Articles | Volume 22, issue 8
https://doi.org/10.5194/acp-22-5685-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-22-5685-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
29 Apr 2022
Research article |
| 29 Apr 2022
| 29 Apr 2022
Chemical transformation of α-pinene-derived organosulfate via heterogeneous OH oxidation: implications for sources and environmental fates of atmospheric organosulfates
Rongshuang Xu
Earth System Science Programme, Faculty of Science, The Chinese
University of Hong Kong, Hong Kong, China
Sze In Madeleine Ng
Earth System Science Programme, Faculty of Science, The Chinese
University of Hong Kong, Hong Kong, China
Wing Sze Chow
Department of Chemistry, The Hong Kong University of Science and
Technology, Hong Kong, China
Yee Ka Wong
Division of Environment and Sustainability, The Hong Kong University
of Science and Technology, Hong Kong, China
Yuchen Wang
Department of Chemistry, The Hong Kong University of Science and
Technology, Hong Kong, China
Donger Lai
Earth System Science Programme, Faculty of Science, The Chinese
University of Hong Kong, Hong Kong, China
Zhongping Yao
State Key Laboratory of Chemical Biology and Drug Discovery and
Department of Applied Biology and Chemical Technology, The Hong Kong
Polytechnic University, Hong Kong, China
Pui-Kin So
The University Research Facility in Life Sciences, The Hong Kong
Polytechnic University, Hong Kong, China
Department of Chemistry, The Hong Kong University of Science and
Technology, Hong Kong, China
Man Nin Chan
CORRESPONDING AUTHOR
Earth System Science Programme, Faculty of Science, The Chinese
University of Hong Kong, Hong Kong, China
The Institute of Environment, Energy, and Sustainability, The Chinese
University of Hong Kong, Hong Kong, China
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We present simultaneous measurements of aerosol volatility and carbonaceous matters in Guangzhou, China, in Feb and Mar 2014 using a VTDMA and OC / EC analyzer. Low volatility particles with no significant evaporation at 300° C in the VTDMA contributed 5–15 % of number concentrations of the 40–300 nm particles. Mass closure suggests that non-volatile organic carbon, in addition to elemental carbon, was one of the components of the non-volatile residuals measured by the VTDMA in this study.
Cheng Wu and Jian Zhen Yu
Atmos. Chem. Phys., 16, 5453–5465, https://doi.org/10.5194/acp-16-5453-2016, https://doi.org/10.5194/acp-16-5453-2016, 2016
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Elemental carbon (EC) has been widely used as a tracer to estimate secondary organic carbon (SOC) from ambient EC and OC data. Key to the EC tracer method is to determine a proper primary OC / EC ratio at the observation site. We examine here a method that derives this ratio by seeking the minimum correlation between SOC and EC. This method has a clear quantitative criterion for the ratio derivation and is demonstrated to have superior accuracy over the commonly used approaches for SOC estimation.
Wei Deng, Qihou Hu, Tengyu Liu, Xinming Wang, Yanli Zhang, Xiang Ding, Yele Sun, Xinhui Bi, Jianzhen Yu, Weiqiang Yang, Xinyu Huang, Zhou Zhang, Zhonghui Huang, Quanfu He, A. Mellouki, and Christian George
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-50, https://doi.org/10.5194/acp-2016-50, 2016
Revised manuscript not accepted
T. Liu, X. Wang, Q. Hu, W. Deng, Y. Zhang, X. Ding, X. Fu, F. Bernard, Z. Zhang, S. Lü, Q. He, X. Bi, J. Chen, Y. Sun, J. Yu, P. Peng, G. Sheng, and J. Fu
Atmos. Chem. Phys., 16, 675–689, https://doi.org/10.5194/acp-16-675-2016, https://doi.org/10.5194/acp-16-675-2016, 2016
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The formation of SOA and sulfate aerosols from the photooxidation of gasoline vehicle exhaust (GVE) when mixing with SO2 was investigated in a smog chamber. We found that the presence of GVE enhanced the conversion of SO2 to sulfate predominantly through reactions with stabilized Criegee intermediates. On the other hand, the elevated particle acidity enhanced the SOA production from GVE. This study indicated that SO2 and GVE could enhance each other in forming secondary aerosols.
T. Liu, X. Wang, W. Deng, Q. Hu, X. Ding, Y. Zhang, Q. He, Z. Zhang, S. Lü, X. Bi, J. Chen, and J. Yu
Atmos. Chem. Phys., 15, 9049–9062, https://doi.org/10.5194/acp-15-9049-2015, https://doi.org/10.5194/acp-15-9049-2015, 2015
B. Y. Kuang, P. Lin, X. H. H. Huang, and J. Z. Yu
Atmos. Chem. Phys., 15, 1995–2008, https://doi.org/10.5194/acp-15-1995-2015, https://doi.org/10.5194/acp-15-1995-2015, 2015
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Humic-like substances (HULIS), the hydrophobic part of water soluble organic material, account for ~10% of PM2.5 mass in the Pearl River Delta, China. Source analysis using PM2.5 chemical composition data revealed that secondary formation process, biomass burning, and residual oil combustion from shipping as significant sources of HULIS. Vehicle emissions contributed little to HULIS. Primary sources of HULIS appeared to be linked to inefficient combustion.
X. H. H. Huang, Q. J. Bian, P. K. K. Louie, and J. Z. Yu
Atmos. Chem. Phys., 14, 9279–9293, https://doi.org/10.5194/acp-14-9279-2014, https://doi.org/10.5194/acp-14-9279-2014, 2014
Q. Bian, X. H. H. Huang, and J. Z. Yu
Atmos. Chem. Phys., 14, 9013–9027, https://doi.org/10.5194/acp-14-9013-2014, https://doi.org/10.5194/acp-14-9013-2014, 2014
X. Wang, T. Liu, F. Bernard, X. Ding, S. Wen, Y. Zhang, Z. Zhang, Q. He, S. Lü, J. Chen, S. Saunders, and J. Yu
Atmos. Meas. Tech., 7, 301–313, https://doi.org/10.5194/amt-7-301-2014, https://doi.org/10.5194/amt-7-301-2014, 2014
D. Wu, C. Wu, B. Liao, H. Chen, M. Wu, F. Li, H. Tan, T. Deng, H. Li, D. Jiang, and J. Z. Yu
Atmos. Chem. Phys., 13, 12257–12270, https://doi.org/10.5194/acp-13-12257-2013, https://doi.org/10.5194/acp-13-12257-2013, 2013
Y. J. Li, B. Y. L. Lee, J. Z. Yu, N. L. Ng, and C. K. Chan
Atmos. Chem. Phys., 13, 8739–8753, https://doi.org/10.5194/acp-13-8739-2013, https://doi.org/10.5194/acp-13-8739-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Enhanced sulfate formation in mixed biomass burning and sea-salt interactions mediated by photosensitization: effects of chloride, nitrogen-containing compounds, and atmospheric aging
Heterogeneous formation and light absorption of secondary organic aerosols from acetone photochemical reactions: remarkably enhancing effects of seeds and ammonia
Experimental observation of the impact of nanostructure on hygroscopicity and reactivity of fatty acid atmospheric aerosol proxies
Technical note: High-resolution analyses of concentrations and sizes of refractory black carbon particles deposited in northwestern Greenland over the past 350 years – Part 1: Continuous flow analysis of the SIGMA-D ice core using the wide-range Single-Particle Soot Photometer and a high-efficiency nebulizer
Particulate emissions from cooking: emission factors, emission dynamics, and mass spectrometric analysis for different cooking methods
Nocturnal atmospheric synergistic oxidation reduces the formation of low-volatility organic compounds from biogenic emissions
The interplay between aqueous replacement reaction and the phase state of internally mixed organic/ammonium aerosols
Measurement report: The Fifth International Workshop on Ice Nucleation phase 1 (FIN-01): intercomparison of single-particle mass spectrometers
Boosting aerosol surface effects: Strongly Enhanced Cooperative Surface Propensity of Atmospherically Relevant Organic Molecular Ions in Aqueous Solution
Characterization of the particle size distribution, mineralogy, and Fe mode of occurrence of dust-emitting sediments from the Mojave Desert, California, USA
The lifetimes and potential change in planetary albedo owing to the oxidation of organic films extracted from atmospheric aerosol by hydroyxl (OH) radical oxidation at the air-water interface of aerosol particles
Atmospheric oxidation of 1,3-butadiene: influence of acidity and relative humidity on SOA composition and air toxic compounds
Measurement Report: Changes of ammonia emissions since the 18th century in south-eastern Europe inferred from an Elbrus (Caucasus, Russia) ice core record
Measurement report: Effects of transition metal ions on the optical properties of humic-like substances (HULIS) reveal a structural preference – a case study of PM2.5 in Beijing, China
Exometabolomic exploration of culturable airborne microorganisms from an urban atmosphere
Probing Iceland's dust-emitting sediments: particle size distribution, mineralogy, cohesion, Fe mode of occurrence, and reflectance spectra signatures
Photoenhanced sulfate formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
Comparison of water-soluble and water-insoluble organic compositions attributing to different light absorption efficiency between residential coal and biomass burning emissions
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
Formation and loss of light absorbance by phenolic aqueous SOA by ●OH and an organic triplet excited state
Technical Note: A technique to convert NO2 to NO2− with S(IV) and its application to measuring nitrate photolysis
Distribution, chemical, and molecular composition of high and low molecular weight humic-like substances in ambient aerosols
Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics
Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole
Secondary organic aerosol formed by Euro 5 gasoline vehicle emissions: chemical composition and gas-to-particle phase partitioning
Assessment of the contribution of residential waste burning to ambient PM10 concentrations in Hungary and Romania
Source differences in the components and cytotoxicity of PM2.5 from automobile exhaust, coal combustion, and biomass burning contributing to urban aerosol toxicity
Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism
Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions
Temperature-dependent aqueous OH kinetics of C2–C10 linear and terpenoid alcohols and diols: new rate coefficients, structure–activity relationship, and atmospheric lifetimes
A possible unaccounted source of nitrogen-containing compound formation in aerosols: amines reacting with secondary ozonides
Seasonal variations in photooxidant formation and light absorption in aqueous extracts of ambient particles
Variability in sediment particle size, mineralogy, and Fe mode of occurrence across dust-source inland drainage basins: the case of the lower Drâa Valley, Morocco
Gas–particle partitioning of toluene oxidation products: an experimental and modeling study
Chemically speciated air pollutant emissions from open burning of household solid waste from South Africa
Bulk and molecular-level composition of primary organic aerosol from wood, straw, cow dung, and plastic burning
Volatile oxidation products and secondary organosiloxane aerosol from D5 + OH at varying OH exposures
Molecular fingerprints and health risks of smoke from home-use incense burning
High enrichment of heavy metals in fine particulate matter through dust aerosol generation
Production of ice-nucleating particles (INPs) by fast-growing phytoplankton
Technical note: In situ measurements and modelling of the oxidation kinetics in films of a cooking aerosol proxy using a quartz crystal microbalance with dissipation monitoring (QCM-D)
Contrasting impacts of humidity on the ozonolysis of monoterpenes: insights into the multi-generation chemical mechanism
Quantifying the seasonal variations in and regional transport of PM2.5 in the Yangtze River Delta region, China: characteristics, sources, and health risks
Opinion: Atmospheric multiphase chemistry – past, present, and future
Distinct photochemistry in glycine particles mixed with different atmospheric nitrate salts
Effects of storage conditions on the molecular-level composition of organic aerosol particles
Characterization of gas and particle emissions from open burning of household solid waste from South Africa
Chemically distinct particle-phase emissions from highly controlled pyrolysis of three wood types
Predicting photooxidant concentrations in aerosol liquid water based on laboratory extracts of ambient particles
Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic
Rongzhi Tang, Jialiang Ma, Ruifeng Zhang, Weizhen Cui, Yuanyuan Qin, Yangxi Chu, Yiming Qin, Alexander L. Vogel, and Chak K. Chan
Atmos. Chem. Phys., 25, 425–439, https://doi.org/10.5194/acp-25-425-2025, https://doi.org/10.5194/acp-25-425-2025, 2025
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This study provides laboratory evidence that the photosensitizers in biomass burning extracts can enhance sulfate formation in NaCl particles, primarily by triggering the formation of secondary oxidants under light and air conditions, with a lower contribution of direct photosensitization via triplets.
Si Zhang, Yining Gao, Xinbei Xu, Luyao Chen, Can Wu, Zheng Li, Rongjie Li, Binyu Xiao, Xiaodi Liu, Rui Li, Fan Zhang, and Gehui Wang
Atmos. Chem. Phys., 24, 14177–14190, https://doi.org/10.5194/acp-24-14177-2024, https://doi.org/10.5194/acp-24-14177-2024, 2024
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Secondary organic aerosols (SOAs) from acetone photooxidation in the presence of various seeds were studied to illustrate SOA formation kinetics under ammonia-rich conditions. The oxidation mechanism of acetone was investigated using an observation-based model incorporating a Master Chemical Mechanism model. A higher SOA yield of acetone was observed compared to methylglyoxal due to an enhanced uptake of the small photooxidation products of acetone.
Adam Milsom, Adam M. Squires, Ben Laurence, Ben Wōden, Andrew J. Smith, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 24, 13571–13586, https://doi.org/10.5194/acp-24-13571-2024, https://doi.org/10.5194/acp-24-13571-2024, 2024
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We followed nano-structural changes in mixtures found in urban organic aerosol emissions (oleic acid, sodium oleate and fructose) during humidity change and ozone exposure. We demonstrate that self-assembly of fatty acid nanostructures can impact water uptake and chemical reactivity, affecting atmospheric lifetimes, urban air quality (preventing harmful emissions from degradation and enabling their long-range transport) and climate (affecting cloud formation), with implications for human health.
Kumiko Goto-Azuma, Remi Dallmayr, Yoshimi Ogawa-Tsukagawa, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Motohiro Hirabayashi, Jun Ogata, Kyotaro Kitamura, Kenji Kawamura, Koji Fujita, Sumito Matoba, Naoko Nagatsuka, Akane Tsushima, Kaori Fukuda, and Teruo Aoki
Atmos. Chem. Phys., 24, 12985–13000, https://doi.org/10.5194/acp-24-12985-2024, https://doi.org/10.5194/acp-24-12985-2024, 2024
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We developed a continuous flow analysis system to analyze an ice core from northwestern Greenland and coupled it with an improved refractory black carbon (rBC) measurement technique. This allowed accurate high-resolution analyses of size distributions and concentrations of rBC particles with diameters of 70 nm–4 μm for the past 350 years. Our results provide crucial insights into rBC's climatic effects. We also found previous ice core studies substantially underestimated rBC mass concentrations.
Julia Pikmann, Frank Drewnick, Friederike Fachinger, and Stephan Borrmann
Atmos. Chem. Phys., 24, 12295–12321, https://doi.org/10.5194/acp-24-12295-2024, https://doi.org/10.5194/acp-24-12295-2024, 2024
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Cooking activities can contribute substantially to indoor and ambient aerosol. We performed a comprehensive study with laboratory measurements cooking 19 different dishes and ambient measurements at two Christmas markets measuring various particle properties and trace gases of emissions in real time. Similar emission characteristics were observed for dishes with the same preparation method, mainly due to similar cooking temperature and use of oil, with barbecuing as an especially strong source.
Han Zang, Zekun Luo, Chenxi Li, Ziyue Li, Dandan Huang, and Yue Zhao
Atmos. Chem. Phys., 24, 11701–11716, https://doi.org/10.5194/acp-24-11701-2024, https://doi.org/10.5194/acp-24-11701-2024, 2024
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Atmospheric organics are subject to synergistic oxidation by different oxidants, yet the mechanisms of such processes are poorly understood. Here, using direct measurements and kinetic modeling, we probe the nocturnal synergistic-oxidation mechanism of α-pinene by O3 and NO3 radicals and in particular the fate of peroxy radical intermediates of different origins, which will deepen our understanding of the monoterpene oxidation chemistry and its contribution to atmospheric particle formation.
Hui Yang, Fengfeng Dong, Li Xia, Qishen Huang, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 24, 11619–11635, https://doi.org/10.5194/acp-24-11619-2024, https://doi.org/10.5194/acp-24-11619-2024, 2024
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Atmospheric secondary aerosols, composed of organic and inorganic components, undergo complex reactions that impact their phase state. Using molecular spectroscopy, we showed that ammonium-promoted aqueous replacement reaction, unique to these aerosols, is closely linked to phase behavior. The interplay between reactions and aerosol phase state can cause atypical phase transition and irreversible changes in aerosol composition during hygroscopic cycles, further impacting atmospheric processes.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
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Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Harmanjot Kaur, Stephan Thürmer, Shirin Gholami, Bruno Credidio, Florian Trinter, Debora Vasconcelos, Ricardo Marinho, Joel Pinheiro, Hendrik Bluhm, Arnaldo Naves de Brito, Gunnar Öhrwall, Bernd Winter, and Olle Björneholm
EGUsphere, https://doi.org/10.5194/egusphere-2024-2609, https://doi.org/10.5194/egusphere-2024-2609, 2024
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The climate effects of atmospheric aerosols are insufficiently known, and the properties of aerosols are affected by their surface due to their small size. Organic molecules are important aerosol constituents. We show that the surface composition of aerosols containing organic molecules and water is very different from the bulk. This affects all surface-related properties and processes. Our results demonstrate the importance of accounting for the aerosol surface composition in climate models.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Melani Hernández-Chiriboga, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert Green, Paul Ginoux, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 9155–9176, https://doi.org/10.5194/acp-24-9155-2024, https://doi.org/10.5194/acp-24-9155-2024, 2024
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In this research, we studied the dust-emitting properties of crusts and aeolian ripples from the Mojave Desert. These properties are key to understanding the effect of dust upon climate. We found two different playa lakes according to the groundwater regime, which implies differences in crusts' cohesion state and mineralogy, which can affect the dust emission potential and properties. We also compare them with Moroccan Sahara crusts and Icelandic top sediments.
