Articles | Volume 22, issue 3
https://doi.org/10.5194/acp-22-1951-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-22-1951-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
11 Feb 2022
Research article |
| 11 Feb 2022
| 11 Feb 2022
Pyruvic acid, an efficient catalyst in SO3 hydrolysis and effective clustering agent in sulfuric-acid-based new particle formation
Narcisse Tsona Tchinda
Environment Research Institute, Shandong University, Qingdao, 266237, China
Environment Research Institute, Shandong University, Qingdao, 266237, China
Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081, China
Xiuhui Zhang
Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081, China
Related authors
Narcisse Tsona Tchinda, Xiaofan Lv, Stanley Numboniu Tasheh, Julius Numboniu Ghogomu, and Lin Du
EGUsphere, https://doi.org/10.5194/egusphere-2025-29, https://doi.org/10.5194/egusphere-2025-29, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This study examines the chemical transformation of selected organosulfates by reactions with HO• radicals both in the gas-phase and in the aqueous-phase. Results show that the nature of the substituents on the carbon chain can effectively alter the decomposition of organosulfates and ozone is highlighted as a key oxidant in the intermediate steps of this decomposition. The primary products from these reactions include inorganic sulfate and carbonyl compounds.
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Atmos. Chem. Phys., 24, 5847–5862, https://doi.org/10.5194/acp-24-5847-2024, https://doi.org/10.5194/acp-24-5847-2024, 2024
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Aromatic acids can be transferred from seawater to the atmosphere through bubble bursting. The air–sea transfer efficiency of aromatic acids was evaluated by simulating SSA generation with a plunging jet. As a whole, the transfer capacity of aromatic acids may depend on their functional groups and on the bridging effect of cations, as well as their concentration in seawater, as these factors influence the global emission flux of aromatic acids via SSA.
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EGUsphere, https://doi.org/10.5194/egusphere-2023-2960, https://doi.org/10.5194/egusphere-2023-2960, 2024
Preprint archived
Short summary
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In this study, the interactions between α-pinene and marine emission dimethyl sulfide (DMS) are investigated. It is found that the yield of secondary organic aerosol initially increases and then decreases with the increasing DMS/α-pinene ratio. This trend can be explained by OH regeneration, acid-catalyzed reactions, and the change in OH reactivity, etc. These findings can improve our understanding of atmospheric processes in coastal areas.
Lin Du, Xiaofan Lv, Makroni Lily, Kun Li, and Narcisse Tsona Tchinda
Atmos. Chem. Phys., 24, 1841–1853, https://doi.org/10.5194/acp-24-1841-2024, https://doi.org/10.5194/acp-24-1841-2024, 2024
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This study explores the pH effect on the reaction of dissolved SO2 with selected organic peroxides. Results show that the formation of organic and/or inorganic sulfate from these peroxides strongly depends on their electronic structures, and these processes are likely to alter the chemical composition of dissolved organic matter in different ways. The rate constants of these reactions exhibit positive pH and temperature dependencies within pH 1–10 and 240–340 K ranges.
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.
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Atmos. Chem. Phys., 23, 2235–2249, https://doi.org/10.5194/acp-23-2235-2023, https://doi.org/10.5194/acp-23-2235-2023, 2023
Short summary
Short summary
The promotion of soluble saccharides on sea spray aerosol (SSA) generation and the changes in particle morphology were observed. On the contrary, the coexistence of surface insoluble fatty acid film and soluble saccharides significantly inhibited the production of SSA. This is the first demonstration that hydrogen bonding mediated by surface-insoluble fatty acids contributes to saccharide transfer in seawater, providing a new mechanism for saccharide enrichment in SSA.
Zhaomin Yang, Kun Li, Narcisse T. Tsona, Xin Luo, and Lin Du
Atmos. Chem. Phys., 23, 417–430, https://doi.org/10.5194/acp-23-417-2023, https://doi.org/10.5194/acp-23-417-2023, 2023
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SO2 significantly promotes particle formation during cyclooctene ozonolysis. Carboxylic acids and their dimers were major products in particles formed in the absence of SO2. SO2 can induce production of organosulfates with stronger particle formation ability than their precursors, leading to the enhancement in particle formation. Formation mechanisms and structures of organosulfates were proposed, which is helpful for better understanding how SO2 perturbs the formation and fate of particles.
Zhaomin Yang, Li Xu, Narcisse T. Tsona, Jianlong Li, Xin Luo, and Lin Du
Atmos. Chem. Phys., 21, 7963–7981, https://doi.org/10.5194/acp-21-7963-2021, https://doi.org/10.5194/acp-21-7963-2021, 2021
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The promotion effects of SO2 and NH3 on particle and organosulfur compound formation from 1,2,4-trimethylbenzene (TMB) photooxidation were observed for the first time. The enhanced organosulfur compounds included hitherto unidentified aromatic sulfonates and organosulfates (OSs). OSs were produced via acid-driven heterogeneous chemistry of hydroperoxides. The production of organosulfur compounds might provide a new pathway for the fate of TMB in regions with considerable SO2 emissions.
Xiaotong Jiang, Narcisse T. Tsona, Long Jia, Shijie Liu, Hailiang Zhang, Yongfu Xu, and Lin Du
Atmos. Chem. Phys., 19, 13591–13609, https://doi.org/10.5194/acp-19-13591-2019, https://doi.org/10.5194/acp-19-13591-2019, 2019
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Atmospheric furan is a primary and secondary pollutant in the atmosphere, and its emission contributes to the formation of ultrafine particles and ground-level ozone. The present study demonstrates the effect of NOx and humidity on secondary organic aerosol (SOA) formation during the furan–NOx–NaCl photooxidation. Furthermore, the results illustrate the importance of studying SOA formation over a comprehensive range of environmental conditions.
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Atmos. Chem. Phys., 19, 649–661, https://doi.org/10.5194/acp-19-649-2019, https://doi.org/10.5194/acp-19-649-2019, 2019
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We used ab initio calculations to explore a new path for ion-induced SO2 oxidation by ozone in the gas phase. We find that, initiated by the superoxide ion, SO2 can readily oxidize to SO−3. The reaction is facilitated by the presence of water, being ~ 4 orders of magnitude faster than the reaction in the absence of water. Depending on the altitude and temperature, it is estimated that this reaction may contribute to 0.1–2.0 % of the total atmospheric sulfate.
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Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-477, https://doi.org/10.5194/acp-2018-477, 2018
Revised manuscript not accepted
Short summary
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The roles of NOx level and RH on the formation of SOA from the photooxidation of furan in the presence of NaCl seed particles were elucidated. The aerosol liquid water (ALW) effects on SOA mass concentration and yield were also evaluated. The chemical composition of furan SOA was investigated by ESI-Exactive-Orbitrap MS, with focus on the formation of organic nitrates. Strong evidences indicate that both the RH and different NOx levels have a significant effect on SOA formation.
