–3424, https://doi.org/10.1016/S1352-2310(03)00359-5, 2003.
Tomaz, S., Wang, D., Zabalegui, N., Li, D., Lamkaddam, H., Bachmeier, F., Vogel, A., Monge, M. E., Perrier, S., Baltensperger, U., George, C., Rissanen, M., Ehn, M., El Haddad, I., and Riva, M.:
Structures and reactivity of peroxy radicals and dimeric products revealed by online tandem mass spectrometry, Nat. Commun., 12, 300, https://doi.org/10.1038/s41467-020-20532-2, 2021.
Tong, H., Arangio, A. M., Lakey, P. S. J., Berkemeier, T., Liu, F., Kampf, C. J., Brune, W. H., Pöschl, U., and Shiraiwa, M.:
Hydroxyl radicals from secondary organic aerosol decomposition in water, Atmos. Chem. Phys., 16, 1761–1771, https://doi.org/10.5194/acp-16-1761-2016, 2016.
Tong, H., Lakey, P. S. J., Arangio, A. M., Socorro, J., Shen, F., Lucas, K., Brune, W. H., Poschl, U., and Shiraiwa, M.:
Reactive oxygen species formed by secondary organic aerosols in water and surrogate lung fluid, Environ. Sci. Technol., 52, 11642–11651, https://doi.org/10.1021/acs.est.8b03695, 2018.
Tong, H., Zhang, Y., Filippi, A., Wang, T., Li, C., Liu, F., Leppla, D., Kourtchev, I., Wang, K., Keskinen, H.-M., Levula, J. T., Arangio, A. M., Shen, F., Ditas, F., Martin, S. T., Artaxo, P., Godoi, R. H. M., Yamamoto, C. I., de Souza, R. A. F., Huang, R.-J., Berkemeier, T., Wang, Y., Su, H., Cheng, Y., Pope, F. D., Fu, P., Yao, M., Pöhlker, C., Petäjä, T., Kulmala, M., Andreae, M. O., Shiraiwa, M., Pöschl, U., Hoffmann, T., and Kalberer, M.:
Radical formation by fine particulate matter associated with highly oxygenated molecules, Environ. Sci. Technol., 53, 12506–12518, https://doi.org/10.1021/acs.est.9b05149, 2019.
Tröstl, J., Chuang, W. K., Gordon, H., Heinritzi, M., Yan, C., Molteni, U., Ahlm, L., Frege, C., Bianchi, F., Wagner, R., Simon, M., Lehtipalo, K., Williamson, C., Craven, J. S., Duplissy, J., Adamov, A., Almeida, J., Bernhammer, A. K., Breitenlechner, M., Brilke, S., Dias, A., Ehrhart, S., Flagan, R. C., Franchin, A., Fuchs, C., Guida, R., Gysel, M., Hansel, A., Hoyle, C. R., Jokinen, T., Junninen, H., Kangasluoma, J., Keskinen, H., Kim, J., Krapf, M., Kurten, A., Laaksonen, A., Lawler, M., Leiminger, M., Mathot, S., Mohler, O., Nieminen, T., Onnela, A., Petäjä, T., Piel, F. M., Miettinen, P., Rissanen, M. P., Rondo, L., Sarnela, N., Schobesberger, S., Sengupta, K., Sipilä, M., Smith, J. N., Steiner, G., Tomè, A., Virtanen, A., Wagner, A. C., Weingartner, E., Wimmer, D., Winkler, P. M., Ye, P., Carslaw, K. S., Curtius, J., Dommen, J., Kirkby, J., Kulmala, M., Riipinen, I., Worsnop, D. R., Donahue, N. M., and Baltensperger, U.:
The role of low-volatility organic compounds in initial particle growth in the atmosphere, Nature, 533, 527–531, https://doi.org/10.1038/nature18271, 2016.
Tu, P., Hall, W. A. t., and Johnston, M. V.:
Characterization of highly oxidized molecules in fresh and aged biogenic secondary organic aerosol, Anal. Chem., 88, 4495–4501, https://doi.org/10.1021/acs.analchem.6b00378, 2016.
Vogel, A. L., Schneider, J., Müller-Tautges, C., Klimach, T., and Hoffmann, T.:
Aerosol chemistry resolved by mass spectrometry: Insights into particle growth after ambient new particle formation, Environ. Sci. Technol., 50, 10814–10822, https://doi.org/10.1021/acs.est.6b01673, 2016.
Wang, L. and Wang, L.:
The oxidation mechanism of gas-phase ozonolysis of limonene in the atmosphere, Phys. Chem. Chem. Phys., 23, 9294–9303, https://doi.org/10.1039/d0cp05803c, 2021.
Wang, M., Chen, D., Xiao, M., Ye, Q., Stolzenburg, D., Hofbauer, V., Ye, P., Vogel, A. L., Mauldin, R. L., 3rd, Amorim, A., Baccarini, A., Baumgartner, B., Brilke, S., Dada, L., Dias, A., Duplissy, J., Finkenzeller, H., Garmash, O., He, X. C., Hoyle, C. R., Kim, C., Kvashnin, A., Lehtipalo, K., Fischer, L., Molteni, U., Petaja, T., Pospisilova, V., Quelever, L. L. J., Rissanen, M., Simon, M., Tauber, C., Tome, A., Wagner, A. C., Weitz, L., Volkamer, R., Winkler, P. M., Kirkby, J., Worsnop, D. R., Kulmala, M., Baltensperger, U., Dommen, J., El-Haddad, I., and Donahue, N. M.:
Photo-oxidation of aromatic hydrocarbons produces low-volatility organic compounds, Environ. Sci. Technol., 54, 7911–7921, https://doi.org/10.1021/acs.est.0c02100, 2020.
