Articles | Volume 22, issue 10
31 May 2022
Research article | 31 May 2022
Reversible and irreversible gas–particle partitioning of dicarbonyl compounds observed in the real atmosphere
Jingcheng Hu et al.
No articles found.
Jiayun Xu, Zhongming Chen, Xuan Qin, and Ping Dong
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
We investigated the photooxidation of isoprene in the presence of water. We found that water enhanced the formation of methacrolein and methyl vinyl ketone in the first-generation reactions by changing the structures of the reaction intermediates and raised formic acid and acetic acid yields considerably in the multi-generation reactions. The results of this study help understand the fate of isoprene in the atmosphere and improve the effect of the atmospheric simulations.
Yiwei Gong and Zhongming Chen
Atmos. Chem. Phys., 21, 813–829,Short summary
Stabilized Criegee intermediates (SCIs) are important factors in estimating aerosol formation in the atmosphere. Here the results show that SCIs account for more than 60 % of aerosol formation in limonene ozonolysis and water is an uncertainty in SCI performances. The aerosol formation potential of SCIs under high-humidity conditions is double that under dry and low-humidity conditions, suggesting SCI reactions are still important in contributing to aerosols at high relative humidity.
Xiaoning Xuan, Zhongming Chen, Yiwei Gong, Hengqing Shen, and Shiyi Chen
Atmos. Chem. Phys., 20, 5513–5526,Short summary
In this study, we found that the effective field-derived Henry's law constant for the ground rainwater and the gas-phase H2O2 was about 2.5 times that of the theoretical value, and the effective gas–particle partitioning coefficient for the aerosol particle and the gas-phase H2O2 was 4 orders of magnitude higher than the theoretical one. We suggested the missing source of H2O2 in the particulate phase, e.g. the contribution from the decomposition/hydrolysis of organic peroxides.
Yiwei Gong, Zhongming Chen, and Huan Li
Atmos. Chem. Phys., 18, 15105–15123,Short summary
In limonene ozonolysis, the endocyclic double bond is inclined to generate hydroxy radicals, while the exocyclic double bond has a higher fraction of forming stabilized Criegee intermediates. The oxidation that happens on the exocyclic double bond greatly contributes to the organic peroxides, which account for a considerable proportion of secondary organic aerosol. Terpenes with multiple double bonds may have more complex effects on the atmosphere than previously thought.
Yin Wang, Zhongming Chen, Qinqin Wu, Hao Liang, Liubin Huang, Huan Li, Keding Lu, Yusheng Wu, Huabin Dong, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 16, 10985–11000,Short summary
Comparison of modeled and measured peroxide concentrations at a rural site in the summer North China Plain demonstrated an underestimation during biomass burning events and an overestimation on haze days, which were related to the direct production of peroxides from biomass burning and the heterogeneous uptake of peroxides by aerosols, respectively. Our findings are of great significance for comprehensively understanding the chemical budget of atmospheric peroxides in detail.
Huan Li, Zhongming Chen, Liubin Huang, and Dao Huang
Atmos. Chem. Phys., 16, 1837–1848,Short summary
The formation, gas-particle partitioning, and evolution of atmospheric organic peroxides are unclear. We investigated the ozonolysis of α-pinene, and focused on peroxides. We found that gas-particle partitioning coefficients of peroxides are much higher than the values from our theoretical prediction, and some gaseous peroxides undergo rapid heterogeneous decomposition on SOA particles in the presence of water vapor, resulting in the additional production of hydrogen peroxide.
Q. Q. Wu, L. B. Huang, H. Liang, Y. Zhao, D. Huang, and Z. M. Chen
Atmos. Chem. Phys., 15, 6851–6866,Short summary
The present study provides the first measurement for the uptake coefficient of gaseous peroxide compounds including peroxyacetic acid and hydrogen peroxide on the ambient particles (PM2.5 and Asian Storm Dust) over a wide range of relative humidity. The measured uptake coefficient values suggest that the heterogeneous reaction on the ambient particles plays an important role in the atmospheric budgets of peroxide compounds and potentially affects the components of aerosols in the atmosphere.
H. Liang, Z. M. Chen, D. Huang, Q. Q. Wu, and L. B. Huang
Atmos. Chem. Phys. Discuss.,
Revised manuscript not acceptedShort summary
The present field measurements have provided strong evidence for the existence of peroxyformic acid (HC(O)OOH) in the atmosphere for the first time. Moreover, the potential impact of peroxyformic acid chemistry on the formic acid production and the radical budget has been evaluated on the basis of model calculations. Our findings are of importance for a full understanding of the cycling of oxidants and the source of organic acids in the atmosphere.