Rosalie Shepherd, Martin King, Andrew Ward, Edward Stuckey, Rebecca Welbourn, Neil Brough, Adam Milsom, Christian Pfrang, and Thomas Arnold
EGUsphere, https://doi.org/10.5194/egusphere-2024-2367, https://doi.org/10.5194/egusphere-2024-2367, 2024
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Thin film formation at the air-water interface from material extracted from atmospheric aerosol was demonstrated, supporting core-shell morphology. The film thicknesses were approximately 10 Å and 17 Å for urban and remote extracts. Exposure to gas-phase OH radicals showed fast reactions and short lifetimes of around 1 hour. The effect on the Earth's radiative balance indicated that removing half of the film could significantly increase the top of the atmosphere albedo for urban films.
Mohammed Jaoui, Klara Nestorowicz, Krzysztof Rudzinski, Michael Lewandowski, Tadeusz Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, and Rafal Szmigielski
EGUsphere, https://doi.org/10.5194/egusphere-2024-2032, https://doi.org/10.5194/egusphere-2024-2032, 2024
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Recent research has established the contribution of 1,3-butadiene (13BD) to organic aerosol formation with negative implications to urban air quality. Health effects studies have focused on whole particulate matter but compounds responsible for adverse health effects remain uncertain. This study provides the effect of relative humidity and acidity on the chemical composition of aerosol formed from 13BD photooxidation.
Michel Legrand, Mstislav Vorobyev, Daria Bokuchava, Stanislav Kutuzov, Andreas Plach, Andreas Stohl, Alexandra Khairedinova, Vladimir Mikhalenko, Maria Vinogradova, Sabine Eckhardt, and Susanne Preunkert
EGUsphere, https://doi.org/10.5194/egusphere-2024-1381, https://doi.org/10.5194/egusphere-2024-1381, 2024
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A record of ammonium covering the years 1750 to 2008 was extracted from a 182-meter-long ice core drilled in 2009 at Mt. Elbrus in the Caucasus, Russia. Changes in ammonia emissions in southeastern Europe during the pre-industrial and industrial periods were investigated. The level of ammonium in 1750 indicates a significant contribution of natural sources to the ammonia budget, contrasting with present-day conditions, where agricultural emissions outweigh those from biogenic sources in Europe.
Juanjuan Qin, Leiming Zhang, Yuanyuan Qin, Shaoxuan Shi, Jingnan Li, Zhao Shu, Yuwei Gao, Ting Qi, Jihua Tan, and Xinming Wang
Atmos. Chem. Phys., 24, 7575–7589, https://doi.org/10.5194/acp-24-7575-2024, https://doi.org/10.5194/acp-24-7575-2024, 2024
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The present research unveiled that acidity dominates while transition metal ions harmonize with the light absorption properties of humic-like substances (HULIS). Cu2+ has quenching effects on HULIS by complexation, hydrogen substitution, or electrostatic adsorption, with aromatic structures of HULIS. Such effects are less pronounced if from Mn2+, Ni2+, Zn2+, and Cu2+. Oxidized HULIS might contain electron-donating groups, whereas N-containing compounds might contain electron-withdrawing groups.
Rui Jin, Wei Hu, Peimin Duan, Ming Sheng, Dandan Liu, Ziye Huang, Mutong Niu, Libin Wu, Junjun Deng, and Pingqing Fu
EGUsphere, https://doi.org/10.5194/egusphere-2024-1880, https://doi.org/10.5194/egusphere-2024-1880, 2024
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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 exometabolite and have significant variations in metabolism among different strains. These insights are pivotal for assessing the biogeochemical impacts of atmospheric microorganisms following their deposition.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert O. Green, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 6883–6910, https://doi.org/10.5194/acp-24-6883-2024, https://doi.org/10.5194/acp-24-6883-2024, 2024
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The knowledge of properties from dust emitted in high latitudes such as in Iceland is scarce. This study focuses on the particle size, mineralogy, cohesion, and iron mode of occurrence and reflectance spectra of dust-emitting sediments. Icelandic top sediments have lower cohesion state, coarser particle size, distinctive mineralogy, and 3-fold bulk Fe content, with a large presence of magnetite compared to Saharan crusts.
Wangjin Yang, Jiawei Ma, Hongxing Yang, Fu Li, and Chong Han
Atmos. Chem. Phys., 24, 6757–6768, https://doi.org/10.5194/acp-24-6757-2024, https://doi.org/10.5194/acp-24-6757-2024, 2024
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We provide evidence that light enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where triplet states of SO2 (3SO2) can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. The SO2 photochemistry on non-photoactive mineral dust contributes to sulfates, highlighting previously unknown pathways to better explain the missing sources of atmospheric sulfates.
Lu Zhang, Jin Li, Yaojie Li, Xinlei Liu, Zhihan Luo, Guofeng Shen, and Shu Tao
Atmos. Chem. Phys., 24, 6323–6337, https://doi.org/10.5194/acp-24-6323-2024, https://doi.org/10.5194/acp-24-6323-2024, 2024
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Brown carbon (BrC) is related to radiative forcing and climate change. The BrC fraction from residential coal and biomass burning emissions, which were the major source of BrC, was characterized at the molecular level. The CHOS aromatic compounds explained higher light absorption efficiencies of biomass burning emissions compared to coal. The unique formulas of coal combustion aerosols were characterized by higher unsaturated compounds, and such information could be used for source appointment.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
Atmos. Chem. Phys., 24, 5625–5636, https://doi.org/10.5194/acp-24-5625-2024, https://doi.org/10.5194/acp-24-5625-2024, 2024
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Cooking is a major source of particles in urban areas. Previous studies demonstrated that the chemical lifetimes of cooking organic aerosols (COAs) were much shorter (~minutes) than the values reported by field observations (~hours). We conducted laboratory experiments to resolve the discrepancy by considering suppressed reactivity under low temperature. The parameterized k2–T relationships and observed surface temperature data were used to estimate the chemical lifetimes of COA particles.
Stephanie Arciva, Lan Ma, Camille Mavis, Chrystal Guzman, and Cort Anastasio
Atmos. Chem. Phys., 24, 4473–4485, https://doi.org/10.5194/acp-24-4473-2024, https://doi.org/10.5194/acp-24-4473-2024, 2024
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We measured changes in light absorption during the aqueous oxidation of six phenols with hydroxyl radical (●OH) or an organic triplet excited state (3C*). All the phenols formed light-absorbing secondary brown carbon (BrC), which then decayed with continued oxidation. Extrapolation to ambient conditions suggest ●OH is the dominant sink of secondary phenolic BrC in fog/cloud drops, while 3C* controls the lifetime of this light absorption in particle water.
Aaron Lieberman, Julietta Picco, Murat Onder, and Cort Anastasio
Atmos. Chem. Phys., 24, 4411–4419, https://doi.org/10.5194/acp-24-4411-2024, https://doi.org/10.5194/acp-24-4411-2024, 2024
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We developed a method that uses aqueous S(IV) to quantitatively convert NO2 to NO2−, which allows both species to be quantified using the Griess method. As an example of the utility of the method, we quantified both photolysis channels of nitrate, with and without a scavenger for hydroxyl radical (·OH). The results show that without a scavenger, ·OH reacts with nitrite to form nitrogen dioxide, suppressing the apparent quantum yield of NO2− and enhancing that of NO2.
Xingjun Fan, Ao Cheng, Xufang Yu, Tao Cao, Dan Chen, Wenchao Ji, Yongbing Cai, Fande Meng, Jianzhong Song, and Ping'an Peng
Atmos. Chem. Phys., 24, 3769–3783, https://doi.org/10.5194/acp-24-3769-2024, https://doi.org/10.5194/acp-24-3769-2024, 2024
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Molecular-level characteristics of high molecular weight (HMW) and low MW (LMW) humic-like substances (HULIS) were comprehensively investigated, where HMW HULIS had larger chromophores and larger molecular size than LMW HULIS and exhibited higher aromaticity and humification. Electrospray ionization high-resolution mass spectrometry revealed more aromatic molecules in HMW HULIS. HMW HULIS had more CHON compounds, while LMW HULIS had more CHO compounds.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
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The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Feng Jiang, Kyla Siemens, Claudia Linke, Yanxia Li, Yiwei Gong, Thomas Leisner, Alexander Laskin, and Harald Saathoff
Atmos. Chem. Phys., 24, 2639–2649, https://doi.org/10.5194/acp-24-2639-2024, https://doi.org/10.5194/acp-24-2639-2024, 2024
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We investigated the optical properties, chemical composition, and formation mechanisms of secondary organic aerosol (SOA) and brown carbon (BrC) from the oxidation of indole with and without NO2 in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) simulation chamber. This work is one of the very few to link the optical properties and chemical composition of indole SOA with and without NO2 by simulation chamber experiments.