Shijie Liu, Long Jia, Yongfu Xu, Narcisse T. Tsona, Shuangshuang Ge, and Lin Du
Atmos. Chem. Phys., 17, 13329–13343, https://doi.org/10.5194/acp-17-13329-2017, https://doi.org/10.5194/acp-17-13329-2017, 2017
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Secondary organic aerosol (SOA) formation from cyclohexene/NOx system with various SO2 concentrations under UV light was investigated to study the effects of cyclic alkenes on the atmospheric environment in polluted urban areas. The composition of organic compounds in SOA was measured using several complementary techniques. We present new evidence that organosulfates were produced from the photooxidation of cyclohexene in the presence of SO2.
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EGUsphere, https://doi.org/10.5194/egusphere-2025-29, https://doi.org/10.5194/egusphere-2025-29, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This study examines the chemical transformation of selected organosulfates by reactions with HO• radicals both in the gas-phase and in the aqueous-phase. Results show that the nature of the substituents on the carbon chain can effectively alter the decomposition of organosulfates and ozone is highlighted as a key oxidant in the intermediate steps of this decomposition. The primary products from these reactions include inorganic sulfate and carbonyl compounds.
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A comprehensive understanding of the optical properties of brown carbon (BrC) is essential to accurately assess its climatic effects. Based on multi-site spectroscopic measurements, this study demonstrated the significant spatial heterogeneity in the optical and structural properties of water-soluble BrC (WS-BrC) in different regions of China, and revealed factors affecting WS-BrC light absorption and the relationship between fluorophores and light absorption of WS-BrC.
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Atmos. Chem. Phys., 24, 5847–5862, https://doi.org/10.5194/acp-24-5847-2024, https://doi.org/10.5194/acp-24-5847-2024, 2024
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Aromatic acids can be transferred from seawater to the atmosphere through bubble bursting. The air–sea transfer efficiency of aromatic acids was evaluated by simulating SSA generation with a plunging jet. As a whole, the transfer capacity of aromatic acids may depend on their functional groups and on the bridging effect of cations, as well as their concentration in seawater, as these factors influence the global emission flux of aromatic acids via SSA.
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The nucleation of iodic acid (HIO3) and iodous acid (HIO2) was proven to be critical in marine areas. However, HIO3–HIO2 nucleation cannot effectively derive the rapid nucleation in some polluted coasts. We find a significant enhancement of dimethylamine (DMA) on the HIO3–HIO2 nucleation in marine and polar regions with abundant DMA sources, which may establish reasonable connections between the HIO3–HIO2 nucleation and the rapid formation of new particles in polluted marine and polar regions.
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Iodic acid (HIO3) nucleates with iodous acid (HIO2) efficiently in marine areas; however, whether methanesulfonic acid (MSA) can synergistically participate in the HIO3–HIO2-based nucleation is unclear. We provide molecular-level evidence that MSA can efficiently promote the formation of HIO3–HIO2-based clusters using a theoretical approach. The proposed MSA-enhanced iodine nucleation mechanism may help us to deeply understand marine new particle formation events with bursts of iodine particles.
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Preprint archived
Short summary
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In this study, the interactions between α-pinene and marine emission dimethyl sulfide (DMS) are investigated. It is found that the yield of secondary organic aerosol initially increases and then decreases with the increasing DMS/α-pinene ratio. This trend can be explained by OH regeneration, acid-catalyzed reactions, and the change in OH reactivity, etc. These findings can improve our understanding of atmospheric processes in coastal areas.
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Atmos. Chem. Phys., 24, 1841–1853, https://doi.org/10.5194/acp-24-1841-2024, https://doi.org/10.5194/acp-24-1841-2024, 2024
Short summary
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This study explores the pH effect on the reaction of dissolved SO2 with selected organic peroxides. Results show that the formation of organic and/or inorganic sulfate from these peroxides strongly depends on their electronic structures, and these processes are likely to alter the chemical composition of dissolved organic matter in different ways. The rate constants of these reactions exhibit positive pH and temperature dependencies within pH 1–10 and 240–340 K ranges.
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
Short summary
Short summary
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.
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Atmos. Chem. Phys., 23, 2235–2249, https://doi.org/10.5194/acp-23-2235-2023, https://doi.org/10.5194/acp-23-2235-2023, 2023
Short summary
Short summary
The promotion of soluble saccharides on sea spray aerosol (SSA) generation and the changes in particle morphology were observed. On the contrary, the coexistence of surface insoluble fatty acid film and soluble saccharides significantly inhibited the production of SSA. This is the first demonstration that hydrogen bonding mediated by surface-insoluble fatty acids contributes to saccharide transfer in seawater, providing a new mechanism for saccharide enrichment in SSA.
Zhaomin Yang, Kun Li, Narcisse T. Tsona, Xin Luo, and Lin Du
Atmos. Chem. Phys., 23, 417–430, https://doi.org/10.5194/acp-23-417-2023, https://doi.org/10.5194/acp-23-417-2023, 2023
Short summary
Short summary
SO2 significantly promotes particle formation during cyclooctene ozonolysis. Carboxylic acids and their dimers were major products in particles formed in the absence of SO2. SO2 can induce production of organosulfates with stronger particle formation ability than their precursors, leading to the enhancement in particle formation. Formation mechanisms and structures of organosulfates were proposed, which is helpful for better understanding how SO2 perturbs the formation and fate of particles.
Yangyang Liu, Yue Deng, Jiarong Liu, Xiaozhong Fang, Tao Wang, Kejian Li, Kedong Gong, Aziz U. Bacha, Iqra Nabi, Qiuyue Ge, Xiuhui Zhang, Christian George, and Liwu Zhang
Atmos. Chem. Phys., 22, 9175–9197, https://doi.org/10.5194/acp-22-9175-2022, https://doi.org/10.5194/acp-22-9175-2022, 2022
Short summary
Short summary
Both CO2 and carbonate salt work as the precursor of carbonate radicals, which largely promotes sulfate formation during the daytime. This study provides the first indication that the carbonate radical not only plays a role as an intermediate in tropospheric anion chemistry but also as a strong oxidant for the surface processing of trace gas in the atmosphere. CO2, carbponate radicals, and sulfate receive attention from those looking at the environment, atmosphere, aerosol, and photochemistry.
An Ning, Ling Liu, Lin Ji, and Xiuhui Zhang
Atmos. Chem. Phys., 22, 6103–6114, https://doi.org/10.5194/acp-22-6103-2022, https://doi.org/10.5194/acp-22-6103-2022, 2022
Short summary
Short summary
Iodic acid (IA) and methanesulfonic acid (MSA) were previously proved to be significant nucleation precursors in marine areas. However, the nucleation process involved in IA and MSA remains unclear. We show the enhancement of MSA on IA cluster formation and reveal the IAM-SA nucleating mechanism using a theoretical approach. This study helps to understand the clustering process in which marine sulfur- and iodine-containing species are jointly involved and its impact on new particle formation.