H. Liang, Z. M. Chen, D. Huang, Y. Zhao, and Z. Y. Li
Atmos. Chem. Phys., 13, 11259–11276,
R. Zhang, J. Jing, J. Tao, S.-C. Hsu, G. Wang, J. Cao, C. S. L. Lee, L. Zhu, Z. Chen, Y. Zhao, and Z. Shen
Atmos. Chem. Phys., 13, 7053–7074,
D. Huang, Z. M. Chen, Y. Zhao, and H. Liang
Atmos. Chem. Phys., 13, 5671–5683,
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)Contribution of wood burning to exposures of PAHs and oxy-PAHs in Eastern SwedenChemical evolution of secondary organic aerosol tracers during high-PM2.5 episodes at a suburban site in Hong Kong over 4 months of continuous measurementSources and processes of water-soluble and water-insoluble organic aerosol in cold season in Beijing, ChinaMeasurement report: Size-resolved chemical characterisation of aerosols in low-income urban settlements in South AfricaMeasurement report: Large contribution of biomass burning and aqueous-phase processes to the wintertime secondary organic aerosol formation in Xi'an, Northwest ChinaPM10 variation, composition, and source analysis in Tuscany (Italy) following the COVID-19 lockdown restrictionsEmissions of organic compounds from western US wildfires and their near-fire transformationsA comprehensive study about the in-cloud processing of nitrate through coupled measurements of individual cloud residuals and cloud waterIron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubilityMeasurement report: On the contribution of long-distance transport to the secondary aerosol formation and agingFactors controlling atmospheric DMS and its oxidation products (MSA and nssSO42−) in the aerosol at Terra Nova Bay, AntarcticaParticle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sourcesPolycyclic aromatic hydrocarbons (PAHs) and their alkylated, nitrated and oxygenated derivatives in the atmosphere over the Mediterranean and Middle East seasNine-year trends of PM10 sources and oxidative potential in a rural background site in FranceDramatic changes in atmospheric pollution source contributions for a coastal megacity in northern China from 2011 to 2020Understanding aerosol composition in a tropical inter-Andean valley impacted by agro-industrial and urban emissionsMeasurement report: The importance of biomass burning in light extinction and direct radiative effect of urban aerosol during the COVID-19 lockdown in Xi'an, ChinaChemical properties, sources and size-resolved hygroscopicity of submicron black-carbon-containing aerosols in urban ShanghaiMeasurement report: Effects of anthropogenic emissions and environmental factors on the formation of biogenic secondary organic aerosol (BSOA) in a coastal city of southeastern ChinaHighly time-resolved chemical speciation and source apportionment of organic aerosol components in Delhi, India, using extractive electrospray ionization mass spectrometryThe chemical composition and mixing state of BC-containing particles and the implications on light absorption enhancementEvidence of haze-driven secondary production of supermicrometer aerosol nitrate and sulfate in size distribution data in South KoreaSpatial variability of air pollutants in a megacity characterized by mobile measurementsLinking Switzerland's PM10 and PM2.5 oxidative potential (OP) with emission sourcesMolecular characteristics, sources, and formation pathways of organosulfur compounds in ambient aerosol in Guangzhou, South ChinaEvolution of source attributed organic aerosols and gases in a megacity of central ChinaMeasurement report: Hygroscopic growth of ambient fine particles measured at five sites in ChinaMeasurement report: Optical properties and sources of water-soluble brown carbon in Tianjin, North China – insights from organic molecular compositionsMeasurement report: characterization and sources of the ambient secondary organic carbon in a Chinese megacity over five years from 2016 to 2020Trends in secondary inorganic aerosol pollution in China and its responses to emission controls of precursors in wintertimeMeasurement report: Source apportionment of carbonaceous aerosol using dual-carbon isotopes (13C and 14C) and levoglucosan in three northern Chinese cities during 2018–2019Chemically speciated mass size distribution, particle density, shape and origin of non-refractory PM1 measured at a rural background site in central EuropeOffline analysis of the chemical composition and hygroscopicity of submicrometer aerosol at an Asian outflow receptor site and comparison with online measurementsHigh number concentrations of transparent exopolymer particles in ambient aerosol particles and cloud water – a case study at the tropical Atlantic OceanMicro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North AtlanticOxidation pathways and emission sources of atmospheric particulate nitrate in Seoul: based on δ15N and Δ17O measurementsMeasurement report: Characterization and source apportionment of coarse particulate matter in Hong Kong: insights into the constituents of unidentified mass and source origins in a coastal city in southern ChinaThe impact of atmospheric motion on source-specific black carbon and the induced direct radiative effect over a river-valley regionThe optical properties and in-situ observational evidence for the formation of brown carbon in cloudsHigh atmospheric oxidation capacity drives wintertime nitrate pollution in the eastern Yangtze River Delta of ChinaDevelopment and evolution of an anomalous Asian dust event across Europe in March 2020The effect of clouds and precipitation on the aerosol concentrations and composition in a boreal forest environmentContributions of primary sources to submicron organic aerosols in Delhi, IndiaWhat caused a record high PM10 episode in northern Europe in October 2020?Sensitivity of low-level clouds and precipitation to anthropogenic aerosol emission in southern West Africa: a DACCIWA case studyPan-Arctic seasonal cycles and long-term trends of aerosol properties from 10 observatoriesAnalysis of reduced and oxidized nitrogen-containing organic compounds at a coastal site in summer and winterMeasurement Report: Ten-year trend of PM2.5 major components and source tracers from 2008 to 2017 in an urban site of Hong Kong, ChinaTechnical note: Use of PM2.5 to CO ratio as a tracer of wildfire smoke in urban areasSources and processes of iron aerosols in a megacity in Eastern China
Hwanmi Lim, Sanna Silvergren, Silvia Spinicci, Farshid Mashayekhy Rad, Ulrika Nilsson, Roger Westerholm, and Christer Johansson
Atmos. Chem. Phys., 22, 11359–11379,Short summary
Air pollutants from wood burning become more important as other regulated emissions are being reduced, e.g. combustion of diesel. We analysed particles in residential areas and found that local wood burning was the most important source of polycyclic aromatic hydrocarbons (PAHs). Specific tracers were used to separate wood combustion from other contributions. Calculations of population exposure showed that the mix of PAHs may cause 13 cancer cases per 0.1 million inhabitants.
