Articles | Volume 20, issue 6
https://doi.org/10.5194/acp-20-3879-2020
© Author(s) 2020. 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-20-3879-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
31 Mar 2020
Research article |
| 31 Mar 2020
| 31 Mar 2020
Effect of inorganic-to-organic mass ratio on the heterogeneous OH reaction rates of erythritol: implications for atmospheric chemical stability of 2-methyltetrols
Rongshuang Xu
Earth System Science Programme, Faculty of Science, The Chinese
University of Hong Kong, Hong Kong, Hong Kong SAR, China
Hoi Ki Lam
Earth System Science Programme, Faculty of Science, The Chinese
University of Hong Kong, Hong Kong, Hong Kong SAR, China
Kevin R. Wilson
Chemical Sciences Division, Lawrence Berkeley National Laboratory,
Berkeley, CA, USA
James F. Davies
Department of Chemistry, University of California Riverside,
Riverside, CA, USA
Mijung Song
Department of Earth and Environmental Sciences, Jeonbuk National
University, Jeonju, Jeollabuk-do, Republic of Korea
Wentao Li
Department of Chemistry, The Chinese University of Hong Kong, Hong
Kong, Hong Kong SAR, China
Ying-Lung Steve Tse
Department of Chemistry, The Chinese University of Hong Kong, Hong
Kong, Hong Kong SAR, China
Man Nin Chan
CORRESPONDING AUTHOR
Earth System Science Programme, Faculty of Science, The Chinese
University of Hong Kong, Hong Kong, Hong Kong SAR, China
The Institute of Environment, Energy and Sustainability, The Chinese
University of Hong Kong, Hong Kong, Hong Kong SAR, China
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M. Song, P. F. Liu, S. J. Hanna, Y. J. Li, S. T. Martin, and A. K. Bertram
Atmos. Chem. Phys., 15, 5145–5159, https://doi.org/10.5194/acp-15-5145-2015, https://doi.org/10.5194/acp-15-5145-2015, 2015
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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.
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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The chemical composition of organic aerosol derived from wood-burning emissions under different burning conditions was characterised. Fresh emissions from flaming and smouldering were largely aromatic in nature, whereas upon aging the aromatic content decreased. This decrease was greater for smouldering due to the loss of toxic polyaromatic species, whereas under flaming conditions highly toxic polyaromatic species were produced. These differences present an important challenge for future policy.
Yueyao Yang, Yahui Liu, Guohua Zhu, Bingcheng Lin, Shanshan Zhang, Xin Li, Fangxi Xu, He Niu, Rong Jin, and Minghui Zheng
Atmos. Chem. Phys., 25, 3981–3994, https://doi.org/10.5194/acp-25-3981-2025, https://doi.org/10.5194/acp-25-3981-2025, 2025
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Halogenated polycyclic aromatic hydrocarbons (XPAHs) are emerging pollutants. Stability during atmospheric transformation processes is crucial for predicting their environmental fate and assessing the associated risks. Here, we conducted field studies and laboratory simulation experiments to reveal the mechanisms, influencing factors and products for XPAHs' heterogeneous phototransformation. Results revealed that the conversion of XPAHs led to a reduction in environmental risk.
Marcel Müller, Marcel Reichmuth, and Ulrich Karl Krieger
EGUsphere, https://doi.org/10.5194/egusphere-2025-1238, https://doi.org/10.5194/egusphere-2025-1238, 2025
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The initiation of autoxidation by ozonolysis was investigated on levitated linoleic acid droplets using electrodynamic balance–mass spectrometry. Exposing the droplets to ozone for one hour before switching the gas phase to air without ozone led to a shortening of the autoxidation initiation phase in comparison to experiments without ozone exposure. Results were compared to a bulk reaction model to investigate the synergistic effects of ozonolysis and autoxidation.
Monika Łożyńska, Marzena Trojanowska, Artur Molik, and Ryszard Świetlik
EGUsphere, https://doi.org/10.5194/egusphere-2025-541, https://doi.org/10.5194/egusphere-2025-541, 2025
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The assessment of chromium occurrence in particulate matter in cities: PM10, PM2.5, PM1 and PM0.25 during the calendar year was presented. The seasonality of both pseudototal chromium content and its valence speciation was examined. Seasonality of changes in Crtot and Cr(VI) concentrations was observed. Maximum in the winter season, most likely due to the greater share of fuel combustion sources. Regardless of the season, the risk levels for Radom residents were within the acceptable risk range.
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
Atmos. Chem. Phys., 25, 3503–3518, https://doi.org/10.5194/acp-25-3503-2025, https://doi.org/10.5194/acp-25-3503-2025, 2025
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Understanding the surface composition of aerosols is crucial for advancing climate models. We investigated the interface of single-component and mixed aqueous solutions of atmospherically relevant carboxylic acid and alkyl-ammonium ions using liquid-jet photoelectron spectroscopy. An exponential increase in surface propensity as a function of chain length was found for the single species, and cooperative effects in the mixtures cause a further drastic increase in surface solute concentration.