Zhaomin Yang, Li Xu, Narcisse T. Tsona, Jianlong Li, Xin Luo, and Lin Du
Atmos. Chem. Phys., 21, 7963–7981, https://doi.org/10.5194/acp-21-7963-2021, https://doi.org/10.5194/acp-21-7963-2021, 2021
Short summary
Short summary
The promotion effects of SO2 and NH3 on particle and organosulfur compound formation from 1,2,4-trimethylbenzene (TMB) photooxidation were observed for the first time. The enhanced organosulfur compounds included hitherto unidentified aromatic sulfonates and organosulfates (OSs). OSs were produced via acid-driven heterogeneous chemistry of hydroperoxides. The production of organosulfur compounds might provide a new pathway for the fate of TMB in regions with considerable SO2 emissions.
Ling Liu, Fangqun Yu, Kaipeng Tu, Zhi Yang, and Xiuhui Zhang
Atmos. Chem. Phys., 21, 6221–6230, https://doi.org/10.5194/acp-21-6221-2021, https://doi.org/10.5194/acp-21-6221-2021, 2021
Short summary
Short summary
Trifluoroacetic acid (TFA) was previously proved to participate in sulfuric acid (SA)–dimethylamine (DMA) nucleation in Shanghai, China. However, complex atmospheric environments can influence the nucleation of aerosol significantly. We show the influence of different atmospheric conditions on the SA-DMA-TFA nucleation and find the enhancement by TFA can be significant in cold and polluted areas, which provides the perspective of the realistic role of TFA in different atmospheric environments.
Qingcai Chen, Zhen Mu, Li Xu, Mamin Wang, Jin Wang, Ming Shan, Xudong Yang, Xingjun Fan, Jianzhong Song, Yuqin Wang, Pengchuan Lin, Lixin Zhang, Zhenxing Shen, and Lin Du
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-1032, https://doi.org/10.5194/acp-2019-1032, 2020
Preprint withdrawn
Short summary
Short summary
It is important to study the formation characteristics and mechanism of triplet state in aerosols to quantify the effect of chromophore substances on the global climate and atmospheric environmental quality. The result of this study reveals that chromophore substances contributes significantly to aerosol photochemistry and plays an important role in aerosol aging. The global models may need to include those potential effects in the future.
Xiaotong Jiang, Narcisse T. Tsona, Long Jia, Shijie Liu, Hailiang Zhang, Yongfu Xu, and Lin Du
Atmos. Chem. Phys., 19, 13591–13609, https://doi.org/10.5194/acp-19-13591-2019, https://doi.org/10.5194/acp-19-13591-2019, 2019
Short summary
Short summary
Atmospheric furan is a primary and secondary pollutant in the atmosphere, and its emission contributes to the formation of ultrafine particles and ground-level ozone. The present study demonstrates the effect of NOx and humidity on secondary organic aerosol (SOA) formation during the furan–NOx–NaCl photooxidation. Furthermore, the results illustrate the importance of studying SOA formation over a comprehensive range of environmental conditions.
Jun Zhang, Xinfeng Wang, Rui Li, Shuwei Dong, Yingnan Zhang, Penggang Zheng, Min Li, Tianshu Chen, Yuhong Liu, Likun Xue, Wei Nie, Aijun Ding, Mingjin Tang, Xuehua Zhou, Lin Du, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-757, https://doi.org/10.5194/acp-2019-757, 2019
Preprint withdrawn
Short summary
Short summary
This study presents the concentrations, variation characteristics, and key influencing factors of particulate organic nitrates at four urban and rural sites in eastern China. The effects of anthropogenic activities (i.e. biomass burning and coal combustion) and meteorological conditions (in particular the humidity) on the secondary formation of organic nitrates have been investigated. The results highlight the greater role of SO2 in organic nitrate chemistry than previously assumed.
Siyang Li, Xiaotong Jiang, Marie Roveretto, Christian George, Ling Liu, Wei Jiang, Qingzhu Zhang, Wenxing Wang, Maofa Ge, and Lin Du
Atmos. Chem. Phys., 19, 9887–9902, https://doi.org/10.5194/acp-19-9887-2019, https://doi.org/10.5194/acp-19-9887-2019, 2019
Short summary
Short summary
We stimulated the photochemical aging of organic film coated on aqueous aerosol in the presence of imidazole-2-carboxaldehyde, humic acid, an atmospheric PM2.5 sample, and a secondary organic aerosol sample from the lab. The unsaturated lipid mixed with photosensitizer under UV irradiation produced hydroperoxides, leading to surface area increase in organic film. Our results reveal the modification of organic film on aqueous aerosol has potential influence on the hygroscopic growth of droplets.
Narcisse Tchinda Tsona and Lin Du
Atmos. Chem. Phys., 19, 649–661, https://doi.org/10.5194/acp-19-649-2019, https://doi.org/10.5194/acp-19-649-2019, 2019
Short summary
Short summary
We used ab initio calculations to explore a new path for ion-induced SO2 oxidation by ozone in the gas phase. We find that, initiated by the superoxide ion, SO2 can readily oxidize to SO−3. The reaction is facilitated by the presence of water, being ~ 4 orders of magnitude faster than the reaction in the absence of water. Depending on the altitude and temperature, it is estimated that this reaction may contribute to 0.1–2.0 % of the total atmospheric sulfate.
Xiaotong Jiang, Narcisse T. Tsona, Long Jia, Shijie Liu, Yongfu Xu, and Lin Du
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-477, https://doi.org/10.5194/acp-2018-477, 2018
Revised manuscript not accepted
Short summary
Short summary
The roles of NOx level and RH on the formation of SOA from the photooxidation of furan in the presence of NaCl seed particles were elucidated. The aerosol liquid water (ALW) effects on SOA mass concentration and yield were also evaluated. The chemical composition of furan SOA was investigated by ESI-Exactive-Orbitrap MS, with focus on the formation of organic nitrates. Strong evidences indicate that both the RH and different NOx levels have a significant effect on SOA formation.
Shijie Liu, Long Jia, Yongfu Xu, Narcisse T. Tsona, Shuangshuang Ge, and Lin Du
Atmos. Chem. Phys., 17, 13329–13343, https://doi.org/10.5194/acp-17-13329-2017, https://doi.org/10.5194/acp-17-13329-2017, 2017
Short summary
Short summary
Secondary organic aerosol (SOA) formation from cyclohexene/NOx system with various SO2 concentrations under UV light was investigated to study the effects of cyclic alkenes on the atmospheric environment in polluted urban areas. The composition of organic compounds in SOA was measured using several complementary techniques. We present new evidence that organosulfates were produced from the photooxidation of cyclohexene in the presence of SO2.