Qiongqiong Wang, Shan Wang, Yuk Ying Cheng, Hanzhe Chen, Zijing Zhang, Jinjian Li, Dasa Gu, Zhe Wang, and Jian Zhen Yu
Atmos. Chem. Phys., 22, 11239–11253,Short summary
Secondary organic aerosol (SOA) is often enhanced during fine-particulate-matter (PM2.5) episodes. We examined bi-hourly measurements of SOA molecular tracers in suburban Hong Kong during 11 city-wide PM2.5 episodes. The tracers showed regional characteristics for both anthropogenic and biogenic SOA as well as biomass-burning-derived SOA. Multiple tracers of the same precursor revealed the dominance of low-NOx formation pathways for isoprene SOA and less-aged monoterpene SOA during winter.
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,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.
Constance K. Segakweng, Pieter G. van Zyl, Cathy Liousse, Johan P. Beukes, Jan-Stefan Swartz, Eric Gardrat, Maria Dias-Alves, Brigitte Language, Roelof P. Burger, and Stuart J. Piketh
Atmos. Chem. Phys., 22, 10291–10317,Short summary
A detailed size-resolved assessment of the chemical characteristics of outdoor and indoor aerosols collected in low-income urban settlements in South Africa indicated the significance of household combustion for cooking and space heating – an important source of pollutants in the developing world – to atmospheric chemical composition. The regional impact of industrial sources in the highly industrialised and densely populated north-eastern interior of South Africa was also evident.
Jing Duan, Ru-Jin Huang, Yifang Gu, Chunshui Lin, Haobin Zhong, Wei Xu, Quan Liu, Yan You, Jurgita Ovadnevaite, Darius Ceburnis, Thorsten Hoffmann, and Colin O'Dowd
Atmos. Chem. Phys., 22, 10139–10153,Short summary
Biomass-burning-influenced oxygenated organic aerosol (OOA-BB), formed from the photochemical oxidation and aging of biomass burning OA (BBOA), was resolved in urban Xi’an. The aqueous-phase processed oxygenated OA (aq-OOA) concentration was more dependent on secondary inorganic aerosol (SIA) content and aerosol liquid water content (ALWC). The increased aq-OOA contribution during SIA-enhanced periods likely reflects OA evolution due to the addition of alcohol or peroxide groups
Fabio Giardi, Silvia Nava, Giulia Calzolai, Giulia Pazzi, Massimo Chiari, Andrea Faggi, Bianca Patrizia Andreini, Chiara Collaveri, Elena Franchi, Guido Nincheri, Alessandra Amore, Silvia Becagli, Mirko Severi, Rita Traversi, and Franco Lucarelli
Atmos. Chem. Phys., 22, 9987–10005,Short summary
The restriction measures adopted to contain the COVID-19 virus offered a unique opportunity to study urban particulate emissions in the near absence of traffic, which is one of the main emission sources in the urban environment. However, the drastic decrease in this source of particulate matter during the months of national lockdown did not lead to an equal decrease in the total particulate load. This is due to the inverse behavior shown by different sources, especially secondary sources.
Yutong Liang, Christos Stamatis, Edward C. Fortner, Rebecca A. Wernis, Paul Van Rooy, Francesca Majluf, Tara I. Yacovitch, Conner Daube, Scott C. Herndon, Nathan M. Kreisberg, Kelley C. Barsanti, and Allen H. Goldstein
Atmos. Chem. Phys., 22, 9877–9893,Short summary
This article reports the measurements of organic compounds emitted from western US wildfires. We identified and quantified 240 particle-phase compounds and 72 gas-phase compounds emitted in wildfire and related the emissions to the modified combustion efficiency. Higher emissions of diterpenoids and monoterpenes were observed, likely due to distillation from unburned heated vegetation. Our results can benefit future source apportionment and modeling studies as well as exposure assessments.
Guohua Zhang, Xiaodong Hu, Wei Sun, Yuxiang Yang, Ziyong Guo, Yuzhen Fu, Haichao Wang, Shengzhen Zhou, Lei Li, Mingjin Tang, Zongbo Shi, Duohong Chen, Xinhui Bi, and Xinming Wang
Atmos. Chem. Phys., 22, 9571–9582,Short summary
We show a significant enhancement of nitrate mass fraction in cloud water and relative intensity of nitrate in the cloud residual particles and highlight that hydrolysis of N2O5 serves as the critical route for the in-cloud formation of nitrate, even during the daytime. Given that N2O5 hydrolysis acts as a major sink of NOx in the atmosphere, further model updates may improve our understanding about the processes contributing to nitrate production in cloud and the cycling of odd nitrogen.
