Articles | Volume 18, issue 4
https://doi.org/10.5194/acp-18-2809-2018
© Author(s) 2018. 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-18-2809-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
27 Feb 2018
Research article |
| 27 Feb 2018
| 27 Feb 2018
Importance of sulfate radical anion formation and chemistry in heterogeneous OH oxidation of sodium methyl sulfate, the smallest organosulfate
Kai Chung Kwong
Earth System Science Programme, Faculty of Science, The Chinese
University of Hong Kong, Hong Kong, China
Man Mei Chim
Earth System Science Programme, Faculty of Science, The Chinese
University of Hong Kong, Hong Kong, China
James F. Davies
Chemical Sciences
Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA
now at: Department of Chemistry, University of California
Riverside, Riverside, CA, USA
Kevin R. Wilson
Chemical Sciences
Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA
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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Hoi Ki Lam, Kai Chung Kwong, Hon Yin Poon, James F. Davies, Zhenfa Zhang, Avram Gold, Jason D. Surratt, and Man Nin Chan
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Organosulfates are ubiquitous in the atmosphere. We find that chemical transformation of IEPOX-derived organosulfates, one of the most abundant organosulfates, can generate inorganic sulfate through heterogeneous OH oxidation. The findings of this work provide new reaction pathways for recycling of inorganic and organic sulfur and may suggest that organosulfates could be reservoirs of inorganic sulfates in the atmosphere.
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This research explores how organosulfate surfactants affect aerosol particles and their response to changes in relative humidity in the atmosphere. Using optical trapping and strong electric fields to investigate single particles, it is found that these surfactants can significantly lower surface tension, even in very small amounts. These findings are important for understanding how such particles influence cloud formation and properties like brightness.
Rani Jeong, Joseph Lilek, Andreas Zuend, Rongshuang Xu, Man Nin Chan, Dohyun Kim, Hi Gyu Moon, and Mijung Song
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In this study, the viscosities of particles of sucrose–H2O, AS–H2O, and sucrose–AS–H2O for OIRs of 4:1, 1:1, and 1:4 for decreasing RH, were quantified by poke-and-flow and bead-mobility techniques at 293 ± 1 K. Based on the viscosity results, the particles of binary and ternary systems ranged from liquid to semisolid, and even the solid state depending on the RH. Moreover, we compared the measured viscosities of ternary systems to the predicted viscosities with excellent agreement.
Rongshuang Xu, Sze In Madeleine Ng, Wing Sze Chow, Yee Ka Wong, Yuchen Wang, Donger Lai, Zhongping Yao, Pui-Kin So, Jian Zhen Yu, and Man Nin Chan
Atmos. Chem. Phys., 22, 5685–5700, https://doi.org/10.5194/acp-22-5685-2022, https://doi.org/10.5194/acp-22-5685-2022, 2022
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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.
Young-Chul Song, Joseph Lilek, Jae Bong Lee, Man Nin Chan, Zhijun Wu, Andreas Zuend, and Mijung Song
Atmos. Chem. Phys., 21, 10215–10228, https://doi.org/10.5194/acp-21-10215-2021, https://doi.org/10.5194/acp-21-10215-2021, 2021
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We report viscosity of binary mixtures of organic material / H2O and inorganic salts / H2O, as well as ternary mixtures of organic material / inorganic salts/ H2O, over the atmospheric relative humidity (RH) range. The viscosity measurements indicate that the studied mixed organic–inorganic particles range in phase state from liquid to semi-solid or even solid across the atmospheric RH range at a temperature of 293 K.
Hoi Ki Lam, Rongshuang Xu, Jack Choczynski, James F. Davies, Dongwan Ham, Mijung Song, Andreas Zuend, Wentao Li, Ying-Lung Steve Tse, and Man Nin Chan
Atmos. Chem. Phys., 21, 2053–2066, https://doi.org/10.5194/acp-21-2053-2021, https://doi.org/10.5194/acp-21-2053-2021, 2021
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This work demonstrates that organic compounds present at or near the surface of aerosols can be subjected to oxidation initiated by gas-phase oxidants, such as hydroxyl radicals (OH). The heterogeneous reactivity is sensitive to their surface concentrations, which are determined by the phase separation behavior. This results of this work emphasize the effects of phase separation and potentially distinct aerosol morphologies on the chemical transformation of atmospheric aerosols.