Wang, S., Zhao, Y., Chan, A. W. H., Yao, M., Chen, Z., and Abbatt, J. P. D.:
Organic peroxides in aerosol: Key reactive intermediates for multiphase processes in the atmosphere, Chem. Rev., 123, 1635–1679, https://doi.org/10.1021/acs.chemrev.2c00430, 2023.
Waring, M. S., Wells, J. R., and Siegel, J. A.:
Secondary organic aerosol formation from ozone reactions with single terpenoids and terpenoid mixtures, Atmos. Environ., 45, 4235–4242, https://doi.org/10.1016/j.atmosenv.2011.05.001, 2011.
Wu, K., Yang, X., Chen, D., Gu, S., Lu, Y., Jiang, Q., Wang, K., Ou, Y., Qian, Y., Shao, P., and Lu, S.: Estimation of biogenic VOC emissions and their corresponding impact on ozone and secondary organic aerosol formation in China, Atmos. Res., 231, 104656, https://doi.org/10.1016/j.atmosres.2019.104656, 2020.
Wu, Z., Rodgers, R. P., and Marshall, A. G.:
Two- and three-dimensional van Krevelen diagrams: A graphical analysis complementary to the kendrick mass plot for sorting elemental compositions of complex organic mixtures based on ultrahigh-resolution broadband Fourier transform ion cyclotron resonance mass measurements, Anal. Chem., 76, 2511–2516, https://doi.org/10.1021/ac0355449, 2004.
Xie, Q., Su, S., Chen, S., Xu, Y., Cao, D., Chen, J., Ren, L., Yue, S., Zhao, W., Sun, Y., Wang, Z., Tong, H., Su, H., Cheng, Y., Kawamura, K., Jiang, G., Liu, C.-Q., and Fu, P.:
Molecular characterization of firework-related urban aerosols using Fourier transform ion cyclotron resonance mass spectrometry, Atmos. Chem. Phys., 20, 6803–6820, https://doi.org/10.5194/acp-20-6803-2020, 2020a.
Xie, Q., Li, Y., Yue, S., Su, S., Cao, D., Xu, Y., Chen, J., Tong, H., Su, H., Cheng, Y., Zhao, W., Hu, W., Wang, Z., Yang, T., Pan, X., Sun, Y., Wang, Z., Liu, C. Q., Kawamura, K., Jiang, G., Shiraiwa, M., and Fu, P.:
Increase of high molecular weight organosulfate with intensifying urban air pollution in the megacity Beijing, J. Geophys. Res.-Atmos., 125, e2019JD032200, https://doi.org/10.1029/2019jd032200, 2020b.
Xie, Q., Su, S., Dai, Y., Hu, W., Yue, S., Cao, D., Jiang, G., and Fu, P.:
Deciphering 13C and 34S isotopes of organosulfates in urban aerosols by FT-ICR mass spectrometry, Environ. Sci. Technol. Lett., 9, 526–532, https://doi.org/10.1021/acs.estlett.2c00255, 2022.
Zhang, X., Lambe, A. T., Upshur, M. A., Brooks, W. A., Gray Be, A., Thomson, R. J., Geiger, F. M., Surratt, J. D., Zhang, Z., Gold, A., Graf, S., Cubison, M. J., Groessl, M., Jayne, J. T., Worsnop, D. R., and Canagaratna, M. R.:
Highly oxygenated multifunctional compounds in α-pinene secondary organic aerosol, Environ. Sci. Technol., 51, 5932–5940, https://doi.org/10.1021/acs.est.6b06588, 2017.
Zhang, Y., Wang, K., Tong, H., Huang, R. J., and Hoffmann, T.:
The maximum carbonyl ratio (MCR) as a new index for the structural classification of secondary organic aerosol components, Rapid Commun. Mass Sp., 35, e9113, https://doi.org/10.1002/rcm.9113, 2021.
Zhao, D. F., Kaminski, M., Schlag, P., Fuchs, H., Acir, I.-H., Bohn, B., Häseler, R., Kiendler-Scharr, A., Rohrer, F., Tillmann, R., Wang, M. J., Wegener, R., Wildt, J., Wahner, A., and Mentel, Th. F.:
Secondary organic aerosol formation from hydroxyl radical oxidation and ozonolysis of monoterpenes, Atmos. Chem. Phys., 15, 991–1012, https://doi.org/10.5194/acp-15-991-2015, 2015.
Short summary
Based on ultra-high-resolution mass spectrometry analysis, we found that β-pinene oxidation-derived highly oxygenated organic molecules (HOMs) exhibit higher yield at high ozone concentration, while limonene oxidation-derived HOMs exhibit higher yield at moderate ozone concentration. The distinct molecular response of HOMs and low-volatile species in different biogenic secondary organic aerosols to ozone concentrations provides a new clue for more accurate air quality prediction and management.
Based on ultra-high-resolution mass spectrometry analysis, we found that β-pinene...
Altmetrics
Final-revised paper
Preprint