Kohei Sakata, Minako Kurisu, Yasuo Takeichi, Aya Sakaguchi, Hiroshi Tanimoto, Yusuke Tamenori, Atsushi Matsuki, and Yoshio Takahashi
Atmos. Chem. Phys., 22, 9461–9482,Short summary
Iron (Fe) species in size-fractionated aerosol particles collected in the western Pacific Ocean were determined to identify factors controlling fractional Fe solubility. We found that labile Fe was mainly present in submicron aerosol particles, and the Fe species were ferric organic complexes combined with humic-like substances (Fe(III)-HULIS). The Fe(III)-HULIS was formed by atmospheric processes. Thus, atmospheric processes play a significant role in controlling Fe solubility.
Haobin Zhong, Ru-Jin Huang, Chunshui Lin, Wei Xu, Jing Duan, Yifang Gu, Wei Huang, Haiyan Ni, Chongshu Zhu, Yan You, Yunfei Wu, Renjian Zhang, Jurgita Ovadnevaite, Darius Ceburnis, and Colin D. O'Dowd
Atmos. Chem. Phys., 22, 9513–9524,Short summary
To investigate the physico-chemical properties of aerosol transported from major pollution regions in China, observations were conducted ~200 m above the ground at the junction location of the two key pollution areas. We found that the formation efficiency, oxidation state and production rate of secondary aerosol were different in the transport sectors from different pollution regions, and they were largely enhanced by the regional long-distance transport.
Silvia Becagli, Elena Barbaro, Simone Bonamano, Laura Caiazzo, Alcide di Sarra, Matteo Feltracco, Paolo Grigioni, Jost Heintzenberg, Luigi Lazzara, Michel Legrand, Alice Madonia, Marco Marcelli, Chiara Melillo, Daniela Meloni, Caterina Nuccio, Giandomenico Pace, Ki-Tae Park, Suzanne Preunkert, Mirko Severi, Marco Vecchiato, Roberta Zangrando, and Rita Traversi
Atmos. Chem. Phys., 22, 9245–9263,Short summary
Measurements of phytoplanktonic dimethylsulfide and its oxidation products in the Antarctic atmosphere allow us to understand the role of the oceanic (sea ice melting, Chl α and dimethylsulfoniopropionate) and atmospheric (wind direction and speed, humidity, solar radiation and transport processes) factors in the biogenic aerosol formation, concentration and characteristic ratio between components in an Antarctic coastal site facing the polynya of the Ross Sea.
Zezhen Cheng, Megan Morgenstern, Bo Zhang, Matthew Fraund, Nurun Nahar Lata, Rhenton Brimberry, Matthew A. Marcus, Lynn Mazzoleni, Paulo Fialho, Silvia Henning, Birgit Wehner, Claudio Mazzoleni, and Swarup China
Atmos. Chem. Phys., 22, 9033–9057,Short summary
We observed a high abundance of liquid and internally mixed particles in samples collected in the North Atlantic free troposphere during summer. We also found several solid and semisolid particles for different emission sources and transport patterns. Our results suggest that considering the mixing state, emission source, and transport patterns of particles is necessary to estimate their phase state in the free troposphere, which is critical for predicting their effects on climate.
Marco Wietzoreck, Marios Kyprianou, Benjamin A. Musa Bandowe, Siddika Celik, John N. Crowley, Frank Drewnick, Philipp Eger, Nils Friedrich, Minas Iakovides, Petr Kukučka, Jan Kuta, Barbora Nežiková, Petra Pokorná, Petra Přibylová, Roman Prokeš, Roland Rohloff, Ivan Tadic, Sebastian Tauer, Jake Wilson, Hartwig Harder, Jos Lelieveld, Ulrich Pöschl, Euripides G. Stephanou, and Gerhard Lammel
Atmos. Chem. Phys., 22, 8739–8766,Short summary
A unique dataset of concentrations and sources of polycyclic aromatic hydrocarbons (PAHs) and their alkylated, oxygenated and nitrated derivatives, in total 74 individual species, in the marine atmosphere is presented. Exposure to these substances poses a major health risk. We found very low concentrations over the Arabian Sea, while both local and long-range-transported pollution caused elevated levels over the Mediterranean Sea and the Arabian Gulf.
Lucille Joanna Borlaza, Samuël Weber, Anouk Marsal, Gaëlle Uzu, Véronique Jacob, Jean-Luc Besombes, Mélodie Chatain, Sébastien Conil, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 22, 8701–8723,Short summary
A 9-year dataset of the chemical and oxidative potential (OP) of PM10 was investigated at a rural background site. Extensive source apportionment led to identification of differences in source impacts between mass and OP, underlining the importance of PM redox activity when considering health effects. The influence of mixing and ageing processes was also tackled. Traffic contributions have decreased here over the years, attributed to regulations limiting vehicular emissions in bigger cities.
Baoshuang Liu, Yanyang Wang, He Meng, Qili Dai, Liuli Diao, Jianhui Wu, Laiyuan Shi, Jing Wang, Yufen Zhang, and Yinchang Feng
Atmos. Chem. Phys., 22, 8597–8615,Short summary
Understanding effectiveness of air pollution regulatory measures is critical for control policy. Machine learning and dispersion-normalized approaches were applied to decouple meteorologically deduced variations in Qingdao, China. Most pollutant concentrations decreased substantially after the Clean Air Action Plan. The largest emission reduction was from coal combustion and steel-related smelting. Qingdao is at risk of increased emissions from increased vehicular population and ozone pollution.