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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The effect of different climate and air quality policies in China on in situ ozone production in Beijing
Assessing the relative impacts of satellite ozone and its precursor observations to improve global tropospheric ozone analysis using multiple chemical reanalysis systems
Evaluating present-day and future impacts of agricultural ammonia emissions on atmospheric chemistry and climate
Enhancing long-term trend simulation of the global tropospheric hydroxyl (TOH) and its drivers from 2005 to 2019: a synergistic integration of model simulations and satellite observations
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
Development of a detailed gaseous oxidation scheme of naphthalene for secondary organic aerosol (SOA) formation and speciation
Anthropogenic emission controls reduce summertime ozone-temperature sensitivity in the United States
Large contributions of soil emissions to the atmospheric nitrogen budget and their impacts on air quality and temperature rise in North China
Why did ozone concentrations remain high during Shanghai's static management? A statistical and radical-chemistry perspective
Revising VOC emissions speciation improves the simulation of global background ethane and propane
Hui Li, Jiaxin Qiu, and Bo Zheng
Atmos. Chem. Phys., 25, 1949–1963, https://doi.org/10.5194/acp-25-1949-2025, https://doi.org/10.5194/acp-25-1949-2025, 2025
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We conduct a sensitivity analysis with 31 tests on various factors including prior emissions, model resolution, satellite constraint, and other system configurations to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. This reveals the robustness of emissions estimated by this air-pollution-satellite-based CO2 emission inversion system, with relative change between tests and base inversion below 4.0 % for national annual NOx and CO2 emissions.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
Atmos. Chem. Phys., 25, 1749–1763, https://doi.org/10.5194/acp-25-1749-2025, https://doi.org/10.5194/acp-25-1749-2025, 2025
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The chemical reactions of ozone (O3) formation are related to meteorology and local emissions. Here, a random forest approach was used to eliminate the effects of meteorological factors (dispersion or transport) on O3 and its precursors. Variations in the sensitivity of O3 formation and the apportionment of emission sources were revealed after meteorological normalization. Our results suggest that meteorological variations should be considered when diagnosing O3 formation.
Jeongmin Yun, Junjie Liu, Brendan Byrne, Brad Weir, Lesley E. Ott, Kathryn McKain, Bianca C. Baier, Luciana V. Gatti, and Sebastien C. Biraud
Atmos. Chem. Phys., 25, 1725–1748, https://doi.org/10.5194/acp-25-1725-2025, https://doi.org/10.5194/acp-25-1725-2025, 2025
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This study quantifies errors in regional net surface–atmosphere CO2 flux estimates from an inverse model ensemble using airborne CO2 measurements. Our results show that flux error estimates based on observations significantly exceed those computed from the ensemble spread of flux estimates in regions with high fossil fuel emissions. This finding suggests the presence of systematic biases in the inversion estimates, associated with errors in the fossil fuel emissions common to all models.
Min Huang, Gregory R. Carmichael, Kevin W. Bowman, Isabelle De Smedt, Andreas Colliander, Michael H. Cosh, Sujay V. Kumar, Alex B. Guenther, Scott J. Janz, Ryan M. Stauffer, Anne M. Thompson, Niko M. Fedkin, Robert J. Swap, John D. Bolten, and Alicia T. Joseph
Atmos. Chem. Phys., 25, 1449–1476, https://doi.org/10.5194/acp-25-1449-2025, https://doi.org/10.5194/acp-25-1449-2025, 2025
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We use model simulations along with multiplatform, multidisciplinary observations and a range of analysis methods to estimate and understand the distributions, temporal changes, and impacts of reactive nitrogen and ozone over the most populous US region that has undergone significant environmental changes. Deposition, biogenic emissions, and extra-regional sources have been playing increasingly important roles in controlling pollutant budgets in this area as local anthropogenic emissions drop.
Xavier Faïn, Sophie Szopa, Vaishali Naïk, Patricia Martinerie, David M. Etheridge, Rachael H. Rhodes, Cathy M. Trudinger, Vasilii V. Petrenko, Kévin Fourteau, and Philip Place
Atmos. Chem. Phys., 25, 1105–1119, https://doi.org/10.5194/acp-25-1105-2025, https://doi.org/10.5194/acp-25-1105-2025, 2025
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Carbon monoxide (CO) plays a crucial role in the atmosphere's oxidizing capacity. In this study, we analyse how historical (1850–2014) [CO] outputs from state-of-the-art global chemistry–climate models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. A disparity in [CO] growth rates emerges in the Northern Hemisphere between models and observations from 1920–1975 CE, possibly linked to uncertainties in CO emission factors.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonné, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
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Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching −35°C are required to reproduce observed NOx.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
Atmos. Chem. Phys., 25, 1121–1143, https://doi.org/10.5194/acp-25-1121-2025, https://doi.org/10.5194/acp-25-1121-2025, 2025
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In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking, are increasingly important and impact air quality. This study uses a box model to evaluate how these emissions impact ozone in the Los Angeles Basin and quantifies the impact of gaseous cooking emissions. Accurate representation of these and other anthropogenic sources in inventories is crucial for informing effective air quality policies.
Xiaodan Ma, Jianping Huang, Michaela I. Hegglin, Patrick Jöckel, and Tianliang Zhao
Atmos. Chem. Phys., 25, 943–958, https://doi.org/10.5194/acp-25-943-2025, https://doi.org/10.5194/acp-25-943-2025, 2025
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Our research explored changes in ozone levels in the northwest Pacific region over 30 years, revealing a significant increase in the middle-to-upper troposphere, especially during spring and summer. This rise is influenced by both stratospheric and tropospheric sources, which affect climate and air quality in East Asia. This work underscores the need for continued study to understand underlying mechanisms.
Hiroo Hata, Norifumi Mizushima, and Tomohiko Ihara
Atmos. Chem. Phys., 25, 1037–1061, https://doi.org/10.5194/acp-25-1037-2025, https://doi.org/10.5194/acp-25-1037-2025, 2025
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The introduction of battery electric vehicles (BEVs) is expected to reduce the primary air pollutants from vehicular exhaust and evaporative emissions while reducing the anthropogenic heat produced by vehicles, ultimately mitigating the urban heat island (UHI) effect. This study revealed the impact of introducing BEVs on the decrease in the UHI effect and the impact of BEVs on the formation of tropospheric ozone and fine particulate matter in the Greater Tokyo Area of Japan.
Carlos Gómez-Ortiz, Guillaume Monteil, Sourish Basu, and Marko Scholze
Atmos. Chem. Phys., 25, 397–424, https://doi.org/10.5194/acp-25-397-2025, https://doi.org/10.5194/acp-25-397-2025, 2025
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In this paper, we test new implementations of our inverse modeling tool to estimate the weekly and regional CO2 emissions from fossil fuels in Europe. We use synthetic atmospheric observations of CO2 and radiocarbon (14CO2) to trace emissions to their sources, while separating the natural and fossil CO2. Our tool accurately estimates fossil CO2 emissions in densely monitored regions like western/central Europe. This approach aids in developing strategies for reducing CO2 emissions.
David D. Parrish, Ian C. Faloona, and Richard G. Derwent
Atmos. Chem. Phys., 25, 263–289, https://doi.org/10.5194/acp-25-263-2025, https://doi.org/10.5194/acp-25-263-2025, 2025
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Observation-based estimates of contributions to maximum ozone (O3) concentrations show that background O3 can exceed the air quality standard of 70 ppb in the southwestern US, precluding standard attainment. Over the past 4 decades, US anthropogenic O3 has decreased by a factor of ~ 6.3, while wildfire contributions have increased, so that the background now dominates maximum concentrations, even in Los Angeles, and the occurrence of maximum O3 has shifted from the eastern to the western US.