Qun Zhang, Wei Zhou, Shanshan Tang, Kai Huang, Jie Fu, Zechen Yu, Yunhe Teng, Shuyi Shen, Yang Mei, Xuezhi Yang, Jianjie Fu, and Guibin Jiang
EGUsphere, https://doi.org/10.5194/egusphere-2025-1028, https://doi.org/10.5194/egusphere-2025-1028, 2025
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This article comprehensively investigates the aqueous-phase OH oxidation of benzothiazoles (BTs), common rubber additives found in urban air, through laboratory simulation experiments. BTs can rapidly degrade, leading to light absorption, high yields of sulfate, and the formation of highly oxidized and/or oligomerized organic compounds. The results reveal that aqueous-phase BTs can contribute to secondary aerosols, altering the chemical and optical properties of atmospheric particles.
Tao Cao, Cuncun Xu, Hao Chen, Jianzhong Song, Jun Li, Haiyan Song, Bin Jiang, Yin Zhong, and Ping’an Peng
EGUsphere, https://doi.org/10.5194/egusphere-2025-561, https://doi.org/10.5194/egusphere-2025-561, 2025
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This study investigated the evolution of biomass and coal combustion-derived WSOM during aqueous photochemical process. The results indicate that photochemical aging induces distinct changes in the optical and molecular properties of WSOM and more pronounced alterations were observed during ·OH photooxidation than direct photolysis. Notably, our results also demostrated that atmospheric photooxidation may represent a significant source of BC-like substances.
Yuting Lyu, Taekyu Joo, Ruihan Ma, Mark Kristan Espejo Cabello, Tianye Zhou, Shun Yeung, Cheuk Ki Wong, Yifang Gu, Yiming Qin, and Theodora Nah
EGUsphere, https://doi.org/10.5194/egusphere-2025-570, https://doi.org/10.5194/egusphere-2025-570, 2025
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We investigated the aqueous nitrate-mediated photooxidation of four green leaf volatiles (GLVs). The aqueous reaction medium conditions, dilute cloud/fog vs. concentrated aqueous aerosol conditions, governed the effects that pH, ionic strength, and sulfate have on the GLV degradation rates and aqSOA mass yields. Most notably, reactions initiated by sulfate photolysis have significant effects in aqueous aerosols, but not in cloud/fog droplets.
Rosalie H. Shepherd, Martin D. King, Andrew D. Ward, Edward J. Stuckey, Rebecca J. L. Welbourn, Neil Brough, Adam Milsom, Christian Pfrang, and Thomas Arnold
Atmos. Chem. Phys., 25, 2569–2588, https://doi.org/10.5194/acp-25-2569-2025, https://doi.org/10.5194/acp-25-2569-2025, 2025
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Thin film formation at the air–water interface from material extracted from atmospheric aerosol was demonstrated, supporting the core–shell morphology. Film thicknesses were approximately 10 Å and 17 Å for urban and remote extracts, respectively. Exposure to gas-phase OH radicals showed fast reactions and short lifetimes of around 1 h. The effect on the Earth's radiative balance indicated that removing half of the film could significantly increase the top-of-atmosphere albedo for urban films.
Marwa Shahin, Julien Kammer, Brice Temime-Roussel, and Barbara D'Anna
EGUsphere, https://doi.org/10.5194/egusphere-2025-833, https://doi.org/10.5194/egusphere-2025-833, 2025
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Air pollution and climate change are influenced by tiny airborne particles called aerosols. This study explores how pollutants from urban sources, as m-xylene and naphthalene, form new particles in the atmosphere under different conditions. Using advanced techniques, we show how temperature and nitrogen oxides affect the formation and behaviour of these particles. Our findings will improve our understanding on secondary organic particle and air quality models.
Laura Marie Dahler Heinlein, Junwei He, Michael Oluwatoyin Sunday, Fangzhou Guo, James Campbell, Allison Moon, Sukriti Kapur, Ting Fang, Kasey Edwards, Meeta Cesler-Maloney, Alyssa J. Burns, Jack Dibb, William Simpson, Manabu Shiraiwa, Becky Alexander, Jingqiu Mao, James H. Flynn III, Jochen Stutz, and Cort Anastasio
EGUsphere, https://doi.org/10.5194/egusphere-2025-824, https://doi.org/10.5194/egusphere-2025-824, 2025
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High-latitude cities like Fairbanks, Alaska, experience severe wintertime pollution episodes. While conventional wisdom holds that oxidation is slow under these conditions, field measurements find oxidized products in particles. To explore this, we measured oxidants in aqueous extracts of winter particles from Fairbanks. We find high concentrations of oxidants during illumination, indicating that particle photochemistry can be significant even in high latitudes during winter.
Rui Jin, Wei Hu, Peimin Duan, Ming Sheng, Dandan Liu, Ziye Huang, Mutong Niu, Libin Wu, Junjun Deng, and Pingqing Fu
Atmos. Chem. Phys., 25, 1805–1829, https://doi.org/10.5194/acp-25-1805-2025, https://doi.org/10.5194/acp-25-1805-2025, 2025
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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 exometabolites and have significant variations in metabolism among different strains. These insights are pivotal for assessing the biogeochemical impacts of atmospheric microorganisms following their deposition.