Lady Mateus-Fontecha, Angela Vargas-Burbano, Rodrigo Jimenez, Nestor Y. Rojas, German Rueda-Saa, Dominik van Pinxteren, Manuela van Pinxteren, Khanneh Wadinga Fomba, and Hartmut Herrmann
Atmos. Chem. Phys., 22, 8473–8495,Short summary
This study reports the chemical composition of regionally representative PM2.5 in an area densely populated and substantially industrialized, located in the inter-Andean valley, with the highest sugarcane yield in the world and where sugarcane is burned and harvested year round. We found that sugarcane burning is not portrayed as a distinguishable sample composition component. Instead, the composition analysis revealed multiple associations among sugarcane burning components and other sources.
Jie Tian, Qiyuan Wang, Huikun Liu, Yongyong Ma, Suixin Liu, Yong Zhang, Weikang Ran, Yongming Han, and Junji Cao
Atmos. Chem. Phys., 22, 8369–8384,Short summary
We investigated aerosol optical properties and the direct radiative effect (DRE) at an urban site in China before and during the COVID-19 lockdown. The total light extinction coefficient (bext) decreased under emission control measures; however, bext from biomass burning increased due to the undiminished need for residential cooking and heating. Biomass burning, rather than traffic-related emissions, became the largest positive effect contributor to aerosol DRE in the lockdown.
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,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.
Youwei Hong, Xinbei Xu, Dan Liao, Taotao Liu, Xiaoting Ji, Ke Xu, Chunyang Liao, Ting Wang, Chunshui Lin, and Jinsheng Chen
Atmos. Chem. Phys., 22, 7827–7841,Short summary
Secondary organic aerosol (SOA) simulation remains uncertain, due to the unknown SOA formation mechanisms. Aerosol samples with a 4 h time resolution were collected, along with online measurements of aerosol chemical compositions and meteorological parameters. We found that anthropogenic emissions, atmospheric oxidation capacity and halogen chemistry have significant effects on the formation of biogenic SOA (BSOA). The findings of this study are helpful to better explore the missed SOA sources.
Varun Kumar, Stamatios Giannoukos, Sophie L. Haslett, Yandong Tong, Atinderpal Singh, Amelie Bertrand, Chuan Ping Lee, Dongyu S. Wang, Deepika Bhattu, Giulia Stefenelli, Jay S. Dave, Joseph V. Puthussery, Lu Qi, Pawan Vats, Pragati Rai, Roberto Casotto, Rangu Satish, Suneeti Mishra, Veronika Pospisilova, Claudia Mohr, David M. Bell, Dilip Ganguly, Vishal Verma, Neeraj Rastogi, Urs Baltensperger, Sachchida N. Tripathi, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 22, 7739–7761,Short summary
Here we present source apportionment results from the first field deployment in Delhi of an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF). The EESI-TOF is a recently developed instrument capable of providing uniquely detailed online chemical characterization of organic aerosol (OA), in particular the secondary OA (SOA) fraction. Here, we are able to apportion not only primary OA but also SOA to specific sources, which is performed for the first time in Delhi.
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,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.
Joseph S. Schlosser, Connor Stahl, Armin Sorooshian, Yen Thi-Hoang Le, Ki-Joon Jeon, Peng Xian, Carolyn E. Jordan, Katherine R. Travis, James H. Crawford, Sung Yong Gong, Hye-Jung Shin, In-Ho Song, and Jong-sang Youn
Atmos. Chem. Phys., 22, 7505–7522,Short summary
During a major haze pollution episode in March 2019, anthropogenic emissions were dominant in the boundary layer over Incheon and Seoul, South Korea. Using supermicrometer and submicrometer size- and chemistry-resolved aerosol particle measurements taken during this haze pollution period, this work shows that local emissions and a shallow boundary layer, enhanced humidity, and low temperature promoted local heterogeneous formation of secondary inorganic and organic aerosol species.
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,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.
Stuart K. Grange, Gaëlle Uzu, Samuël Weber, Jean-Luc Jaffrezo, and Christoph Hueglin
Atmos. Chem. Phys., 22, 7029–7050,Short summary
Oxidative potential (OP), a biologically relevant metric for particulate matter (PM), was linked to PM10 and PM2.5 sources and constituents across Switzerland between 2018 and 2019. Wood burning and non-exhaust traffic emissions were identified as key processes that led to enhanced OP. Therefore, the make-up of the PM mix was very important for OP. The results highlight the importance of the management of wood burning and non-exhaust emissions to reduce OP, and presumably biological harm.
Hongxing Jiang, Jun Li, Jiao Tang, Min Cui, Shizhen Zhao, Yangzhi Mo, Chongguo Tian, Xiangyun Zhang, Bin Jiang, Yuhong Liao, Yingjun Chen, and Gan Zhang
Atmos. Chem. Phys., 22, 6919–6935,Short summary
We conducted field observation employing Fourier transform ion cyclotron resonance mass spectrometry to characterize the molecular composition and major formation pathways or sources of organosulfur compounds in Guangzhou, where is heavily influenced by biogenic–anthropogenic interactions and has high relative humidity and temperature. We suggested that heterogeneous reactions such as SO2 uptake and heterogeneous oxidations are important to the molecular variations of organosulfur compounds.