William P. L. Carter, Jia Jiang, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 25, 199–242, https://doi.org/10.5194/acp-25-199-2025, https://doi.org/10.5194/acp-25-199-2025, 2025
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This paper describes the scientific basis for gas-phase atmospheric chemical mechanisms derived using the SAPRC mechanism generation system, MechGen. It can derive mechanisms for most organic compounds with C, H, O, or N atoms, including initial reactions of organics with OH, O3, NO3, and O3P or by photolysis, as well as the reactions of the various types of intermediates that are formed. The paper includes a description of areas of uncertainty where additional research and updates are needed.
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
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Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Hassnae Erraji, Philipp Franke, Astrid Lampert, Tobias Schuldt, Ralf Tillmann, Andreas Wahner, and Anne Caroline Lange
Atmos. Chem. Phys., 24, 13913–13934, https://doi.org/10.5194/acp-24-13913-2024, https://doi.org/10.5194/acp-24-13913-2024, 2024
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Four-dimensional variational data assimilation allows for the simultaneous optimisation of initial values and emission rates by using trace-gas profiles from drone observations in a regional air quality model. Assimilated profiles positively impact the representation of air pollutants in the model by improving their vertical distribution and ground-level concentrations. This case study highlights the potential of drone data to enhance air quality analyses including local emission evaluation.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
Atmos. Chem. Phys., 24, 13693–13713, https://doi.org/10.5194/acp-24-13693-2024, https://doi.org/10.5194/acp-24-13693-2024, 2024
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This work uses chemical transport and box modeling to study the gas- and aqueous-phase production of organic acid concentrations measured in cloud water at the summit of Whiteface Mountain on 1 July 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas-phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
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Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
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Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 24, 12943–12962, https://doi.org/10.5194/acp-24-12943-2024, https://doi.org/10.5194/acp-24-12943-2024, 2024
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This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for representative winter and summer conditions. The study provides insights into further air quality control in China with reduced primary emissions.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Baoshuang Liu, Yao Gu, Yutong Wu, Qili Dai, Shaojie Song, Yinchang Feng, and Philip K. Hopke
Atmos. Chem. Phys., 24, 12861–12879, https://doi.org/10.5194/acp-24-12861-2024, https://doi.org/10.5194/acp-24-12861-2024, 2024
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Reactive loss of volatile organic compounds (VOCs) is a long-term issue yet to be resolved in VOC source analyses. We assess common methods of, and existing issues in, reducing losses, impacts of losses, and sources in current source analyses. We offer a potential supporting role for solving issues of VOC conversion. Source analyses of consumed VOCs that reacted to produce ozone and secondary organic aerosols can play an important role in the effective control of secondary pollution in air.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 2024
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to explain the weaker hourly variation in NO2 columns than at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
Atmos. Chem. Phys., 24, 12575–12593, https://doi.org/10.5194/acp-24-12575-2024, https://doi.org/10.5194/acp-24-12575-2024, 2024
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We incorporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratio predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understanding chemical transport models, with implications for better air quality management and environmental protection in the region.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
Atmos. Chem. Phys., 24, 12537–12555, https://doi.org/10.5194/acp-24-12537-2024, https://doi.org/10.5194/acp-24-12537-2024, 2024
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Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to understand ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the pattern of ozone in the tropics, except in southeast Asia, although it systematically overestimates it at all sites. This work highlights that UKESM1 can capture seasonal and hourly variability.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 24, 12495–12507, https://doi.org/10.5194/acp-24-12495-2024, https://doi.org/10.5194/acp-24-12495-2024, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation in this parameter for future modifications to models.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyoung Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
Atmos. Chem. Phys., 24, 12465–12493, https://doi.org/10.5194/acp-24-12465-2024, https://doi.org/10.5194/acp-24-12465-2024, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show that SF6 emissions are decreasing in the USA and in the EU, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, EU, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Yasin Elshorbany, Jerald R. Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo J. Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca R. Buchholz, Benjamin Gaubert, Néstor Y. Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
Atmos. Chem. Phys., 24, 12225–12257, https://doi.org/10.5194/acp-24-12225-2024, https://doi.org/10.5194/acp-24-12225-2024, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone and its precursors, nitrogen dioxide, formaldehyde, and total column CO, as well as ozonesonde data and model simulations.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
Atmos. Chem. Phys., 24, 12079–12106, https://doi.org/10.5194/acp-24-12079-2024, https://doi.org/10.5194/acp-24-12079-2024, 2024
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We quantified the contributions of land transport, shipping, and aviation emissions to tropospheric ozone; its radiative forcing; and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highlight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long lifetime.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Siting Li, Yiming Liu, Yuqi Zhu, Yinbao Jin, Yingying Hong, Ao Shen, Yifei Xu, Haofan Wang, Haichao Wang, Xiao Lu, Shaojia Fan, and Qi Fan
Atmos. Chem. Phys., 24, 11521–11544, https://doi.org/10.5194/acp-24-11521-2024, https://doi.org/10.5194/acp-24-11521-2024, 2024
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This study establishes an inventory of anthropogenic chlorine emissions in China in 2019 with expanded species (HCl, Cl-, Cl2, HOCl) and sources (41 specific sources). The inventory is validated by a modeling study against the observations. This study enhances the understanding of anthropogenic chlorine emissions in the atmosphere, identifies key sources, and provides scientific support for pollution control and climate change.
Willem E. van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
Atmos. Chem. Phys., 24, 11545–11563, https://doi.org/10.5194/acp-24-11545-2024, https://doi.org/10.5194/acp-24-11545-2024, 2024
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Methane in the atmosphere contributes to the production of ozone gas – an air pollutant and greenhouse gas. Our results highlight that simultaneous reductions in methane emissions help avoid offsetting the air pollution benefits already achieved by the already-approved precursor emission reductions by 2050 in the European Monitoring and Evaluation Programme region, while also playing an important role in bringing air pollution further down towards World Health Organization guideline limits.
Jinya Yang, Yutong Wang, Lei Zhang, and Yu Zhao
EGUsphere, https://doi.org/10.5194/egusphere-2024-2713, https://doi.org/10.5194/egusphere-2024-2713, 2024
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We develop a modeling framework to predict future ozone concentrations (till 2060s) in China following an IPCC scenario. We further evaluate and separate the contributions of climatic, anthropogenic, and biogenic factors by season and region. We find persistent emission controls will alter the nonlinear response of ozone to its precursors, and dominate the declining ozone level. The outcomes highlight the importance of human actions even with a climate penalty on air quality in the future.
Laura Stecher, Franziska Winterstein, Patrick Jöckel, Michael Ponater, Mariano Mertens, and Martin Dameris
EGUsphere, https://doi.org/10.5194/egusphere-2024-2938, https://doi.org/10.5194/egusphere-2024-2938, 2024
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Methane, the second most important anthropogenic greenhouse gas, is chemically decomposed in the atmosphere. The chemical sink of atmospheric methane is not constant, but depends on the temperature and on the abundance of its reaction partners. In this study, we use a global chemistry-climate model to assess the feedback of atmospheric methane induced by changes of the chemical sink in a warming climate, and its implications for the chemical composition and the surface air temperature change.