Sophie Bogler, Jun Zhang, Rico K. Y. Cheung, Kun Li, Andre S. H. Prevot, Imad El Haddad, and David M. Bell
EGUsphere, https://doi.org/10.5194/egusphere-2025-385, https://doi.org/10.5194/egusphere-2025-385, 2025
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Authentic aerosols emitted from residential wood stoves and open burning processes are only slightly oxidized by ozone in the atmosphere. Under dry conditions the reaction does not proceed to completion, while under high humidity conditions the reactivity proceeds further. These results indicate the reactivity with ozone is likely impacted by aerosol phase state (e.g. aerosol viscosity).
Michel Legrand, Mstislav Vorobyev, Daria Bokuchava, Stanislav Kutuzov, Andreas Plach, Andreas Stohl, Alexandra Khairedinova, Vladimir Mikhalenko, Maria Vinogradova, Sabine Eckhardt, and Susanne Preunkert
Atmos. Chem. Phys., 25, 1385–1399, https://doi.org/10.5194/acp-25-1385-2025, https://doi.org/10.5194/acp-25-1385-2025, 2025
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Past atmospheric NH3 pollution in south-eastern Europe was reconstructed by analysing ammonium in an ice core drilled at the Mount Elbrus (Caucasus, Russia). The observed 3.5-fold increase in ice concentrations between 1750 and 1990 CE is in good agreement with estimated past dominant ammonia emissions from agriculture, mainly from south European Russia and Türkiye. In contrast to present-day conditions, the ammonium level observed in 1750 CE indicates significant natural emissions at that time.
Mohammed Jaoui, Klara Nestorowicz, Krzysztof J. Rudzinski, Michael Lewandowski, Tadeusz E. Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, and Rafal Szmigielski
Atmos. Chem. Phys., 25, 1401–1432, https://doi.org/10.5194/acp-25-1401-2025, https://doi.org/10.5194/acp-25-1401-2025, 2025
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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.
Francesco Battaglia, Paola Formenti, Chiara Giorio, Mathieu Cazaunau, Edouard Pangui, Antonin Bergé, Aline Gratien, Thomas Bertin, Joël F. de Brito, Manolis N. Romanias, Vincent Michoud, Clarissa Baldo, Servanne Chevaillier, Gaël Noyalet, Philippe Decorse, Bénédicte Picquet-Varrault, and Jean-François Doussin
EGUsphere, https://doi.org/10.5194/egusphere-2024-4073, https://doi.org/10.5194/egusphere-2024-4073, 2025
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This paper presents an experimental investigation of the interactions between glyoxal, an important volatile organic compound, and mineral dust particles of size and composition typical of natural conditions. We show that their interactions modifies in a definitive way the concentrations of the gas phase and the properties of the dust, which could have important implications of the atmospheric composition and the Earth's climate.
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.
Anni Hartikainen, Mika Ihalainen, Deeksha Shukla, Marius Rohkamp, Arya Mukherjee, Quanfu He, Sandra Piel, Aki Virkkula, Delun Li, Tuukka Kokkola, Seongho Jeong, Hanna Koponen, Uwe Etzien, Anusmita Das, Krista Luoma, Lukas Schwalb, Thomas Gröger, Alexandre Barth, Martin Sklorz, Thorsten Streibel, Hendryk Czech, Benedikt Gündling, Markus Kalberer, Bert Buchholz, Andreas Hupfer, Thomas Adam, Thorsten Hohaus, Johan Øvrevik, Ralf Zimmermann, and Olli Sippula
EGUsphere, https://doi.org/10.5194/egusphere-2024-3836, https://doi.org/10.5194/egusphere-2024-3836, 2025
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Photochemical reactions altered the properties of kerosene-operated jet engine burner exhaust emissions, which were studied in laboratory using an oxidation flow reactor. Particle mass increased 300-fold as particles and gases became more oxidized. Light absorption increased, but the total direct radiative forcing efficiency was estimated to shift from positive to negative. The results highlight the importance of considering secondary aerosol formation when assessing the impacts of aviation.
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.
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.
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
Short summary
Short summary
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.
Cited articles
Abbatt, J. P. D., Lee, A. K. Y., and Thornton, J. A.: Quantifying trace gas uptake to tropospheric aerosol: recent advances and remaining challenges, Chem. Soc. Rev., 41, 6555–6581, 2012.
Anastasio, C. and Newberg, J. T.: Sources and sinks of hydroxyl radical in
sea-salt particles, J. Geophys. Res.-Atmos., 112, D10306, https://doi.org/10.1029/2006jd008061,
2007.
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.
Bethel, H. L., Atkinson, R., and Arey, J.: Hydroxycarbonyl products of the
reactions of selected diols with the OH radical, J. Phys. Chem. A, 107,
6200–6205, https://doi.org/10.1021/jp027693l, 2003.
Bothe, E., Schuchmann, M. N., Schulte-Frohlinde, D., and Sonntag, C. V.:
HO2 elimination from α-hydroxyalkylperoxyl radicals in aqueous
solution, Photochem. Photobiol., 28, 639–643,
https://doi.org/10.1111/j.1751-1097.1978.tb06984.x, 1978a.