Siyuan Li, Dantong Liu, Shaofei Kong, Yangzhou Wu, Kang Hu, Huang Zheng, Yi Cheng, Shurui Zheng, Xiaotong Jiang, Shuo Ding, Dawei Hu, Quan Liu, Ping Tian, Delong Zhao, and Jiujiang Sheng
Atmos. Chem. Phys., 22, 6937–6951,Short summary
The understanding of secondary organic aerosols is hindered by the aerosol–gas evolution by different oxidation mechanisms. By concurrently measuring detailed mass spectra of aerosol and gas phases in a megacity online, we identified the primary and secondary source sectors and investigated the transformation between gas and aerosol phases influenced by photooxidation and moisture. The results will help us to understand the respective evolution of major sources in a typical urban environment.
Lu Chen, Fang Zhang, Dongmei Zhang, Xinming Wang, Wei Song, Jieyao Liu, Jingye Ren, Sihui Jiang, Xue Li, and Zhanqing Li
Atmos. Chem. Phys., 22, 6773–6786,Short summary
Aerosol hygroscopicity is critical when evaluating its effect on visibility and climate. Here, the size-resolved particle hygroscopicity at five sites in China is characterized using field measurements. We show the distinct behavior of hygroscopic particles during pollution evolution among the five sites. Moreover, different hygroscopic behavior during NPF events were also observed. The dataset is helpful for understanding the spatial variability in particle composition and formation mechanisms.
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,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.
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. Discuss.,
Revised manuscript accepted for ACPShort summary
In this study, we report a 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 SOC, in one of the largest megacities in the world and are helpful to develop pollution control measures from a long-term planning perspective.
Fanlei Meng, Yibo Zhang, Jiahui Kang, Mathew R. Heal, Stefan Reis, Mengru Wang, Lei Liu, Kai Wang, Shaocai Yu, Pengfei Li, Jing Wei, Yong Hou, Ying Zhang, Xuejun Liu, Zhenling Cui, Wen Xu, and Fusuo Zhang
Atmos. Chem. Phys., 22, 6291–6308,Short summary
PM2.5 pollution is a pressing environmental issue threatening human health and food security globally. We combined a meta-analysis of nationwide measurements and air quality modeling to identify efficiency gains by striking a balance between controlling NH3 and acid gas emissions. Persistent secondary inorganic aerosol pollution in China is limited by acid gas emissions, while an additional control on NH3 emissions would become more important as reductions in SO2 and NOx emissions progress.
Huiyizhe Zhao, Zhenchuan Niu, Weijian Zhou, Sen Wang, Xue Feng, Shugang Wu, Xuefeng Lu, and Hua Du
Atmos. Chem. Phys., 22, 6255–6274,Short summary
In this study, we investigated the characteristics and changes in the sources of carbonaceous aerosols in northern Chinese cities using dual-carbon isotopes (13C and 14C) and levoglucosan during 2018 to 2019 and compared them with the research in previous decades. The results show that the contribution of fossil sources has decreased (6–16%) significantly, and non-fossil sources have become the main part of carbonaceous aerosols, which verified the effectiveness of air quality management.
Petra Pokorná, Naděžda Zíková, Petr Vodička, Radek Lhotka, Saliou Mbengue, Adéla Holubová Šmejkalová, Véronique Riffault, Jakub Ondráček, Jaroslav Schwarz, and Vladimír Ždímal
Atmos. Chem. Phys., 22, 5829–5858,Short summary
By examining individual episodes of high mass and number concentrations, we show that the seasonality in the physicochemical properties of aerosol particles was caused by the sources' diversity and was related to the different air masses and meteorology. We also confirmed the relation between particle size and age that is reflected in oxidation state and shape (difference in densities; effective vs. material). The results have general validity and thus transcend the study regional character.
Yange Deng, Hiroaki Fujinari, Hikari Yai, Kojiro Shimada, Yuzo Miyazaki, Eri Tachibana, Dhananjay K. Deshmukh, Kimitaka Kawamura, Tomoki Nakayama, Shiori Tatsuta, Mingfu Cai, Hanbing Xu, Fei Li, Haobo Tan, Sho Ohata, Yutaka Kondo, Akinori Takami, Shiro Hatakeyama, and Michihiro Mochida
Atmos. Chem. Phys., 22, 5515–5533,Short summary
Offline analyses of the hygroscopicity and composition of atmospheric aerosols are complementary to online analyses in view of the applicability to broader sizes, specific compound groups, and investigations at remote sites. This offline study characterized the composition of water-soluble matter in aerosols and their humidity-dependent hygroscopicity on Okinawa, a receptor site of East Asian outflow. Further, comparison with online analyses showed the appropriateness of the offline method.