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
EGUsphere, https://doi.org/10.5194/egusphere-2024-2912, https://doi.org/10.5194/egusphere-2024-2912, 2024
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Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimise these natural emissions over Africa in 2019. Our approach led to an increase in natural emissions that is supported by independent data showing that current estimates are underestimated.
Tia R. Scarpelli, Paul I. Palmer, Mark Lunt, Ingrid Super, and Arjan Droste
Atmos. Chem. Phys., 24, 10773–10791, https://doi.org/10.5194/acp-24-10773-2024, https://doi.org/10.5194/acp-24-10773-2024, 2024
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Under the Paris Agreement, countries must track their anthropogenic greenhouse gas emissions. This study describes a method to determine self-consistent estimates for combustion emissions and natural fluxes of CO2 from atmospheric data. We report consistent estimates inferred using this approach from satellite data and ground-based data over Europe, suggesting that satellite data can be used to determine national anthropogenic CO2 emissions for countries where ground-based CO2 data are absent.
Yufen Wang, Ke Li, Xi Chen, Zhenjiang Yang, Minglong Tang, Pascoal M. D. Campos, Yang Yang, Xu Yue, and Hong Liao
EGUsphere, https://doi.org/10.5194/egusphere-2024-2576, https://doi.org/10.5194/egusphere-2024-2576, 2024
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The impact of biomass burning and anthropogenic emissions on high tropospheric ozone was not well studied in Southern Africa. We combined the model simulation with recent observations at the surface and from space to quantify tropospheric ozone and its main drivers in Southern Africa. Our work focuses on the impact of emissions from different sources at different spatial scales, contributing to a comprehensive understanding of air pollution drivers and their uncertainties in Southern Africa.
Wenbin Kou, Yang Gao, Dan Tong, Xiaojie Guo, Xiadong An, Wenyu Liu, Mengshi Cui, Xiuwen Guo, Shaoqing Zhang, Huiwang Gao, and Lixin Wu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2500, https://doi.org/10.5194/egusphere-2024-2500, 2024
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Unlike traditional numerical studies, we apply a high-resolution Earth system model, improving simulations of ozone and large-scale circulations such as atmospheric blocking. In addition to local heatwave effects, we quantify the impact of atmospheric blocking on downstream ozone concentrations, which is closely associated with the blocking position. We identify three major pathways of Rossby wave propagation, stressing the critical role of large-scale circulation play in regional air quality.
Qianqian Zhang, K. Folkert Boersma, Chiel van der Laan, Alba Mols, Bin Zhao, Shengyue Li, and Yuepeng Pan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2641, https://doi.org/10.5194/egusphere-2024-2641, 2024
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Accurate NOx emission estimates are required to better understand air pollution. This study investigates and demonstrates the ability of the superposition column model in combination with TROPOMI tropospheric NO2 column data to estimate city-scale NOx emissions and lifetimes and their variabilities. The results of this work nevertheless confirm the strength of the superposition column model in estimating urban NOx emissions with reasonable accuracy.
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Mingzhao Liu, Lars Hoffmann, Jens-Uwe Grooß, Zhongyin Cai, Sabine Grießbach, and Yi Heng
EGUsphere, https://doi.org/10.5194/egusphere-2024-2596, https://doi.org/10.5194/egusphere-2024-2596, 2024
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We studied the transport and chemical decomposition of volcanic SO2, focusing on the 2019 Raikoke event. By comparing two different chemistry modeling schemes, we found that including complex chemical reactions leads to a more accurate prediction of how long SO2 stays in the atmosphere. This research helps improve our understanding of volcanic pollution and its impact on air quality and climate, providing better tools for scientists to track and predict the movement of these pollutants.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
Atmos. Chem. Phys., 24, 9031–9044, https://doi.org/10.5194/acp-24-9031-2024, https://doi.org/10.5194/acp-24-9031-2024, 2024
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The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing was investigated. Emissions inventory data were used to estimate future pollutant mixing ratios relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes, but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emissions of organic pollutants.
Takashi Sekiya, Emanuele Emili, Kazuyuki Miyazaki, Antje Inness, Zhen Qu, R. Bradley Pierce, Dylan Jones, Helen Worden, William Y. Y. Cheng, Vincent Huijnen, and Gerbrand Koren
EGUsphere, https://doi.org/10.5194/egusphere-2024-2426, https://doi.org/10.5194/egusphere-2024-2426, 2024
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Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursors measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows for evaluating dependency of the impacts on different reanalysis systems. The results suggested the importance of satellite ozone and its precursor measurements for improving ozone analysis in the whole troposphere, with varying the magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
EGUsphere, https://doi.org/10.5194/egusphere-2024-2022, https://doi.org/10.5194/egusphere-2024-2022, 2024
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Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, significant changes in radiative forcing, and could significantly elevate N2O.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
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Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Victor Lannuque and Karine Sartelet
Atmos. Chem. Phys., 24, 8589–8606, https://doi.org/10.5194/acp-24-8589-2024, https://doi.org/10.5194/acp-24-8589-2024, 2024
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation and speciation from naphthalene oxidation. This study details the development of the first near-explicit chemical scheme for naphthalene oxidation by OH, which includes kinetic and mechanistic data, and is able to reproduce most of the experimentally identified products in both gas and particle phases.