Evangelia Kostenidou, Baptiste Marques, Brice Temime-Roussel, Yao Liu, Boris Vansevenant, Karine Sartelet, and Barbara D'Anna
Atmos. Chem. Phys., 24, 2705–2729, https://doi.org/10.5194/acp-24-2705-2024, https://doi.org/10.5194/acp-24-2705-2024, 2024
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Secondary organic aerosol (SOA) from gasoline vehicles can be a significant source of particulate matter in urban areas. Here the chemical composition of secondary volatile organic compounds and SOA produced by photo-oxidation of Euro 5 gasoline vehicle emissions was studied. The volatility of the SOA formed was calculated. Except for the temperature and the concentration of the aerosol, additional parameters may play a role in the gas-to-particle partitioning.
András Hoffer, Aida Meiramova, Ádám Tóth, Beatrix Jancsek-Turóczi, Gyula Kiss, Ágnes Rostási, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 24, 1659–1671, https://doi.org/10.5194/acp-24-1659-2024, https://doi.org/10.5194/acp-24-1659-2024, 2024
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Specific tracer compounds identified previously in controlled test burnings of different waste types in the laboratory were detected and quantified in ambient PM10 samples collected in five Hungarian and four Romanian settlements. Back-of-the-envelope calculations based on the relative emission factors of individual tracers suggested that the contribution of solid waste burning particulate emissions to ambient PM10 mass concentrations may be as high as a few percent.
Xiao-San Luo, Weijie Huang, Guofeng Shen, Yuting Pang, Mingwei Tang, Weijun Li, Zhen Zhao, Hanhan Li, Yaqian Wei, Longjiao Xie, and Tariq Mehmood
Atmos. Chem. Phys., 24, 1345–1360, https://doi.org/10.5194/acp-24-1345-2024, https://doi.org/10.5194/acp-24-1345-2024, 2024
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PM2.5 are air pollutants threatening health globally, but they are a mixture of chemical compositions from many sources and result in unequal toxicity. Which composition from which source of PM2.5 as the most hazardous object is a question hindering effective pollution control policy-making. With chemical and toxicity experiments, we found automobile exhaust and coal combustion to be priority emissions with higher toxic compositions for precise air pollution control, ensuring public health.
Matthew B. Goss and Jesse H. Kroll
Atmos. Chem. Phys., 24, 1299–1314, https://doi.org/10.5194/acp-24-1299-2024, https://doi.org/10.5194/acp-24-1299-2024, 2024
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The chemistry driving dimethyl sulfide (DMS) oxidation and subsequent sulfate particle formation in the atmosphere is poorly constrained. We oxidized two related compounds (dimethyl sulfoxide and dimethyl disulfide) in the laboratory under varied NOx conditions and measured the gas- and particle-phase products. These results demonstrate that both the OH addition and OH abstraction pathways for DMS oxidation contribute to particle formation via mechanisms that do not involve the SO2 intermediate.
Ryan J. Patnaude, Kathryn A. Moore, Russell J. Perkins, Thomas C. J. Hill, Paul J. DeMott, and Sonia M. Kreidenweis
Atmos. Chem. Phys., 24, 911–928, https://doi.org/10.5194/acp-24-911-2024, https://doi.org/10.5194/acp-24-911-2024, 2024
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In this study we examined the effect of atmospheric aging on sea spray aerosols (SSAs) to form ice and how newly formed secondary marine aerosols (SMAs) may freeze at cirrus temperatures (< −38 °C). Results show that SSAs freeze at different relative humidities (RHs) depending on the temperature and that the ice-nucleating ability of SSA was not hindered by atmospheric aging. SMAs are shown to freeze at high RHs and are likely inefficient at forming ice at cirrus temperatures.
Bartłomiej Witkowski, Priyanka Jain, Beata Wileńska, and Tomasz Gierczak
Atmos. Chem. Phys., 24, 663–688, https://doi.org/10.5194/acp-24-663-2024, https://doi.org/10.5194/acp-24-663-2024, 2024
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This article reports the results of the kinetic measurements for the aqueous oxidation of the 29 aliphatic alcohols by hydroxyl radical (OH) at different temperatures. The data acquired and the literature data were used to optimize a model for predicting the aqueous OH reactivity of alcohols and carboxylic acids and to estimate the atmospheric lifetimes of five terpenoic alcohols. The kinetic data provided new insights into the mechanism of aqueous oxidation of aliphatic molecules by the OH.
Junting Qiu, Xinlin Shen, Jiangyao Chen, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 155–166, https://doi.org/10.5194/acp-24-155-2024, https://doi.org/10.5194/acp-24-155-2024, 2024
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We studied reactions of secondary ozonides (SOZs) with amines. SOZs formed from ozonolysis of β-caryophyllene and α-humulene are found to be reactive to ethylamine and methylamine. Products from SOZs with various conformations reacting with the same amine had different functional groups. Our findings indicate that interaction of SOZs with amines in the atmosphere is very complicated, which is potentially a hitherto unrecognized source of N-containing compound formation.
Lan Ma, Reed Worland, Laura Heinlein, Chrystal Guzman, Wenqing Jiang, Christopher Niedek, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 24, 1–21, https://doi.org/10.5194/acp-24-1-2024, https://doi.org/10.5194/acp-24-1-2024, 2024
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We measured concentrations of three photooxidants – the hydroxyl radical, triplet excited states of organic carbon, and singlet molecular oxygen – in fine particles collected over a year. Concentrations are highest in extracts of fresh biomass burning particles, largely because they have the highest particle concentrations and highest light absorption. When normalized by light absorption, rates of formation for each oxidant are generally similar for the four particle types we observed.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Cristina Reche, Patricia Córdoba, Natalia Moreno, Andres Alastuey, Konrad Kandler, Martina Klose, Clarissa Baldo, Roger N. Clark, Zongbo Shi, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 15815–15834, https://doi.org/10.5194/acp-23-15815-2023, https://doi.org/10.5194/acp-23-15815-2023, 2023
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The effect of dust emitted from desertic surfaces upon climate and ecosystems depends on size and mineralogy, but data from soil mineral atlases of desert soils are scarce. We performed particle-size distribution, mineralogy, and Fe speciation in southern Morocco. Results show coarser particles with high quartz proportion are near the elevated areas, while in depressed areas, sizes are finer, and proportions of clays and nano-Fe oxides are higher. This difference is important for dust modelling.
Victor Lannuque, Barbara D'Anna, Evangelia Kostenidou, Florian Couvidat, Alvaro Martinez-Valiente, Philipp Eichler, Armin Wisthaler, Markus Müller, Brice Temime-Roussel, Richard Valorso, and Karine Sartelet
Atmos. Chem. Phys., 23, 15537–15560, https://doi.org/10.5194/acp-23-15537-2023, https://doi.org/10.5194/acp-23-15537-2023, 2023
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from toluene oxidation. In this study, speciation measurements in gaseous and particulate phases were carried out, providing partitioning and volatility data on individual toluene SOA components at different temperatures. A new detailed oxidation mechanism was developed to improve modeled speciation, and effects of different processes involved in gas–particle partitioning at the molecular scale are explored.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Steven Sai Hang Ho, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 15375–15393, https://doi.org/10.5194/acp-23-15375-2023, https://doi.org/10.5194/acp-23-15375-2023, 2023
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Open burning of municipal solid waste emits chemicals that are harmful to the environment. This paper reports source profiles and emission factors for PM2.5 species and acidic/alkali gases from laboratory combustion of 10 waste categories (including plastics and biomass) that represent open burning in South Africa. Results will be useful for health and climate impact assessments, speciated emission inventories, source-oriented dispersion models, and receptor-based source apportionment.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Rico K. Y. Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 23, 14561–14576, https://doi.org/10.5194/acp-23-14561-2023, https://doi.org/10.5194/acp-23-14561-2023, 2023
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We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bag burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Hyun Gu Kang, Yanfang Chen, Yoojin Park, Thomas Berkemeier, and Hwajin Kim
Atmos. Chem. Phys., 23, 14307–14323, https://doi.org/10.5194/acp-23-14307-2023, https://doi.org/10.5194/acp-23-14307-2023, 2023
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D5 is an emerging anthropogenic pollutant that is ubiquitous in indoor and urban environments, and the OH oxidation of D5 forms secondary organosiloxane aerosol (SOSiA). Application of a kinetic box model that uses a volatility basis set (VBS) showed that consideration of oxidative aging (aging-VBS) predicts SOSiA formation much better than using a standard-VBS model. Ageing-dependent parameterization is needed to accurately model SOSiA to assess the implications of siloxanes for air quality.