Bothe, E., Schulte-Frohlinde, D., and Sonntag, C. V.: Radiation chemistry of
carbohydrates. Part 16. Kinetics of HO2 elimination from peroxyl
radicals derived from glucose and polyhydric alcohols, J. Chem. Soc., 2, 416, https://doi.org/10.1039/p29780000416, 1978b.
Bothe, E., Schuchmann, M. N., Schulte-Frohlinde, D., and Sonntag, C. V.:
Hydroxyl radical-induced oxidation of ethanol in oxygenated aqueous
solutions. a pulse radiolysis and product study, Zeitschrift für
Naturforschung B, 38, 212–219, https://doi.org/10.1515/znb-1983-0218, 1983.
Boyer, H. C. and Dutcher, C. S.: Atmospheric aqueous aerosol surface
tensions: isotherm-based modeling and biphasic microfluidic measurements, J.
Phys. Chem. A, 121, 4733–4742, https://doi.org/10.1021/acs.jpca.7b03189, 2017.
Braban, C. F. and Abbatt, J. P. D.: A study of the phase transition behavior of internally mixed ammonium sulfate – malonic acid aerosols, Atmos. Chem. Phys., 4, 1451–1459, https://doi.org/10.5194/acp-4-1451-2004, 2004.
Budisulistiorini, S. H., Canagaratna, M. R., Croteau, P. L., Marth, W. J.,
Baumann, K., Edgerton, E. S., Shaw, S. L., Knipping, E. M., Worsnop, D. R.,
Jayne, J. T., Gold, A., and Surratt, J. D.: Real-time continuous
characterization of secondary organic aerosol derived from isoprene
epoxydiols in downtown Atlanta, Georgia, using the aerodyne aerosol chemical
speciation monitor, Environ. Sci. Technol., 47, 5686–5694,
https://doi.org/10.1021/es400023n, 2013.
Carlton, A. G., Wiedinmyer, C., and Kroll, J. H.: A review of Secondary Organic Aerosol (SOA) formation from isoprene, Atmos. Chem. Phys., 9, 4987–5005, https://doi.org/10.5194/acp-9-4987-2009, 2009.
Chan, M. N., Nah, T., and Wilson, K. R.: Real time in situ chemical
characterization of sub-micron organic aerosols using Direct Analysis in
Real Time mass spectrometry (DART-MS): the effect of aerosol size and
volatility, The Analyst, 138, 3749, https://doi.org/10.1039/c3an00168g, 2013.
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.
Chapleski Jr., R. C., Zhang, Y., Troyaa, D., and Morris, J. R.: Heterogeneous chemistry and reaction dynamics of the atmospheric oxidants, O3, NO3, and OH, on organic surfaces, Chem. Soc. Rev., 45, 3731–3746, 2016.
Cheng, C. T., Chan, M. N., and Wilson, K. R.: Importance of unimolecular
HO2 elimination in the heterogeneous OH reaction of highly oxygenated
tartaric acid aerosol, J. Phys. Chem. A, 120, 5887–5896,
https://doi.org/10.1021/acs.jpca.6b05289, 2016.
Chim, M. M., Cheng, C. T., Davies, J. F., Berkemeier, T., Shiraiwa, M., Zuend, A., and Chan, M. N.: Compositional evolution of particle-phase reaction products and water in the heterogeneous OH oxidation of model aqueous organic aerosols, Atmos. Chem. Phys., 17, 14415–14431, https://doi.org/10.5194/acp-17-14415-2017, 2017a.
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, 2017b.
Chim, M. M., Lim, C. Y., Kroll, J. H., and Chan, M. N.: Evolution in the
reactivity of citric acid toward heterogeneous oxidation by gas-phase OH
radicals, ACS Earth Space Chem., 2, 1323–1329,
https://doi.org/10.1021/acsearthspacechem.8b00118, 2018.
Chu, Y., Evoy, E., Kamal, S., Song, Y. C., Reid, J. P., Chan, C. K., and Bertram, A. K.: Viscosity of erythritol and erythritol–water particles as a function of water activity: new results and an intercomparison of techniques for measuring the viscosity of particles, Atmos. Meas. Tech., 11, 4809–4822, https://doi.org/10.5194/amt-11-4809-2018, 2018.
Claeys, M.: Formation of secondary organic aerosols through photooxidation
of isoprene, Science, 303, 1173–1176, https://doi.org/10.1126/science.1092805, 2004.
Cody, R. B., Laramée, J. A., and Durst, H. D.: Versatile new ion source
for the analysis of materials in open air under ambient conditions, Anal.
Chem., 77, 2297–2302, https://doi.org/10.1021/ac050162j, 2005.
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.
Cooper, P. L. and Abbatt, J. P. D.: Heterogeneous Interactions of OH and HO2
Radicals with Surfaces Characteristic of Atmospheric Particulate Matter, J.
Phys. Chem., 100, 2249–2254, https://doi.org/10.1021/jp952142z, 1996.