Rongshuang Xu, Hoi Ki Lam, Kevin R. Wilson, James F. Davies, Mijung Song, Wentao Li, Ying-Lung Steve Tse, and Man Nin Chan
Atmos. Chem. Phys., 20, 3879–3893, https://doi.org/10.5194/acp-20-3879-2020, https://doi.org/10.5194/acp-20-3879-2020, 2020
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Atmospheric particles, a complex mixture of inorganic salts, organic compounds and water, can continually undergo heterogeneous oxidation initiated by gas-phase oxidants at the particle surface. We found that ammonium sulfate can decelerate the rate of heterogeneous OH reaction with 2-methyltetrols when the inorganic-to-organic mass ratio increases. These results would suggest 2-methyltetrols are likely chemically stable against heterogeneous OH oxidation in the atmosphere.
Hoi Ki Lam, Sze Man Shum, James F. Davies, Mijung Song, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 19, 9581–9593, https://doi.org/10.5194/acp-19-9581-2019, https://doi.org/10.5194/acp-19-9581-2019, 2019
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We show the presence of dissolved inorganic salts could reduce the overall heterogeneous reactivity of organic compounds with gas–phase OH radicals at the surface by lowering the surface concentration of organic compounds. Until recently, the kinetic parameters reported in the literature were mostly measured based on experiments with pure organic particles. The lifetime of organic compounds or chemical tracers against heterogeneous OH reaction in the atmosphere could be longer than expected.
James F. Davies, Andreas Zuend, and Kevin R. Wilson
Atmos. Chem. Phys., 19, 2933–2946, https://doi.org/10.5194/acp-19-2933-2019, https://doi.org/10.5194/acp-19-2933-2019, 2019
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The formation of cloud droplets involves the condensation of water onto preexisting particles in the atmosphere. The efficiency of this process depends on the nature of the particles, and recent work has shown that organic-rich particles may exhibit a suppressed surface tension that promotes the formation of cloud droplets. In this technical note, we discuss the mechanism for this and highlight the evolution of surface tension as the key factor in the extent of surface effects.
Hoi Ki Lam, Kai Chung Kwong, Hon Yin Poon, James F. Davies, Zhenfa Zhang, Avram Gold, Jason D. Surratt, and Man Nin Chan
Atmos. Chem. Phys., 19, 2433–2440, https://doi.org/10.5194/acp-19-2433-2019, https://doi.org/10.5194/acp-19-2433-2019, 2019
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Organosulfates are ubiquitous in the atmosphere. We find that chemical transformation of IEPOX-derived organosulfates, one of the most abundant organosulfates, can generate inorganic sulfate through heterogeneous OH oxidation. The findings of this work provide new reaction pathways for recycling of inorganic and organic sulfur and may suggest that organosulfates could be reservoirs of inorganic sulfates in the atmosphere.
Man Mei Chim, Chiu Tung Cheng, James F. Davies, Thomas Berkemeier, Manabu Shiraiwa, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 17, 14415–14431, https://doi.org/10.5194/acp-17-14415-2017, https://doi.org/10.5194/acp-17-14415-2017, 2017
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In this work, we report that methyl-substituted succinic acid present at or near the surface of aqueous organic droplets can be efficiently oxidized by gas-phase OH radicals. The alkoxy radical chemistry appears to be an important reaction pathway. In addition, our model simulations reveal the relative importance of functionalization and fragmentation processes, alongside volatilization, in the evolution of the particle-phase reaction, which is largely dependent on the extent of oxidation.
M. R. Canagaratna, J. L. Jimenez, J. H. Kroll, Q. Chen, S. H. Kessler, P. Massoli, L. Hildebrandt Ruiz, E. Fortner, L. R. Williams, K. R. Wilson, J. D. Surratt, N. M. Donahue, J. T. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, https://doi.org/10.5194/acp-15-253-2015, 2015
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Atomic oxygen-to-carbon (O:C), hydrogen-to-carbon (H:C), and organic mass-to-organic carbon (OM:OC) ratios of ambient organic aerosol (OA) species provide key constraints for understanding their sources and impacts. Here an improved method for obtaining accurate O:C, H:C, and OM:OC with a widely used aerosol mass spectrometer is developed. These results imply that OA is more oxidized than previously estimated and indicate the need for new chemical mechanisms that simulate ambient oxidation.
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Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
The importance of burning conditions on the composition of domestic biomass-burning organic aerosol and the impact of atmospheric ageing
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The lifetimes and potential change in planetary albedo owing to the oxidation of thin surfactant organic films extracted from atmospheric aerosol by hydroxyl (OH) radicals at the air–water interface of particles
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Heterogeneous formation and light absorption of secondary organic aerosols from acetone photochemical reactions: remarkably enhancing effects of seeds and ammonia
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Recent research has established the contribution of 1,3-butadiene (13BD) to organic aerosol formation with negative implications for urban air quality. Health effect 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 seed aerosol acidity on the chemical composition of aerosol formed from 13BD photooxidation.