Kai Song, Rongzhi Tang, Jingshun Zhang, Zichao Wan, Yuan Zhang, Kun Hu, Yuanzheng Gong, Daqi Lv, Sihua Lu, Yu Tan, Ruifeng Zhang, Ang Li, Shuyuan Yan, Shichao Yan, Baoming Fan, Wenfei Zhu, Chak K. Chan, Maosheng Yao, and Song Guo
Atmos. Chem. Phys., 23, 13585–13595, https://doi.org/10.5194/acp-23-13585-2023, https://doi.org/10.5194/acp-23-13585-2023, 2023
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Incense burning is common in Asia, posing threats to human health and air quality. However, less is known about its emissions and health risks. Full-volatility organic species from incense-burning smoke are detected and quantified. Intermediate-volatility volatile organic compounds (IVOCs) are crucial organics accounting for 19.2 % of the total emission factors (EFs) and 40.0 % of the secondary organic aerosol (SOA) estimation, highlighting the importance of incorporating IVOCs into SOA models.
Qianqian Gao, Shengqiang Zhu, Kaili Zhou, Jinghao Zhai, Shaodong Chen, Qihuang Wang, Shurong Wang, Jin Han, Xiaohui Lu, Hong Chen, Liwu Zhang, Lin Wang, Zimeng Wang, Xin Yang, Qi Ying, Hongliang Zhang, Jianmin Chen, and Xiaofei Wang
Atmos. Chem. Phys., 23, 13049–13060, https://doi.org/10.5194/acp-23-13049-2023, https://doi.org/10.5194/acp-23-13049-2023, 2023
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Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Dust aerosols are mainly generated by wind erosion, which may have some chemical selectivity. Mn, Cd and Pb were found to be highly enriched in fine-dust (PM2.5) aerosols. In addition, estimation of heavy metal emissions from dust generation by air quality models may have errors without using proper dust profiles.
Daniel C. O. Thornton, Sarah D. Brooks, Elise K. Wilbourn, Jessica Mirrielees, Alyssa N. Alsante, Gerardo Gold-Bouchot, Andrew Whitesell, and Kiana McFadden
Atmos. Chem. Phys., 23, 12707–12729, https://doi.org/10.5194/acp-23-12707-2023, https://doi.org/10.5194/acp-23-12707-2023, 2023
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A major uncertainty in our understanding of clouds and climate is the sources and properties of the aerosol on which clouds grow. We found that aerosol containing organic matter from fast-growing marine phytoplankton was a source of ice-nucleating particles (INPs). INPs facilitate freezing of ice crystals at warmer temperatures than otherwise possible and therefore change cloud formation and properties. Our results show that ecosystem processes and the properties of sea spray aerosol are linked.
Adam Milsom, Shaojun Qi, Ashmi Mishra, Thomas Berkemeier, Zhenyu Zhang, and Christian Pfrang
Atmos. Chem. Phys., 23, 10835–10843, https://doi.org/10.5194/acp-23-10835-2023, https://doi.org/10.5194/acp-23-10835-2023, 2023
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Aerosols and films are found indoors and outdoors. Our study measures and models reactions of a cooking aerosol proxy with the atmospheric oxidant ozone relying on a low-cost but sensitive technique based on mass changes and film rigidity. We found that film morphology changed and film rigidity increased with evidence of surface crust formation during ozone exposure. Our modelling results demonstrate clear potential to take this robust method to the field for reaction monitoring.
Shan Zhang, Lin Du, Zhaomin Yang, Narcisse Tsona Tchinda, Jianlong Li, and Kun Li
Atmos. Chem. Phys., 23, 10809–10822, https://doi.org/10.5194/acp-23-10809-2023, https://doi.org/10.5194/acp-23-10809-2023, 2023
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In this study, we have investigated the distinct impacts of humidity on the ozonolysis of two structurally different monoterpenes (limonene and Δ3-carene). We found that the molecular structure of precursors can largely influence the SOA formation under high RH by impacting the multi-generation reactions. Our results could advance knowledge on the roles of water content in aerosol formation and inform ongoing research on particle environmental effects and applications in models.
Yangzhihao Zhan, Min Xie, Wei Zhao, Tijian Wang, Da Gao, Pulong Chen, Jun Tian, Kuanguang Zhu, Shu Li, Bingliang Zhuang, Mengmeng Li, Yi Luo, and Runqi Zhao
Atmos. Chem. Phys., 23, 9837–9852, https://doi.org/10.5194/acp-23-9837-2023, https://doi.org/10.5194/acp-23-9837-2023, 2023
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Although the main source contribution of pollution is secondary inorganic aerosols in Nanjing, health risks mainly come from industry sources and vehicle emissions. Therefore, the development of megacities should pay more attention to the health burden of vehicle emissions, coal combustion, and industrial processes. This study provides new insight into assessing the relationship between source apportionment and health risks and can provide valuable insight into air pollution strategies.
Jonathan P. D. Abbatt and A. R. Ravishankara
Atmos. Chem. Phys., 23, 9765–9785, https://doi.org/10.5194/acp-23-9765-2023, https://doi.org/10.5194/acp-23-9765-2023, 2023
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With important climate and air quality impacts, atmospheric multiphase chemistry involves gas interactions with aerosol particles and cloud droplets. We summarize the status of the field and discuss potential directions for future growth. We highlight the importance of a molecular-level understanding of the chemistry, along with atmospheric field studies and modeling, and emphasize the necessity for atmospheric multiphase chemists to interact widely with scientists from neighboring disciplines.
Zhancong Liang, Zhihao Cheng, Ruifeng Zhang, Yiming Qin, and Chak K. Chan
Atmos. Chem. Phys., 23, 9585–9595, https://doi.org/10.5194/acp-23-9585-2023, https://doi.org/10.5194/acp-23-9585-2023, 2023
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In this study, we found that the photolysis of sodium nitrate leads to a much quicker decay of free amino acids (FAAs, with glycine as an example) in the particle phase than ammonium nitrate photolysis, which is likely due to the molecular interactions between FAAs and different nitrate salts. Since sodium nitrate likely co-exists with FAAs in the coarse-mode particles, particulate nitrate photolysis can possibly contribute to a rapid decay of FAAs and affect atmospheric nitrogen cycling.
Julian Resch, Kate Wolfer, Alexandre Barth, and Markus Kalberer
Atmos. Chem. Phys., 23, 9161–9171, https://doi.org/10.5194/acp-23-9161-2023, https://doi.org/10.5194/acp-23-9161-2023, 2023
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Detailed chemical analysis of organic aerosols is necessary to better understand their effects on climate and health. Aerosol samples are often stored for days to months before analysis. We examined the effects of storage conditions (i.e., time, temperature, and aerosol storage on filters or as solvent extracts) on composition and found significant changes in the concentration of individual compounds, indicating that sample storage can strongly affect the detailed chemical particle composition.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 8921–8937, https://doi.org/10.5194/acp-23-8921-2023, https://doi.org/10.5194/acp-23-8921-2023, 2023
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Open burning of household and municipal solid waste is a common practice in developing countries and is a significant source of air pollution. However, few studies have measured emissions from open burning of waste. This study determined gas and particulate emissions from open burning of 10 types of household solid-waste materials. These results can improve emission inventories, air quality management, and assessment of the health and climate effects of open burning of household waste.
Anita M. Avery, Mariam Fawaz, Leah R. Williams, Tami Bond, and Timothy B. Onasch
Atmos. Chem. Phys., 23, 8837–8854, https://doi.org/10.5194/acp-23-8837-2023, https://doi.org/10.5194/acp-23-8837-2023, 2023
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Pyrolysis is the thermal decomposition of fuels like wood which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to investigate both the uncombusted emissions from wildfires and the fuel that participates in combustion.
Lan Ma, Reed Worland, Wenqing Jiang, Christopher Niedek, Chrystal Guzman, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, https://doi.org/10.5194/acp-23-8805-2023, 2023
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Although photooxidants are important in airborne particles, little is known of their concentrations. By measuring oxidants in a series of particle dilutions, we predict their concentrations in aerosol liquid water (ALW). We find •OH concentrations in ALW are on the order of 10−15 M, similar to their cloud/fog values, while oxidizing triplet excited states and singlet molecular oxygen have ALW values of ca. 10−13 M and 10−12 M, respectively, roughly 10–100 times higher than in cloud/fog drops.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
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Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Cited articles
Bahl, A. and Bahl, B. S: Advanced Organic Chemistry, 1st edn., S. Chand Publication, New Delhi, India, ISBN 9788121935159, 2010.