D'Ambro, E. L., Lee, B. H., Liu, J., Shilling, J. E., Gaston, C. J., Lopez-Hilfiker, F. D., Schobesberger, S., Zaveri, R. A., Mohr, C., Lutz, A., Zhang, Z., Gold, A., Surratt, J. D., Rivera-Rios, J. C., Keutsch, F. N., and Thornton, J. A.: Molecular composition and volatility of isoprene photochemical oxidation secondary organic aerosol under low- and high-NOx conditions, Atmos. Chem. Phys., 17, 159–174, https://doi.org/10.5194/acp-17-159-2017, 2017.
Davies, J. F. and Wilson, K. R.: Nanoscale interfacial gradients formed by
the reactive uptake of OH radicals onto viscous aerosol surfaces, Chem.
Sci., 6, 7020–7027, https://doi.org/10.1039/c5sc02326b, 2015.
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.
Drewnick, F., Diesch, J.-M., Faber, P., and Borrmann, S.: Aerosol mass spectrometry: particle–vaporizer interactions and their consequences for the measurements, Atmos. Meas. Tech., 8, 3811–3830, https://doi.org/10.5194/amt-8-3811-2015, 2015.
Ekström, S., Nozière, B., and Hansson, H.-C.: The Cloud Condensation Nuclei (CCN) properties of 2-methyltetrols and C3-C6 polyols from osmolality and surface tension measurements, Atmos. Chem. Phys., 9, 973–980, https://doi.org/10.5194/acp-9-973-2009, 2009.
Enami, S., Hoffmann, M. R., and Colussi, A. J.: Extensive H-atom abstraction
from benzoate by OH-radicals at the air–water interface, Phys. Chem. Chem.
Phys., 18, 31505–31512, https://doi.org/10.1039/c6cp06652f, 2016.
Estillore, A. D., Trueblood, J. V., and Grassian, V. H.: Atmospheric
chemistry of bioaerosols: heterogeneous and multiphase reactions with
atmospheric oxidants and other trace gases, Chem. Sci., 7, 6604–6616,
https://doi.org/10.1039/c6sc02353c, 2016.
Fan, H., Tinsley, M. R., and Goulay, F.: Effect of relative humidity on the OH-initiated heterogeneous oxidation of monosaccharide nanoparticles, J. Phys. Chem. A, 119, 11182–11190, 2015.
Fan, H., Masaya, T. W., and Goulay, F.: Effect of surface–bulk partitioning
on the heterogeneous oxidation of aqueous saccharide aerosols, Phys. Chem.
Chem. Phys., 21, 2992–3001, https://doi.org/10.1039/c8cp06785f, 2019.
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.
Grayson, J. W., Evoy, E., Song, M., Chu, Y., Maclean, A., Nguyen, A., Upshur, M. A., Ebrahimi, M., Chan, C. K., Geiger, F. M., Thomson, R. J., and Bertram, A. K.: The effect of hydroxyl functional groups and molar mass on the viscosity of non-crystalline organic and organic–water particles, Atmos. Chem. Phys., 17, 8509–8524, https://doi.org/10.5194/acp-17-8509-2017, 2017.
Hajslova, J., Cajka, T., and Vaclavik, L.: Challenging applications offered
by direct analysis in real time (DART) in food-quality and safety analysis,
TrAC-Trend Anal. Chem., 30, 204–218,
https://doi.org/10.1016/j.trac.2010.11.001, 2011.
He, Q.-F., Ding, X., Fu, X.-X., Zhang, Y.-Q., Wang, J.-Q., Liu, Y.-X., Tang,
M.-J., Wang, X.-M., and Rudich, Y.: Secondary organic aerosol formation from
isoprene epoxides in the Pearl River Delta, South China: IEPOX- and
HMML-Derived Tracers, J. Geophys. Res.-Atmos., 123, 6999–7012,
https://doi.org/10.1029/2017jd028242, 2018.
Hu, W. W., Campuzano-Jost, P., Palm, B. B., Day, D. A., Ortega, A. M., Hayes, P. L., Krechmer, J. E., Chen, Q., Kuwata, M., Liu, Y. J., de Sá, S. S., McKinney, K., Martin, S. T., Hu, M., Budisulistiorini, S. H., Riva, M., Surratt, J. D., St. Clair, J. M., Isaacman-Van Wertz, G., Yee, L. D., Goldstein, A. H., Carbone, S., Brito, J., Artaxo, P., de Gouw, J. A., Koss, A., Wisthaler, A., Mikoviny, T., Karl, T., Kaser, L., Jud, W., Hansel, A., Docherty, K. S., Alexander, M. L., Robinson, N. H., Coe, H., Allan, J. D., Canagaratna, M. R., Paulot, F., and Jimenez, J. L.: Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements, Atmos. Chem. Phys., 15, 11807–11833, https://doi.org/10.5194/acp-15-11807-2015, 2015.
Hu, W., Palm, B. B., Day, D. A., Campuzano-Jost, P., Krechmer, J. E., Peng, Z., de Sá, S. S., Martin, S. T., Alexander, M. L., Baumann, K., Hacker, L., Kiendler-Scharr, A., Koss, A. R., de Gouw, J. A., Goldstein, A. H., Seco, R., Sjostedt, S. J., Park, J.-H., Guenther, A. B., Kim, S., Canonaco, F., Prévôt, A. S. H., Brune, W. H., and Jimenez, J. L.: Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA), Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, 2016.