Manuela van Pinxteren, Tiera-Brandy Robinson, Sebastian Zeppenfeld, Xianda Gong, Enno Bahlmann, Khanneh Wadinga Fomba, Nadja Triesch, Frank Stratmann, Oliver Wurl, Anja Engel, Heike Wex, and Hartmut Herrmann
Atmos. Chem. Phys., 22, 5725–5742,Short summary
A class of marine particles (transparent exopolymer particles, TEPs) that is ubiquitously found in the world oceans was measured for the first time in ambient marine aerosol particles and marine cloud waters in the tropical Atlantic Ocean. TEPs are likely to have good properties for influencing clouds. We show that TEPs are transferred from the ocean to the marine atmosphere via sea-spray formation and our results suggest that they can also form directly in aerosol particles and in cloud water.
Daniel A. Knopf, Joseph C. Charnawskas, Peiwen Wang, Benny Wong, Jay M. Tomlin, Kevin A. Jankowski, Matthew Fraund, Daniel P. Veghte, Swarup China, Alexander Laskin, Ryan C. Moffet, Mary K. Gilles, Josephine Y. Aller, Matthew A. Marcus, Shira Raveh-Rubin, and Jian Wang
Atmos. Chem. Phys., 22, 5377–5398,Short summary
Marine boundary layer aerosols collected in the remote region of the eastern North Atlantic induce immersion freezing and deposition ice nucleation under typical mixed-phase and cirrus cloud conditions. Corresponding ice nucleation parameterizations for model applications have been derived. Chemical imaging of ambient aerosol and ice-nucleating particles demonstrates that the latter is dominated by sea salt and organics while also representing a major particle type in the particle population.
Saehee Lim, Meehye Lee, Joel Savarino, and Paolo Laj
Atmos. Chem. Phys., 22, 5099–5115,Short summary
We determined δ15N(NO3−) and Δ17O(NO3−) of PM2.5 in Seoul during 2018–2019 and estimated quantitatively the contribution of oxidation pathways to NO3− formation and NOx emission sources. The nighttime pathway played a significant role in NO3− formation during the winter, and its contribution further increased up to 70 % on haze days when PM2.5 was greater than 75 µg m−3. Vehicle emissions were confirmed as a main NO3− source with an increasing contribution from coal combustion in winter.
Yee Ka Wong, Kin Man Liu, Claisen Yeung, Kenneth K. M. Leung, and Jian Zhen Yu
Atmos. Chem. Phys., 22, 5017–5031,Short summary
Coarse particulate matter (PM) has been shown to cause adverse health impacts, but compared to PM2.5, the source of coarse PM is less studied through field measurements. We collected chemical composition data for coarse PM in Hong Kong for a 1-year period. Using statistical models, we found that regional transport of fugitive dust is responsible for the elevated coarse PM. This work sets an example of how field measurements can be effectively utilized for evidence-based policymaking.
Huikun Liu, Qiyuan Wang, Suixin Liu, Bianhong Zhou, Yao Qu, Jie Tian, Ting Zhang, Yongming Han, and Junji Cao
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Atmospheric motion plays an important role in the mass concentration and the direct radiative effect (DRE) of black carbon (BC). The finding from this study elaborated the impacts of different scales of atmospheric motion on source-specific BCs and their DRE, which revealed the disproportional change between BC mass concentration and its DRE, and highlighted the enhanced DRE efficiency of BC during the regional transport which could lead to greater climatic consequences in receptor regions.
Ziyong Guo, Yuxiang Yang, Xiaodong Hu, Xiaocong Peng, Yuzhen Fu, Wei Sun, Guohua Zhang, Duohong Chen, Xinhui Bi, Xinming Wang, and Ping'an Peng
Atmos. Chem. Phys., 22, 4827–4839,Short summary
We show that in-cloud aqueous processing facilitates the formation of brown carbon (BrC), based on the simultaneous measurements of the light-absorption properties of the cloud residuals, cloud interstitial, and cloud-free particles. While extensive laboratory evidence indicated the formation of BrC in aqueous phase, our study represents the first attempt to show the possibility in real clouds, which would have potential implications in the atmospheric evolution and radiation forcing of BrC.
Han Zang, Yue Zhao, Juntao Huo, Qianbiao Zhao, Qingyan Fu, Yusen Duan, Jingyuan Shao, Cheng Huang, Jingyu An, Likun Xue, Ziyue Li, Chenxi Li, and Huayun Xiao
Atmos. Chem. Phys., 22, 4355–4374,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.
Laura Tositti, Erika Brattich, Claudio Cassardo, Pietro Morozzi, Alessandro Bracci, Angela Marinoni, Silvana Di Sabatino, Federico Porcù, and Alessandro Zappi
Atmos. Chem. Phys., 22, 4047–4073,Short summary
We present a thorough investigation of an anomalous transport of mineral dust over a region renowned for excess airborne particulate matter, the Italian Po Valley, which occurred in late March 2021. Both the origin of this dust outbreak, which was localized in central Asia (i.e., the so-called Aralkum Desert), and the upstream synoptic conditions, investigated here in extreme detail using multiple integrated observations including in situ measurements and remote sensing, were atypical.
Sini Isokääntä, Paul Kim, Santtu Mikkonen, Thomas Kühn, Harri Kokkola, Taina Yli-Juuti, Liine Heikkinen, Krista Luoma, Tuukka Petäjä, Zak Kipling, Daniel Partridge, and Annele Virtanen
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
This study employs airmass history analysis and observations to investigate how clouds and precipitation affect atmospheric aerosols during their transport to a boreal forest site. The mass concentrations of studied chemical species showed exponential decrease as a function accumulated rain along the airmass route. Our analysis revealed in-cloud sulfate formation, while no major changes in organic concentrations were seen. Most of the sulfate formed were distributed to particle sizes > 200 nm.