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.
Yuchen Wang, Xiang Zhang, Yuanlong Huang, Yutong Liang, and Nga L. Ng
EGUsphere, https://doi.org/10.5194/egusphere-2024-3849, https://doi.org/10.5194/egusphere-2024-3849, 2024
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This work provides the first fundamental laboratory data to evaluate SOA production from styrene+NO3 chemistry. Additionally, the formation mechanisms of aromatic ONs are reported for the first time, highlighting that previously identified nitroaromatics in ambient field campaigns can be aromatic ONs. Finally, the hydrolysis lifetime observed for ONs generated from styrene+NO3 oxidation can serve as experimentally constrained parameter for modeling hydrolysis of aromatic ONs in general.
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.
Kathleen A. Thompson, Paul Bieber, Anna J. Miller, Nicole Link, Benjamin J. Murray, and Nadine Borduas-Dedekind
EGUsphere, https://doi.org/10.5194/egusphere-2024-2827, https://doi.org/10.5194/egusphere-2024-2827, 2024
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Lignin and Snomax are surface-active macromolecules that show a relationship between increasing concentrations, decreasing surface tension, and increasing ice-nucleating ability. However, this relationship did not hold for agricultural soil extracts collected in the UK and Canada. Hydrophobic interfaces play an important role in the ice-nucleating activity of organic matter; as the complexity of the sample increases, the hydrophobic interfaces in the bulk compete with the air-water interface.
Sergio Harb, Manuela Cirtog, Stéphanie Alage, Christopher Cantrell, Mathieu Cazaunau, Vincent Michoud, Edouard Pangui, Antonin Bergé, Chiara Giorio, Francesco Battaglia, and Bénédicte Picquet-Varrault
EGUsphere, https://doi.org/10.5194/egusphere-2024-3419, https://doi.org/10.5194/egusphere-2024-3419, 2024
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We investigated the reactions of α- and β-phellandrenes (from vegetation emissions) with NO3 radicals, a major nighttime oxidant from human activities. Using lab-based simulations, we examined these reactions and measured particle formation and by-products. Our findings reveal that α- and β-phellandrenes are efficient particle sources and enhance our understanding of biogenic-anthropogenic interactions and their contributions to atmospheric changes affecting climate and health.
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.
Michael Oluwatoyin Sunday, Laura Marie Dahler Heinlein, Junwei He, Allison Moon, Sukriti Kapur, Ting Fang, Kasey C. Edwards, Fangzhou Guo, Jack Dibb, James H. Flynn III, Becky Alexander, Manabu Shiraiwa, and Cort Anastasio
EGUsphere, https://doi.org/10.5194/egusphere-2024-3272, https://doi.org/10.5194/egusphere-2024-3272, 2024
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Hydrogen peroxide (HOOH) is an important oxidant that forms atmospheric sulfate. We demonstrate that illumination of brown carbon can rapidly form HOOH within particles, even under the low sunlight conditions of Fairbanks, Alaska during winter. This in-particle formation of HOOH is fast enough that it forms sulfate at significant rates. In contrast, the formation of HOOH in the gas phase during the campaign is expected to be negligible because of high NOx levels.
Kevin Kilchhofer, Markus Ammann, Laura Torrent, Ka Yuen Cheung, and Peter Aaron Alpert
EGUsphere, https://doi.org/10.5194/egusphere-2024-3226, https://doi.org/10.5194/egusphere-2024-3226, 2024
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Aerosol particles composed of metal complexes generate radicals as the result of photochemical reactions. Reactive species generated are hazardous to human health. We report microscopy data with particles composed of an organic proxy exposed to UV light. We found that copper influenced the reoxidation and initial iron reduction via photolysis of the complex. New model results suggest that we need to account a decreased photochemical activity and use a copper-induced reoxidation reaction.
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.
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.
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.
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.
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Short summary
To date, it remains unclear how organosulfates evolve over time in the atmosphere. We demonstrate that heterogeneous OH oxidation of sodium methyl sulfate, the smallest organosulfate found in atmospheric aerosols, is efficient. The oxidation can lead to the formation of sulfate radical anion and produce inorganic sulfate. In addition to OH radicals, sulfate radical anion chemistry can play a role in determining the evolution of sodium methyl sulfate and other organosulfates during oxidation.
To date, it remains unclear how organosulfates evolve over time in the atmosphere. We...
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