Shuai Li, Xiao Lu, and Haolin Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1889, https://doi.org/10.5194/egusphere-2024-1889, 2024
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We report that the summertime ozone-temperature sensitivity decreased by 50 % from 3.0 ppbv/K in 1990 to 1.5 ppb/K in 2021 in the US. GEOS-Chem simulations show that anthropogenic NOx emission reduction is the dominant driver of the ozone-temperature sensitivity decline, through influencing both the temperature-direct and temperature-indirect processes. Reduced ozone-temperature sensitivity has decreased the ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
Atmos. Chem. Phys., 24, 8441–8455, https://doi.org/10.5194/acp-24-8441-2024, https://doi.org/10.5194/acp-24-8441-2024, 2024
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Using an updated soil reactive nitrogen emission scheme in the Unified Inputs for Weather Research and Forecasting coupled with Chemistry (UI-WRF-Chem) model, we investigate the role of soil NO and HONO (Nr) emissions in air quality and temperature in North China. Contributions of soil Nr emissions to O3 and secondary pollutants are revealed, exceeding effects of soil NOx or HONO emission. Soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
Jian Zhu, Shanshan Wang, Chuanqi Gu, Zhiwen Jiang, Sanbao Zhang, Ruibin Xue, Yuhao Yan, and Bin Zhou
Atmos. Chem. Phys., 24, 8383–8395, https://doi.org/10.5194/acp-24-8383-2024, https://doi.org/10.5194/acp-24-8383-2024, 2024
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In 2022, Shanghai implemented city-wide static management measures during the high-ozone season in April and May, providing a chance to study ozone pollution control. Despite significant emissions reductions, ozone levels increased by 23 %. Statistically, the number of days with higher ozone diurnal variation types increased during the lockdown period. The uneven decline in VOC and NO2 emissions led to heightened photochemical processes, resulting in the observed ozone level rise.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
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Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Cited articles
Almeida, J., Schobesberger, S., Kuerten, A., Ortega, I. K., Kupiainen-Maatta, O., Praplan, A. P., Adamov, A., Amorim, A., Bianchi, F., Breitenlechner, M., David, A., Dommen, J., Donahue, N. M., Downard, A., Dunne, E., Duplissy, J., Ehrhart, S., Flagan, R. C., Franchin, A., Guida, R., Hakala, J., Hansel, A., Heinritzi, M., Henschel, H., Jokinen, T., Junninen, H., Kajos, M., Kangasluoma, J., Keskinen, H., Kupc, A., Kurten, T., Kvashin, A. N., Laaksonen, A., Lehtipalo, K., Leiminger, M., Leppa, J., Loukonen, V., Makhmutov, V., Mathot, S., McGrath, M. J., Nieminen, T., Olenius, T., Onnela, A., Petaja, T., Riccobono, F., Riipinen, I., Rissanen, M., Rondo, L., Ruuskanen, T., Santos, F. D., Sarnela, N., Schallhart, S., Schnitzhofer, R., Seinfeld, J. H., Simon, M., Sipila, M., Stozhkov, Y., Stratmann, F., Tome, A., Troestl, J., Tsagkogeorgas, G., Vaattovaara, P., Viisanen, Y., Virtanen, A., Vrtala, A., Wagner, P. E., Weingartner, E., Wex, H., Williamson, C., Wimmer, D., Ye, P., Yli-Juuti, T., Carslaw, K. S., Kulmala, M., Curtius, J., Baltensperger, U., Worsnop, D. R., Vehkamaki, H., and Kirkby, J.:
Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere,
Nature,
502, 359–363, https://doi.org/10.1038/nature12663, 2013.
Andreae, M. O., Talbot, R. W., and Li, S.-M.:
Atmospheric measurements of pyruvic and formic acid,
J. Geophys. Res.-Atmos.,
92, 6635–6641, https://doi.org/10.1029/JD092iD06p06635, 1987.
Baboukas, E. D., Kanakidou, M., and Mihalopoulos, N.:
Carboxylic acids in gas and particulate phase above the Atlantic Ocean,
J. Geophys. Res.-Atmos.,
105, 14459–14471, https://doi.org/10.1029/1999JD900977, 2000.
Bardouki, H., Liakakou, H., Economou, C., Sciare, J., Smolík, J., Ždímal, V., Eleftheriadis, K., Lazaridis, M., Dye, C., and Mihalopoulos, N.:
Chemical composition of size-resolved atmospheric aerosols in the eastern Mediterranean during summer and winter,
Atmos. Environ.,
37, 195–208, https://doi.org/10.1016/S1352-2310(02)00859-2, 2003.
Bork, N., Kurtén, T., and Vehkamäki, H.: Exploring the atmospheric chemistry of
Bork, N., Elm, J., Olenius, T., and Vehkamäki, H.: Methane sulfonic acid-enhanced formation of molecular clusters of sulfuric acid and dimethyl amine, Atmos. Chem. Phys., 14, 12023–12030, https://doi.org/10.5194/acp-14-12023-2014, 2014.
Buszek, R. J., Barker, J. R., and Francisco, J. S.:
Water Effect on the OH plus HCl Reaction,
J. Phys. Chem. A,
116, 4712–4719, https://doi.org/10.1021/jp3025107, 2012.
Canneaux, S., Bohr, F., and Henon, E.:
KiSThelP: a program to predict thermodynamic properties and rate constants from quantum chemistry results,
J. Comput. Chem.,
35, 82–93, https://doi.org/10.1002/jcc.23470, 2014.
Chebbi, A. and Carlier, P.:
Carboxylic acids in the troposphere, occurrence, sources, and sinks: A review,
Atmos. Environ.,
30, 4233–4249, https://doi.org/10.1016/1352-2310(96)00102-1, 1996.
Church, J. R., Vaida, V., and Skodje, R. T.:
Gas-Phase Reaction Kinetics of Pyruvic Acid with OH Radicals: The Role of Tunneling, Complex Formation, and Conformational Structure,
J. Phys. Chem. A,
124, 790–800, https://doi.org/10.1021/acs.jpca.9b09638, 2020.
Daub, C. D., Riccardi, E., Hänninen, V., and Halonen, L.:
Path sampling for atmospheric reactions: formic acid catalysed conversion of SO3 + H2O to H2SO4,
PeerJ Physical Chemistry,
2, e7, https://doi.org/10.7717/peerj-pchem.7, 2020.
Duchovic, R. J., Pettigrew, J. D., Welling, B., and Shipchandler, T.:
Conventional transition state theory/Rice–Ramsperger–Kassel–Marcus theory calculations of thermal termolecular rate coefficients for H(D) + O2 + M,
J. Chem. Phys.,
105, 10367–10379, https://doi.org/10.1063/1.47299, 1996.
Eger, P. G., Schuladen, J., Sobanski, N., Fischer, H., Karu, E., Williams, J., Riva, M., Zha, Q., Ehn, M., Quéléver, L. L. J., Schallhart, S., Lelieveld, J., and Crowley, J. N.: Pyruvic acid in the boreal forest: gas-phase mixing ratios and impact on radical chemistry, Atmos. Chem. Phys., 20, 3697–3711, https://doi.org/10.5194/acp-20-3697-2020, 2020.
Eisenreich, W., Rohdich, F., and Bacher, A.:
Deoxyxylulose phosphate pathway to terpenoids,
Trends Plant Sci.,
6, 78–84, https://doi.org/10.1016/S1360-1385(00)01812-4, 2001.
Elm, J. and Mikkelsen, K. V.:
Computational approaches for efficiently modelling of small atmospheric clusters,
Chem. Phys. Lett.,
615, 26–29, https://doi.org/10.1016/j.cplett.2014.09.060, 2014.
Fukui, K.:
The path of chemical reactions-the IRC approach,
Accounts Chem. Res.,
14, 363–368, 1981.
Hazra, M. K. and Sinha, A.:
Formic acid catalyzed hydrolysis of SO3 in the gas phase: a barrierless mechanism for sulfuric acid production of potential atmospheric importance,
J. Am. Chem. Soc.,
133, 17444–17453, https://doi.org/10.1021/ja207393v, 2011.
Helas, G., Bingemer, H., and Andreae, M. O.:
Organic acids over equatorial Africa: Results from DECAFE 88,
J. Geophys. Res.-Atmos.,
97, 6187–6193, https://doi.org/10.1029/91JD01438, 1992.