Huang, Y., Barraza, K. M., Kenseth, C. M., Zhao, R., Wang, C., Beauchamp, J.
L., and Seinfeld, J. H.: Probing the OH oxidation of pinonic acid at the
air–water interface using Field-Induced Droplet Ionization Mass
Spectrometry (FIDI-MS), J. Phys. Chem. A., 122, 6445–6456,
https://doi.org/10.1021/acs.jpca.8b05353, 2018.
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.
Karadima, K. S., Mavrantzas, V. G., and Pandis, S. N.: Insights into the morphology of multicomponent organic and inorganic aerosols from molecular dynamics simulations, Atmos. Chem. Phys., 19, 5571–5587, https://doi.org/10.5194/acp-19-5571-2019, 2019.
Kessler, S. H., Smith, J. D., Che, D. L., Worsnop, D. R., Wilson, K. R., and
Kroll, J. H.: Chemical sinks of organic aerosol: kinetics and products of
the heterogeneous oxidation of erythritol and levoglucosan, Environ. Sci.
Technol., 44, 7005–7010, https://doi.org/10.1021/es101465m, 2010.
Kleindienst, T. E., Lewandowski, M., Offenberg, J. H., Edney, E. O., Jaoui,
M., Zheng, M., Ding, X., and Edgerton, E. S.: Contribution of primary and
secondary sources to organic aerosol and PM2.5 at SEARCH Network
Sites, J. Air Waste Manage. Assoc., 60, 1388–1399,
https://doi.org/10.3155/1047-3289.60.11.1388, 2010.
Kourtchev, I., Ruuskanen, T., Maenhaut, W., Kulmala, M., and Claeys, M.: Observation of 2-methyltetrols and related photo-oxidation products of isoprene in boreal forest aerosols from Hyytiälä, Finland, Atmos. Chem. Phys., 5, 2761–2770, https://doi.org/10.5194/acp-5-2761-2005, 2005.
Kroll, J. H., Lim, C. Y., Kessler, S. H., and Wilson, K. R.: 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, 2018a.
Kwong, K. C., Chim, M. M., Hoffmann, E. H., Tilgner, A., Herrmann, H.,
Davies, J. F., Wilson, K. R., and Chan, M. N.: Chemical transformation of
methanesulfonic acid and sodium methanesulfonate through heterogeneous OH
oxidation, ACS Earth Space Chem., 2, 895–903,
https://doi.org/10.1021/acsearthspacechem.8b00072, 2018b.
Laguerie, C., Aubry, M., and Couderc, J. P.: Some physicochemical data on monohydrate citric acid solutions in water: solubility, density, viscosity, diffusivity, pH of standard solution, and refractive index, J. Chem. Eng. Data, 21, 85–87, 1976.
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, 2019a.
Lam, H. K., Shum, S. M., Davies, J. F., Song, M., Zuend, A., and Chan, M. N.: Effects of inorganic salts on the heterogeneous OH oxidation of organic compounds: insights from methylglutaric acid–ammonium sulfate, Atmos. Chem. Phys., 19, 9581–9593, https://doi.org/10.5194/acp-19-9581-2019, 2019b.
Lewandowski, M., Jaoui, M., Kleindienst, T. E., Offenberg, J. H., and Edney,
E. O.: Composition of PM2.5 during the summer of 2003 in Research
Triangle Park, North Carolina, Atmos. Environ., 41, 4073–4083,
https://doi.org/10.1016/j.atmosenv.2007.01.012, 2007.
Li, W., Pak, C. Y., Wang, X., and Tse, Y.-L. S.: Uptake of common atmospheric
gases by organic-coated water droplets, J. Phys. Chem. C, 123, 18924–18931,
2019.
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.
Marsh, A., Miles, R. E. H., Rovelli, G., Cowling, A. G., Nandy, L., Dutcher, C. S., and Reid, J. P.: Influence of organic compound functionality on aerosol hygroscopicity: dicarboxylic acids, alkyl-substituents, sugars and amino acids, Atmos. Chem. Phys., 17, 5583–5599, https://doi.org/10.5194/acp-17-5583-2017, 2017.
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.
Mukundan, T. and Kishore, K.: Synthesis, characterization and reactivity of
polymeric peroxides, Prog. Poly. Sci., 15, 475–505,
https://doi.org/10.1016/0079-6700(90)90004-k, 1990.
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, 2017.
Nah, T., Chan, M., Leone, S. R., and Wilson, K. R.: Real time in situ
chemical characterization of submicrometer organic particles using direct
analysis in Real Time-Mass Spectrometry, Anal. Chem., 85, 2087–2095,
https://doi.org/10.1021/ac302560c, 2013.
Olson, N. E., Lei, Z., Craig, R. L., Zhang, Y., Chen, Y., Lambe, A. T.,
Zhang, Z., Gold, A., Surratt, J. D., and Ault, A. P.: Reactive Uptake of
Isoprene Epoxydiols Increases the Viscosity of the Core of Phase-Separated
Aerosol Particles, ACS Earth Space Chem., 3, 1402–1414,
https://doi.org/10.1021/acsearthspacechem.9b00138, 2019.