Bateman, A. P., Walser, M. L., Desyaterik, Y., Laskin, J., Laskin, A., and
Nizkorodov, S. A.: The effect of solvent on the analysis of secondary
organic aerosol using electrospray ionization mass spectrometry, Environ.
Sci. Technol., 42, 7341–7346, https://doi.org/10.1021/es801226w, 2008.
Bennett, J. E. and Summers, R.: Product studies of the mutual termination reactions of sec-alkylperoxy radicals: evidence for non-cyclic termination, Can. J. Chem., 52, 1377–1379, https://doi.org/10.1139/v74-209, 1974.
Bentley, R. and Chasteen, T. G.: Environmental VOSCs – formation and
degradation of dimethyl sulfide, methanethiol and related materials,
Chemos., 55, 291–317, https://doi.org/10.1016/j.chemosphere.2003.12.017,
2004.
Bergh, v. d., Vanhees, V. I., de Boer, R., Compernolle, F., and Vinckier, C.:
Identification of the oxidation products of the reaction between α-pinene and hydroxyl radicals by gas and high-performance liquid
chromatography with mass spectrometric detection, J. Chrom. A., 896,
135–148, https://doi.org/10.1016/s0021-9673(00)00680-4, 2000.
Brüggemann, M., Xu, R., Tilgner, A., Kwong, K. C., Mutzel, A., Poon, H.
Y., Otto, T., Schaefer, T., Poulain, L., Chan, M. N., and Herrmann, H.:
Organosulfates in ambient aerosol: state of knowledge and future research
directions on formation, abundance, fate, and importance, Environ. Sci.
Technol., 54, 3767–3782, https://doi.org/10.1021/acs.est.9b06751.s001,
2020.
Bruice, P. Y.: Organic chemistry, 6th edn., Pearson Publication, Lebanon, Indiana, USA, ISBN 9780321663139, 2010.
Budisulistiorini, S. H., Li, X., Bairai, S. T., Renfro, J., Liu, Y., Liu, Y. J., McKinney, K. A., Martin, S. T., McNeill, V. F., Pye, H. O. T., Nenes, A., Neff, M. E., Stone, E. A., Mueller, S., Knote, C., Shaw, S. L., Zhang, Z., Gold, A., and Surratt, J. D.: Examining the effects of anthropogenic emissions on isoprene-derived secondary organic aerosol formation during the 2013 Southern Oxidant and Aerosol Study (SOAS) at the Look Rock, Tennessee ground site, Atmos. Chem. Phys., 15, 8871–8888, https://doi.org/10.5194/acp-15-8871-2015, 2015.
Capouet, M., Peeters, J., Nozi`ere, B., and Müller, J.-F.: Alpha-pinene oxidation by OH: simulations of laboratory experiments, Atmos. Chem. Phys., 4, 2285–2311, https://doi.org/10.5194/acp-4-2285-2004, 2004.
Carrasquillo A. J., Daumit K. E., Kroll J. H.: Radical reactivity in the
condensed phase: intermolecular versus intramolecular reactions of alkoxy
radicals, J. Phys. Chem. Lett., 6, 2388–2392,
https://doi.org/10.1021/acs.jpclett.5b00913, 2015.
Chan, M. N., Zhang, H., Goldstein, A. H., and Wilson, K. R.: Role of water
and phase in the heterogeneous oxidation of solid and aqueous succinic acid
aerosol by hydroxyl radicals, J. Phys. Chem. C, 118, 28978–28992,
https://doi.org/10.1021/jp5012022, 2014.
Chen, Y., Zhang, Y., Lambe, A. T., Xu, R., Lei, Z., Olson, N. E., Zhang, Z.,
Szalkowski, T., Cui, T., Vizuete, W., Gold, A., Turpin, B. J., Ault, A. P.,
Chan, M. N., and Surratt, J. D.: Heterogeneous hydroxyl radical oxidation of
isoprene-epoxydiol-derived methyltetrol sulfates: plausible formation
mechanisms of previously unexplained organosulfates in ambient fine
aerosols, Environ. Sci. Technol. Letters, 7, 460–468,
https://doi.org/10.1021/acs.estlett.0c00276.s001, 2020.
Chim, M. M., Chow, C. Y., Davies, J. F., and Chan, M. N.: Effects of relative
humidity and particle phase water on the heterogeneous OH oxidation of
2-methylglutaric acid aqueous droplets, J. Phys. Chem. A, 121, 1666–1674,
https://doi.org/10.1021/acs.jpca.6b11606, 2017.
Compernolle, S., Ceulemans, K., and Müller, J.-F.: EVAPORATION: a new vapour pressure estimation methodfor organic molecules including non-additivity and intramolecular interactions, Atmos. Chem. Phys., 11, 9431–9450, https://doi.org/10.5194/acp-11-9431-2011, 2011.
Craig, R. L., Peterson, P. K., Nandy, L., Lei, Z., Hossain, M. A., Camarena,
S., Dodson, R. A., Cook, R. D., Dutcher, C. S., and Ault, A. P.: Direct
determination of aerosol pH: size-resolved measurements of submicrometer and
supermicrometer aqueous particles, Anal. Chem., 90, 11232–11239,
https://doi.org/10.1021/acs.analchem.8b00586, 2018.
Darer, A. I., Cole-Filipiak, N. C., O'Connor, A. E., and Elrod, M. J.:
Formation and stability of atmospherically relevant isoprene-derived
organosulfates and organonitrates, Environ. Sci. Technol., 45, 1895–1902,
https://doi.org/10.1021/es103797z, 2011.
Dennis-Smither, B. J., Miles, R. E. H., and Reid, J. P.: Oxidative aging of
mixed oleic acid/sodium chlo-ride aerosol particles, J. Geophys. Res., 117,
D20204, https://doi.org/10.1029/2012JD018163, 2012.
Domingos, J. S. S., Regis, C. D., Santos, V. S., Andrade, B., and Rocha, O.: A
comprehensive and suitable method for determining major ions from
atmospheric particulate matter matrices, J. Chrom. A., 1266, 17–23,
https://doi.org/10.1016/j.chroma.2012.08.074, 2012.
Freedman, M. A.: Phase separation in organic aerosol, Chem. Soc. Rev., 46,
7694–7705,
https://doi.org/10.1039/C6CS00783J, 2017.
Freedman, M. A.: Liquid–liquid phase separation in supermicrometer and
submicrometer aerosol particles, Acc. Chem. Res., 53, 1102–1110,
https://doi.org/10.1021/acs.accounts.0c00093, 2020.
George, I. J. and Abbatt, J. P. D.: Heterogeneous oxidation of atmospheric
aerosol particles by gas-phase radicals, Nat. Chem., 2, 713–722,
https://doi.org/10.1038/nchem.806, 2010.
Gopalakrishnan, S., Jungwirth, P., Tobias, D. J., and Allen, H. C.: Air–Liquid
Interfaces of Aqueous Solutions Containing Ammonium and Sulfate:
Spectroscopic and Molecular Dynamics Studies, J. Phys. Chem. B, 109,
8861–8872, 2005.
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.
Hansen, A. M. K., Hong, J., Raatikainen, T., Kristensen, K., Ylisirniö, A., Virtanen, A., Petäjä, T., Glasius, M., and Prisle, N. L.: Hygroscopic properties and cloud condensation nuclei activation of limonene-derived organosulfates and their mixtures with ammonium sulfate, Atmos. Chem. Phys., 15, 14071–14089, https://doi.org/10.5194/acp-15-14071-2015, 2015.
Hettiyadura, A. P. S., Jayarathne, T., Baumann, K., Goldstein, A. H., de Gouw, J. A., Koss, A., Keutsch, F. N., Skog, K., and Stone, E. A.: Qualitative and quantitative analysis of atmospheric organosulfates in Centreville, Alabama, Atmos. Chem. Phys., 17, 1343–1359, https://doi.org/10.5194/acp-17-1343-2017, 2017.
Hettiyadura, A. P. S., Al-Naiema, I. M., Hughes, D. D., Fang, T., and Stone, E. A.: Organosulfates in Atlanta, Georgia: anthropogenic influences on biogenic secondary organic aerosol formation, Atmos. Chem. Phys., 19, 3191–3206, https://doi.org/10.5194/acp-19-3191-2019, 2019.
Hu, K. S., Darer, A. I., and Elrod, M. J.: Thermodynamics and kinetics of the hydrolysis of atmospherically relevant organonitrates and organosulfates, Atmos. Chem. Phys., 11, 8307–8320, https://doi.org/10.5194/acp-11-8307-2011, 2011.