Sahil Bhandari, Zainab Arub, Gazala Habib, Joshua S. Apte, and Lea Hildebrandt Ruiz
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Here we determine the sources of primary organic aerosol in Delhi, India, in two different seasons. In winter, the main sources are traffic and biomass burning; in the summer, the main sources are traffic and cooking. We obtain this result by conducting source apportionment resolved by time of day, using data from and aerosol chemical speciation monitor. Results from this work can be used to better design policies that target sources of organic aerosol.
Christine D. Groot Zwaaftink, Wenche Aas, Sabine Eckhardt, Nikolaos Evangeliou, Paul Hamer, Mona Johnsrud, Arve Kylling, Stephen M. Platt, Kerstin Stebel, Hilde Uggerud, and Karl Espen Yttri
Atmos. Chem. Phys., 22, 3789–3810,Short summary
We investigate causes of a poor-air-quality episode in northern Europe in October 2020 during which EU health limits for air quality were vastly exceeded. Such episodes may trigger measures to improve air quality. Analysis based on satellite observations, transport simulations, and surface observations revealed two sources of pollution. Emissions of mineral dust in Central Asia and biomass burning in Ukraine arrived almost simultaneously in Norway, and transport continued into the Arctic.
Adrien Deroubaix, Laurent Menut, Cyrille Flamant, Peter Knippertz, Andreas H. Fink, Anneke Batenburg, Joel Brito, Cyrielle Denjean, Cheikh Dione, Régis Dupuy, Valerian Hahn, Norbert Kalthoff, Fabienne Lohou, Alfons Schwarzenboeck, Guillaume Siour, Paolo Tuccella, and Christiane Voigt
Atmos. Chem. Phys., 22, 3251–3273,Short summary
During the summer monsoon in West Africa, pollutants emitted in urbanized areas modify cloud cover and precipitation patterns. We analyze these patterns with the WRF-CHIMERE model, integrating the effects of aerosols on meteorology, based on the numerous observations provided by the Dynamics-Aerosol-Climate-Interactions campaign. This study adds evidence to recent findings that increased pollution levels in West Africa delay the breakup time of low-level clouds and reduce precipitation.
Julia Schmale, Sangeeta Sharma, Stefano Decesari, Jakob Pernov, Andreas Massling, Hans-Christen Hansson, Knut von Salzen, Henrik Skov, Elisabeth Andrews, Patricia K. Quinn, Lucia M. Upchurch, Konstantinos Eleftheriadis, Rita Traversi, Stefania Gilardoni, Mauro Mazzola, James Laing, and Philip Hopke
Atmos. Chem. Phys., 22, 3067–3096,Short summary
Long-term data sets of Arctic aerosol properties from 10 stations across the Arctic provide evidence that anthropogenic influence on the Arctic atmospheric chemical composition has declined in winter, a season which is typically dominated by mid-latitude emissions. The number of significant trends in summer is smaller than in winter, and overall the pattern is ambiguous with some significant positive and negative trends. This reflects the mixed influence of natural and anthropogenic emissions.
Jenna C. Ditto, Jo Machesky, and Drew R. Gentner
Atmos. Chem. Phys., 22, 3045–3065,Short summary
We analyzed gases and aerosols sampled in summer and winter in a coastal region that is often downwind of urban areas and observed large contributions of nitrogen-containing organic compounds influenced by a mix of biogenic, anthropogenic, and/or marine sources as well as photochemical and aqueous-phase atmospheric processes. The results show the prevalence of key reduced and oxidized nitrogen functional groups and advance knowledge on the chemical structure of nitrogen-containing compounds.
Wing Sze Chow, Kezheng Liao, X. H. Hilda Huang, Ka Fung Leung, Alexis K. H. Lau, and Jian Zhen Yu
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Long-term monitoring data of PM2.5 chemical composition provide essential information for evaluation and planning of control measures. We present here a 10-year (2008–2017) time series of PM2.5, its major components, and select source markers in an urban site in Hong Kong. The data set verified the success of local vehicular emission control measures as well as reduction of sulfate and regional sources such as industrial and coal combustion, and crop residue burning emissions over the decade.
Daniel Jaffe, Brendan Schnieder, and Daniel Inouye
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
In this manuscript we use commonly measured pollutants (PM2.5 and carbon monoxide) to develop a Monte Carlo simulation of the mixing of urban pollution with smoke. The simulations compare well with observations from a heavily impacted smoke site and show that we can use standard regulatory measurements to quantify the amount of smoke in urban areas.
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,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.
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The gas–particle partitioning process of glyoxal and methylglyoxal could contribute to secondary organic aerosol formation. Here, we launched five observations in different seasons and simultaneously measured glyoxal and methylglyoxal in the gas and particle phases. Compared to reversible pathways, irreversible pathways played a dominant role with a proportion of more than 90 % in the ambient atmosphere, and the proportion was influenced by relative humidity and inorganic components in aerosols.
The gas–particle partitioning process of glyoxal and methylglyoxal could contribute to secondary...