Peeters, J., Fantechi, G., and Vereecken, L.: A generalized
structure-activity relationship for the decomposition of (substituted)
alkoxy radicals, J. Atmos. Chem., 48, 59–80,
https://doi.org/10.1023/b:joch.0000034510.07694.ce, 2004.
Renbaum, L. H. and Smith G. D.: The importance of phase in the
radical-initiated oxidation of model organic aerosols: reactions of solid
and liquid brassidic acid particles, Phys. Chem. Chem. Phys., 11,
2441–2451, https://doi.org/10.1039/b816799k, 2009.
Riva, M., Chen, Y., Zhang, Y., Lei, Z., Olson, N. E., Boyer, H. C., Narayan,
S., Yee, L. D., Green, H. S., Cui, T., Zhang, Z., Baumann, K., Fort, M.,
Edgerton, E., Budisulistiorini, S. H., Rose, C. A., Ribeiro, I. O.,
Oliveira, R. L. E., Santos, E. O. D., Machado, C. M. D., Szopa, S., Zhao,
Y., Alves, E. G., Sá, S. S. D., Hu, W., Knipping, E. M., Shaw, S. L.,
Junior, S. D., Souza, R. A. F. D., Palm, B. B., Jimenez, J.-L., Glasius, M.,
Goldstein, A. H., Pye, H. O. T., Gold, A., Turpin, B. J., Vizuete, W.,
Martin, S. T., Thornton, J. A., Dutcher, C. S., Ault, A. P., and Surratt, J.
D.: Increasing Isoprene Epoxydiol-to-Inorganic Sulfate Aerosol Ratio Results
in Extensive Conversion of Inorganic Sulfate to Organosulfur Forms:
Implications for Aerosol Physicochemical Properties, Environ. Sci. Technol.,
53, 8682–8694, https://doi.org/10.1021/acs.est.9b01019, 2019.
Rudich, Y., Donahue, N. M., and Mentel, T. F.: Aging of organic aerosol:
bridging the gap between laboratory and field studies, Annu. Rev. Phys.
Chem., 58, 321–352, https://doi.org/10.1146/annurev.physchem.58.032806.104432, 2007.
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.
Schauer, J. J., Fraser, M. P., Cass, G. R., and Simoneit, B. R. T.: Source
reconciliation of atmospheric gas-phase and particle-phase pollutants during
a severe photochemical smog episode, Environ. Sci. Technol., 36, 3806–3814,
https://doi.org/10.1021/es011458j, 2002.
Shrivastava, M., Cappa, C. D., Fan, J., Goldstein, A. H., Guenther, A. B.,
Jimenez, J. L., Kuang, C., Laskin, A., Martin, S. T., Ng, N. L., Petaja, T.,
Pierce, J. R., Rasch, P. J., Roldin, P., Seinfeld, J. H., Shilling, J.,
Smith, J. N., Thornton, J. A., Volkamer, R., Wang, J., Worsnop, D. R.,
Zaveri, R. A., Zelenyuk, A., and Zhang, Q.: Recent advances in understanding
secondary organic aerosol: Implications for global climate forcing, Rev.
Geophys., 55, 509–559, https://doi.org/10.1002/2016rg000540, 2017.
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.
Socorro, J., Lakey, P. S. J., Han, L., Berkemeier, T., Lammel, G., Zetzsch,
C., Pöschl, U., and Shiraiwa, M.: Heterogeneous OH oxidation, shielding
effects and implications for the atmospheric fate of terbuthylazine and
other pesticides, Environ. Sci. Technol., 51, 13749–13754, 2017.
Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.:
Liquid-liquid phase separation in aerosol particles: Dependence on O:C,
organic functionalities, and compositional complexity, Geophys. Res. Lett.,
39, L19801, https://doi.org/10.1029/2012gl052807, 2012.
Song, Y. C., Haddrell, A. E., Bzdek, B. R., Reid, J. P., Bannan, T.,
Topping, D. O., Percival, C., and Cai, C.: Measurements and predictions of
binary component aerosol particle viscosity, J. Phys. Chem. A, 120,
8123–8137, https://doi.org/10.1021/acs.jpca.6b07835, 2016.
Stark, H., Yatavelli, R. L. N., Thompson, S. L., Kang, H., Krechmer, J. E.,
Kimmel, J. R., Palm, B. B., Hu, W. W., Hayes, P. L., Day, D. A.,
Campuzano-Jost, P., Canagaratna, M. R., Jayne, J. T., Worsnop, D. R., and
Jimenez, J. L.: Impact of Thermal Decomposition on Thermal Desorption
Instruments: Advantage of Thermogram Analysis for Quantifying Volatility
Distributions of Organic Species, Environ. Sci. Technol., 51, 8491–8500,
2017.
Veghte, D. P., Bittner, D. R., and Freedman, M. A.: Cryo-transmission
electron microscopy imaging of the morphology of submicrometer aerosol
containing organic acids and ammonium sulfate, Anal. Chem., 86, 2436–2442,
https://doi.org/10.1021/ac403279f, 2014.