Huang, D. D., Li, Y. J., Lee, B. P., and Chan, C. K.: Analysis of organic
sulfur compounds in atmospheric aerosols at the HKUST supersite in Hong Kong
using HR-ToF-AMS, Environ. Sci. Technol., 49, 3672–3679,
https://doi.org/10.1021/es5056269, 2015.
Huang, R.-J., Cao, J., Chen, Y., Yang, L., Shen, J., You, Q., Wang, K., Lin, C., Xu, W., Gao, B., Li, Y., Chen, Q., Hoffmann, T., O'Dowd, C. D., Bilde, M., and Glasius, M.: Organosulfates in atmospheric aerosol: synthesis and quantitative analysis of PM2.5 from Xi'an, northwestern China, Atmos. Meas. Tech., 11, 3447–3456, https://doi.org/10.5194/amt-11-3447-2018, 2018.
Hughes, D. D. and Stone, E. A.: Organosulfates in the Midwestern United
States: Abundance, composition and stability, Environ. Chem., 16, 312–322,
https://doi.org/10.1071/EN18260, 2019.
Hyttinen, N., Elm, J., Malila, J., Calderón, S. M., and Prisle, N. L.: Thermodynamic properties of isoprene- and monoterpene-derived organosulfates estimated with COSMOtherm, Atmos. Chem. Phys., 20, 5679–5696, https://doi.org/10.5194/acp-20-5679-2020, 2020.
Iinuma, Y., Böge, O., Miao, Y., Sierau, B., Gnauk, T., and Herrmann, H.:
Laboratory studies on secondary organic aerosol formation from terpenes,
Faraday Discuss., 130, 279–294, https://doi.org/10.1039/b502160j, 2005.
Iinuma, Y., Müller, C., Berndt, T., Böge, O., Claeys, M., and Herrmann, H.: Evidence for the existence of
organosulfates from β-pinene ozonolysis in ambient secondary organic
aerosol, Environ. Sci. Technol., 41, 6678–6683,
https://doi.org/10.1021/es070938t, 2007.
Jungwirth P. and Tobias D. J.: Ions at the Air/Water Interface, J. Phys.
Chem. B, 106, 6361–6373, https://doi.org/10.1021/jp020242g, 2002.
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.
Kang, E., Root, M. J., Toohey, D. W., and Brune, W. H.: Introducing the concept of Potential Aerosol Mass (PAM), Atmos. Chem. Phys., 7, 5727–5744, https://doi.org/10.5194/acp-7-5727-2007, 2007.
Koop, T., Bookhold, J., Shiraiwa, M., and Pöschl, U.: Glass transition
and phase state of organic compounds: Dependency on molecular properties and
implications for secondary organic aerosols in the atmosphere, Phys. Chem.
Chem. Phys., 13, 19238–19255, https://doi.org/10.1039/C1CP22617G, 2011.
Kristensen, K. and Glasius, M.: Organosulfates and oxidation products from
biogenic hydrocarbons in fine aerosols from a forest in Northwest Europe
during spring, Atmos. Environ., 45, 4546–4556,
https://doi.org/10.1016/j.atmosenv.2011.05.063, 2011.
Kroll, J., Lim, C., Kessler, S., and Wilson, K.: Heterogeneous oxidation of
atmospheric organic aerosol: kinetics of changes to the amount and oxidation
state of particle-phase organic carbon, J. Phys. Chem. A., 119,
10767–10783, https://doi.org/10.1021/acs.jpca.5b06946, 2015.
Kwong, K. C., Chim, M. M., Davies, J. F., Wilson, K. R., and Chan, M. N.: Importance of sulfate radical anion formation and chemistry in heterogeneous OH oxidation of sodium methyl sulfate, the smallest organosulfate, Atmos. Chem. Phys., 18, 2809–2820, https://doi.org/10.5194/acp-18-2809-2018, 2018.
Lam, H. K., Kwong, K. C., Poon, H. Y., Davies, J. F., Zhang, Z., Gold, A., Surratt, J. D., and Chan, M. N.: Heterogeneous OH oxidation of isoprene-epoxydiol-derived organosulfates: kinetics, chemistry and formation of inorganic sulfate, Atmos. Chem. Phys., 19, 2433–2440, https://doi.org/10.5194/acp-19-2433-2019, 2019.
Lam, H. K., Xu, R., Choczynski, J., Davies, J. F., Ham, D., Song, M., Zuend, A., Li, W., Tse, Y.-L. S., and Chan, M. N.: Effects of liquid–liquid phase separation and relative humidity on the heterogeneous OH oxidation of inorganic–organic aerosols: insights from methylglutaric acid and ammonium sulfate particles, Atmos. Chem. Phys., 21, 2053–2066, https://doi.org/10.5194/acp-21-2053-2021, 2021.
Liggio, J. and Li, S.-M.: Organosulfate Formation during the uptake of
pinonaldehyde on acidic sulfate aerosols, Geophys. Res. Lett., 33, L13808,
https://doi.org/10.1029/2006gl026079, 2006.
Ma, Y., Xu, X., Song, W., Geng, F., and Wang, L.: Seasonal and Diurnal
Variations of Particulate Organosulfates in Urban Shanghai, China, Atmos.
Environ., 85, 152–160, https://doi.org/10.1016/j.atmosenv.2013.12.017,
2014.
Mao, J., Ren, X., Brune, W. H., Olson, J. R., Crawford, J. H., Fried, A., Huey, L. G., Cohen, R. C., Heikes, B., Singh, H. B., Blake, D. R., Sachse, G. W., Diskin, G. S., Hall, S. R., and Shetter, R. E.: Airborne measurement of OH reactivity during INTEX-B, Atmos. Chem. Phys., 9, 163–173, https://doi.org/10.5194/acp-9-163-2009, 2009.
Marshall, F. H., Miles, R. E. H., Song, Y.-C., Ohm, P. B., Power, R. M., Reid, J. P., and Dutcher, C. S.: Diffusion and reactivity in ultra-viscous aerosol and the correlation with particle viscosity, Chem. Sci., 7, 1298–1308, https://doi.org/10.1039/c5sc03223g, 2016.
Marshall, F. H., Berkemeier, T., Shiraiwa, M., Nandy, L., Ohm, P. B.,
Dutcher, C. S., and Reid, J. P.: Influence of particle viscosity on mass
transfer and heterogeneous ozonolysis kinetics in aqueous-sucrose-maleic
acid aerosol, Phys. Chem. Chem. Phys., 20, 15560–15573,
https://doi.org/10.1039/c8cp01666f, 2018.
McNeill, V. F., Wolfe, G. M., and Thornton, J. A.: The Oxidation of oleate in
submicron aqueous salt aerosols: evidence of a surface process, J. Phys.
Chem. A, 111, 1073–1083, https://doi.org/10.1021/jp066233f, 2007.
McNeill, V. F., Yatavelli, R. L. N., Thornton, J. A., Stipe, C. B., and Landgrebe, O.: Heterogeneous OH oxidation of palmitic acid in single component and internally mixed aerosol particles: vaporization and the role of particle phase, Atmos. Chem. Phys., 8, 5465–5476, https://doi.org/10.5194/acp-8-5465-2008, 2008.
Monod A. and Doussin, J. F.: Structure-activity relationship for the
estimation of OH-oxidation rate constants of aliphatic organic compounds in
the aqueous phase: alkanes, alcohols, organic acids and bases, Atmos.
Environ., 42, 7611–7622, https://doi.org/10.1016/j.atmosenv.2008.06.005,
2008.
Mungall, E. L., Wong, J. P. S., and Abbatt, J. P. D.: Heterogeneous
Oxidation of Particulate Methanesulfonic Acid by the Hydroxyl Radical:
Kinetics and Atmospheric Implications, ACS Earth Space Chem., 2, 48–55,
https://doi.org/10.1021/acsearthspacechem.7b00114, 2017.
Peeters, J., Vereecken, L., and Fantechi, G.: The detailed mechanism of the
OH-initiated atmospheric oxidation of α-pinene: a theoretical study,
Phys. Chem. Chem. Phys., 3, 5489–5504, https://doi.org/10.1039/b106555f,
2001.
Pye, H. O. T., Chan, A. W. H., Barkley, M. P., and Seinfeld, J. H.: Global modeling of organic aerosol: the importance of reactive nitrogen (NOx and NO3), Atmos. Chem. Phys., 10, 11261–11276, https://doi.org/10.5194/acp-10-11261-2010, 2010.
Qiu, Y. and Molinero, V.: Morphology of liquid-liquid phase separated
aerosols, J. Am. Chem. Soc., 137, 10642–10651, https://doi.org/10.1021/jacs.5b05579, 2015.
Rowley D. M., Lightfoot P. D., Lesclaux R., and Wallington T. J.:
Ultraviolet absorption spectrum and self-reaction of cyclopentylperoxy
radicals, J. Chem. Soc. Faraday T., 88, 1369–1376,
https://doi.org/10.1039/ft9928801369, 1992.
Riva, M., Tomaz, S., Cui, T. Q., Lin, Y. H., Perraudin, E., Gold, A., Stone,
E. A., Villenave, E., and Surratt, J. D.: Evidence for an unrecognized
secondary anthropogenic source of organosulfates and sulfonates: gas-phase
oxidation of polycyclic aromatic hydrocarbons in the presence of sulfate
aerosol, Environ. Sci. Technol., 49, 6654–6664,
https://doi.org/10.1021/acs.est.5b00836, 2015.
Russell, G. A.: Deuterium-isotope effects in the autoxidation of aralkyl hydrocarbons. mechanism of the interaction of peroxy radicals1, J. Am. Chem. Soc., 79, 3871–3877, https://doi.org/10.1021/ja01571a068, 1957.
Shakya, K. M. and Peltier, R. E.: Investigating missing sources of sulfur
at Fairbanks, Alaska, Environ. Sci. Technol., 47, 9332−9338,
https://doi.org/10.1021/es402020b, 2013.
Shakya, K. M. and Peltier, R. E.: Non-sulfate sulfur in fine aerosols
across the United States: insight for organosulfate prevalence, Atmos.
Environ., 100, 159–166, https://doi.org/10.1016/j.atmosenv.2014.10.058,
2015.
Shiraiwa, M., Ammann, M., Koop, T., and Pöschl, U.: Gas uptake and
chemical aging of semisolid organic aerosol particles, Proc. Natl. Acad.
Sci., 108, 11003–11008, https://doi.org/10.1073/pnas.1103045108, 2011.
Shiraiwa, M., Zuend, A., Bertram, A. K., and Seinfeld, J. H.: Gas–particle
partitioning of atmospheric aerosols: Interplay of physical state, non-ideal
mixing and morphology, Phys. Chem. Chem. Phys., 15, 11441–11453,
https://doi.org/10.1039/C3CP51595H, 2013.
Slade, J. H. and Knopf, D. A.: Multiphase OH oxidation kinetics of organic
aerosol: The role of particle phase state and relative humidity, Geophys.
Res. Lett., 41, 5297–5306, https://doi.org/10.1002/2014gl060582, 2014.
Smith, J. D., Kroll, J. H., Cappa, C. D., Che, D. L., Liu, C. L., Ahmed, M., Leone, S. R., Worsnop, D. R., and Wilson, K. R.: The heterogeneous reaction of hydroxyl radicals with sub-micron squalane particles: a model system for understanding the oxidative aging of ambient aerosols, Atmos. Chem. Phys., 9, 3209–3222, https://doi.org/10.5194/acp-9-3209-2009, 2009.
Stadtler, S., Kühn, T., Schröder, S., Taraborrelli, D., Schultz, M. G., and Kokkola, H.: Isoprene-derived secondary organic aerosol in the global aerosol–chemistry–climate model ECHAM6.3.0–HAM2.3–MOZ1.0, Geosci. Model Dev., 11, 3235–3260, https://doi.org/10.5194/gmd-11-3235-2018, 2018.
Stone, E. A., Yang, L., Yu, L. E., and Rupakheti, M.: Characterization of
Organosulfates in Atmospheric Aerosols at Four Asian Locations, Atmos.
Environ., 47, 323–329, https://doi.org/10.1016/j.atmosenv.2011.10.058,
2012.
Surratt, J. D., Gómez-González, Y., Chan, A. W. H., Vermeylen, R.,
Shahgholi, M., Kleindienst, T. E., Edney, E. O., Offenberg, J. H.,
Lewandowski, M., Jaoui, M., Maenhaut, W., Claeys, M., Flagan, R. C., and
Seinfeld, J. H.: Organosulfate formation in biogenic secondary organic
aerosol, J. Phys. Chem. A., 112, 8345–8378,
https://doi.org/10.1021/jp802310p, 2008.
Tolocka, M. P. and Turpin, B.: Contribution of organosulfur compounds to
organic aerosol mass, Environ. Sci. Technol., 46, 7978–7983,
https://doi.org/10.1021/es300651v, 2012.
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 particle formation, Environ.
Sci. Technol., 50, 10814–10822, https://doi.org/10.1021/acs.est.6b01673,
2016.
Wang, Y., Ren, J., Huang, X. H. H., Tong, R., and Yu, J. Z.: Synthesis of
four monoterpene-derived organosulfates and their quantification in
atmospheric aerosol samples, Environ. Sci. Technol., 51, 6791–6801,
https://doi.org/10.1021/acs.est.7b01179, 2017.
Wang, Y., Hu, M., Guo, S., Wang, Y., Zheng, J., Yang, Y., Zhu, W., Tang, R., Li, X., Liu, Y., Le Breton, M., Du, Z., Shang, D., Wu, Y., Wu, Z., Song, Y., Lou, S., Hallquist, M., and Yu, J.: The secondary formation of organosulfates under interactions between biogenic emissions and anthropogenic pollutants in summer in Beijing, Atmos. Chem. Phys., 18, 10693–10713, https://doi.org/10.5194/acp-18-10693-2018, 2018.
Wang, Y., Zhao, Y., Wang, Y., Yu, J.-Z., Shao, J., Liu, P., Zhu, W., Cheng, Z., Li, Z., Yan, N., and Xiao, H.: Organosulfates in atmospheric aerosols in Shanghai, China: seasonal and interannual variability, origin, and formation mechanisms, Atmos. Chem. Phys., 21, 2959–2980, https://doi.org/10.5194/acp-21-2959-2021, 2021.
Wilsey, S., Dowd, P., and Houk, K. N.: Effect of alkyl substituents and ring
size on alkoxy radical cleavage reactions, J. Organ. Chem., 64, 8801–8811,
https://doi.org/10.1021/jo990652+, 1999.
Xu, R., Ge, Y., Kwong, K. C., Poon, H. Y., Wilson, K. R., Yu, J. Z., and
Chan, M. N.: Inorganic sulfur species formed upon heterogeneous OH oxidation
of organosulfates: a case study of methyl sulfate, ACS Earth Space Chem., 4,
2041–2049, https://doi.org/10.1021/acsearthspacechem.0c00209, 2020a.
Xu, R., Lam, H. K., Wilson, K. R., Davies, J. F., Song, M., Li, W., Tse, Y.-L. S., and Chan, M. N.: Effect of inorganic-to-organic mass ratio on the heterogeneous OH reaction rates of erythritol: implications for atmospheric chemical stability of 2-methyltetrols, Atmos. Chem. Phys., 20, 3879–3893, https://doi.org/10.5194/acp-20-3879-2020, 2020b.
Yamazaki, Y., Naganuma, J., and Gotoh, H.: A Theoretical, dynamical
evaluation method of the steric hindrance in nitroxide radicals using
transition states of model reactions, Sci. Rep., 9, 20339,
https://doi.org/10.1038/s41598-019-56342-w, 2019.
You, Y., Smith, M. L., Song, M., Martin, S. T., and Bertram, A. K.:
Liquid–liquid phase separation in atmospherically relevant particles
consisting of organic species and inorganic salts, Int. Rev. Phys. Chem.,
33, 43–77, https://doi.org/10.1080/0144235x.2014.890786, 2014.
Zhang, H., Worton, D. R., Lewandowski, M., Ortega, J., Rubitschun, C. L.,
Park, J.-H., Kristensen, K., Campuzano-Jost, P., Day, D. A., Jimenez, J. L.,
Jaoui, M., Offenberg, J. H., Kleindienst, T. E., Gilman, J., Kuster, W. C.,
de Gouw, J., Park, C., Schade, G. W., Frossard, A. A., Russell, L., Kaser,
L., Jud, W., Hansel, A., Cappellin, L., Karl, T., Glasius, M., Guenther, A.,
Goldstein, A. H., Seinfeld, J. H., Gold, A., Kamens, R. M., and Surratt, J.
D.: Organosulfates as tracers for Secondary Organic Aerosol (SOA) formation
from 2-Methyl-3-Buten-2-ol (MBO) in the atmosphere, Environ. Sci. Technol.,
46, 9437–9446, https://doi.org/10.1021/es301648z, 2012.
Short summary
To date, while over a hundred organosulfates (OSs) have been detected in atmospheric aerosols, many of them are still unidentified, with unknown precursors and formation processes. We found the heterogeneous OH oxidation of an α-pinene-derived organosulfate (C10H17O5SNa, αpOS-249, αpOS-249) can proceed at an efficient rate and transform into more oxygenated OSs, which have been commonly detected in atmospheric aerosols and α-pinene-derived SOA in chamber studies.
To date, while over a hundred organosulfates (OSs) have been detected in atmospheric aerosols,...
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