Vereecken, L. and Peeters, J.: Decomposition of substituted alkoxy
radicals – part I: a generalized structure–activity relationship for
reaction barrier heights, Phys. Chem. Chem. Phys., 11, 9062,
https://doi.org/10.1039/b909712k, 2009.
Vieceli, J., Roeselova, M., Potter, N., Dang, L. X., Garrett, B. C., and Tobias,
D. J.: Molecular dynamics simulations of atmospheric oxidants at the
air-water interface: solvation and accommodation of OH and O3, J. Phys.
Chem. B, 109, 15876–15892, 2005.
Wennberg, P. O., Bates, K. H., Crounse, J. D., Dodson, L. G., Mcvay, R. C.,
Mertens, L. A., Nguyen, T. B., Praske, E., Schwantes, R. H., Smarte, M. D.,
Clair, J. M. S., Teng, A. P., Zhang, X., and Seinfeld, J. H.: Gas-phase
reactions of isoprene and its major oxidation products, Chem. Rev., 118,
3337–3390, https://doi.org/10.1021/acs.chemrev.7b00439, 2018.
Xia, X. and Hopke, P. K.: Seasonal variation of 2-methyltetrols in ambient
air samples, Environ. Sci. Technol., 40, 6934–6937, https://doi.org/10.1021/es060988i,
2006.
Xu, L., Guo, H., Boyd, C. M., Klein, M., Bougiatioti, A., Cerully, K. M.,
Hite, J. R., Isaacman-Vanwertz, G., Kreisberg, N. M., Knote, C., Olson, K.,
Koss, A., Goldstein, A. H., Hering, S. V., Gouw, J. D., Baumann, K., Lee,
S.-H., Nenes, A., Weber, R. J., and Ng, N. L.: Effects of anthropogenic
emissions on aerosol formation from isoprene and monoterpenes in the
southeastern United States, P. Natl. Acad. Sci. USA, 112, 37–42,
https://doi.org/10.1073/pnas.1417609112, 2014.
You, Y., Renbaum-Wolff, L., and Bertram, A. K.: Liquid–liquid phase separation in particles containing organics mixed with ammonium sulfate, ammonium bisulfate, ammonium nitrate or sodium chloride, Atmos. Chem. Phys., 13, 11723–11734, https://doi.org/10.5194/acp-13-11723-2013, 2013.
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, C. and Carloni, P.: Salt effects on water/hydrophobic liquid
interfaces: A molecular dynamics study, J. Phys.-Condens. Matter, 24,
124109, https://doi.org/10.1088/0953-8984/24/12/124109, 2012.
Zhang, H., Worton, D. R., Shen, S., Nah, T., Isaacman-Vanwertz, G., Wilson,
K. R., and Goldstein, A. H.: Fundamental time scales governing organic
aerosol multiphase partitioning and oxidative aging, Environ. Sci. Technol.,
49, 9768–9777, https://doi.org/10.1021/acs.est.5b02115, 2015.
Zhang, Z.-S., Engling, G., Chan, C.-Y., Yang, Y.-H., Lin, M., Shi, S., He,
J., Li, Y.-D., and Wang, X.-M.: Determination of isoprene-derived secondary
organic aerosol tracers (2-methyltetrols) by HPAEC-PAD: Results from
size-resolved aerosols in a tropical rainforest, Atmos. Environ., 70,
468–476, https://doi.org/10.1016/j.atmosenv.2013.01.020, 2013.
Zhang, Y., Chen, Y., Lei, Z., Olson, N. E., Riva, M., Koss, A. R., Zhang,
Z., Gold, A., Jayne, J. T., Worsnop, D. R., Onasch, T. B., Kroll, J. H.,
Turpin, B. J., Ault, A. P., and Surratt, J. D.: Joint Impacts of Acidity and
Viscosity on the Formation of Secondary Organic Aerosol from Isoprene
Epoxydiols (IEPOX) in Phase Separated Particles, ACS Earth Space Chem., 3,
2646–2658, https://doi.org/10.1021/acsearthspacechem.9b00209, 2019.
Zhao, Z., Xu, Q., Yang, X., and Zhang, H.: Heterogeneous ozonolysis of
endocyclic unsaturated organic aerosol proxies: implications for criegee
intermediate dynamics and later-generation reactions, ACS Earth Space Chem.,
3, 344–356, https://doi.org/10.1021/acsearthspacechem.8b00177, 2019.
Zuend, A., Marcolli, C., Luo, B. P., and Peter, T.: A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients, Atmos. Chem. Phys., 8, 4559–4593, https://doi.org/10.5194/acp-8-4559-2008, 2008.
Zuend, A., Marcolli, C., Booth, A. M., Lienhard, D. M., Soonsin, V., Krieger, U. K., Topping, D. O., McFiggans, G., Peter, T., and Seinfeld, J. H.: New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coefficients for organic-inorganic mixtures containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and aromatic functional groups, Atmos. Chem. Phys., 11, 9155–9206, https://doi.org/10.5194/acp-11-9155-2011, 2011.
Short summary
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.
Atmospheric particles, a complex mixture of inorganic salts, organic compounds and water, can...
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