Henschel, H., Navarro, J. C. A., Yli-Juuti, T., Kupiainen-Määttä, O., Olenius, T., Ortega, I. K., Clegg, S. L., Kurtén, T., Riipinen, I., and Vehkamäki, H.:
Hydration of Atmospherically Relevant Molecular Clusters: Computational Chemistry and Classical Thermodynamics,
J. Phys. Chem. A,
118, 2599–2611, https://doi.org/10.1021/jp500712y, 2014.
Hofmann, M. and Schleyer, P. v. R.:
Acid Rain: Ab Initio Investigation of the H2O.SO3 Complex and Its Conversion to H2SO4,
J. Am. Chem. Soc.,
116, 4947–4952, https://doi.org/10.1021/ja00090a045, 1994.
Hofmann-Sievert, R. and Castleman, A. W.:
Reaction of sulfur trioxide with water clusters and the formation of sulfuric acid,
J. Phys. Chem.,
88, 3329–3333, https://doi.org/10.1021/j150659a038, 1984.
Holland, P. M. and Castleman, A. W.:
Gas phase complexes: considerations of the stability of clusters in the sulfur trioxide-water system,
Chem. Phys. Lett.,
56, 511–514, https://doi.org/10.1016/0009-2614(78)89028-9, 1978.
Jardine, K. J., Sommer, E. D., Saleska, S. R., Huxman, T. E., Harley, P. C., and Abrell, L.:
Gas Phase Measurements of Pyruvic Acid and Its Volatile Metabolites,
Environ. Sci. Technol.,
44, 2454–2460, https://doi.org/10.1021/es903544p, 2010.
Jayne, J. T., Pöschl, U., Chen, Y.-m., Dai, D., Molina, L. T., Worsnop, D. R., Kolb, C. E., and Molina, M. J.:
Pressure and Temperature Dependence of the Gas-Phase Reaction of SO3 with H2O and the Heterogeneous Reaction of SO3 with H2O/H2SO4 Surfaces,
J. Phys. Chem. A,
101, 10000–10011, https://doi.org/10.1021/jp972549z, 1997.
Jenkin, M. E., Cox, R. A., Emrich, M., and Moortgat, G. K.:
Mechanisms of the Cl-atom-initiated oxidation of acetone and hydroxyacetone in air,
J. Chem. Soc. Faraday T.,
89, 2983–2991, https://doi.org/10.1039/FT9938902983, 1993.
Kawamura, K. and Bikkina, S.:
A review of dicarboxylic acids and related compounds in atmospheric aerosols: Molecular distributions, sources and transformation,
Atmos. Res.,
170, 140–160, https://doi.org/10.1016/j.atmosres.2015.11.018, 2016.
Kawamura, K., Kasukabe, H., and Barrie, L. A.:
Source and reaction pathways of dicarboxylic acids, ketoacids and dicarbonyls in arctic aerosols: One year of observations,
Atmos. Environ.,
30, 1709–1722, https://doi.org/10.1016/1352-2310(95)00395-9, 1996.
Kawamura, K., Tachibana, E., Okuzawa, K., Aggarwal, S. G., Kanaya, Y., and Wang, Z. F.: High abundances of water-soluble dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in the mountaintop aerosols over the North China Plain during wheat burning season, Atmos. Chem. Phys., 13, 8285–8302, https://doi.org/10.5194/acp-13-8285-2013, 2013.
Kuang, C., McMurry, P., McCormick, A., and Eisele, F.:
Dependence of nucleation rates on sulfuric acid vapor concentration in diverse atmospheric locations,
J. Geophys. Res.-Atmos.,
113, D10209, https://doi.org/10.1029/2007JD009253, 2008.
Kulmala, M.:
How particles nucleate and grow,
Science,
302, 1000–1001, 2003.
Kulmala, M., Pirjola, L., and Mäkelä, J. M.:
Stable sulphate clusters as a source of new atmospheric particles,
Nature,
404, 66–69, https://doi.org/10.1038/35003550, 2000.
Larson, L. J., Kuno, M., and Tao, F.-M.:
Hydrolysis of sulfur trioxide to form sulfuric acid in small water clusters,
J. Chem. Phys.,
112, 8830–8838, 2000.
Li, H., Zhong, J., Vehkamäki, H., Kurtén, T., Wang, W., Ge, M., Zhang, S., Li, Z., Zhang, X., Francisco, J. S., and Zeng, X. C.:
Self-Catalytic Reaction of SO3 and NH3 To Produce Sulfamic Acid and Its Implication to Atmospheric Particle Formation,
J. Am. Chem. Soc.,
140, 11020–11028, https://doi.org/10.1021/jacs.8b04928, 2018.
Liu, L., Zhong, J., Vehkamäki, H., Kurtén, T., Du, L., Zhang, X., Francisco, J. S., and Zeng, X. C.:
Unexpected quenching effect on new particle formation from the atmospheric reaction of methanol with SO3,
P. Natl. Acad. Sci. USA,
116, 24966, https://doi.org/10.1073/pnas.1915459116, 2019.
Liu, L., Yu, F., Tu, K., Yang, Z., and Zhang, X.: Influence of atmospheric conditions on the role of trifluoroacetic acid in atmospheric sulfuric acid–dimethylamine nucleation, Atmos. Chem. Phys., 21, 6221–6230, https://doi.org/10.5194/acp-21-6221-2021, 2021.
Loerting, T. and Liedl, K. R.:
Toward elimination of discrepancies between theory and experiment: The rate constant of the atmospheric conversion of SO3 to H2SO4,
P. Natl. Acad. Sci. USA,
97, 8874, https://doi.org/10.1073/pnas.97.16.8874, 2000.
Long, B., Chang, C.-R., Long, Z.-W., Wang, Y.-B., Tan, X.-F., and Zhang, W.-J.:
Nitric acid catalyzed hydrolysis of SO3 in the formation of sulfuric acid: A theoretical study,
Chem. Phys. Lett., 581, 26–29, https://doi.org/10.1016/j.cplett.2013.07.012, 2013.
Lu, Y., Liu, L., Ning, A., Yang, G., Liu, Y., Kurtén, T., Vehkamäki, H., Zhang, X., and Wang, L.:
Atmospheric Sulfuric Acid-Dimethylamine Nucleation Enhanced by Trifluoroacetic Acid,
Geophys. Res. Lett.,
47, e2019GL085627, https://doi.org/10.1029/2019GL085627, 2020.
Lv, G., Sun, X., Zhang, C., and Li, M.: Understanding the catalytic role of oxalic acid in SO3 hydration to form H2SO4 in the atmosphere, Atmos. Chem. Phys., 19, 2833–2844, https://doi.org/10.5194/acp-19-2833-2019, 2019.
Magel, E., Mayrhofer, S., Müller, A., Zimmer, I., Hampp, R., and Schnitzler, J. P.:
Photosynthesis and substrate supply for isoprene biosynthesis in poplar leaves,
Atmos. Environ.,
40, 138–151, https://doi.org/10.1016/j.atmosenv.2005.09.091, 2006.
Mattila, J. M., Brophy, P., Kirkland, J., Hall, S., Ullmann, K., Fischer, E. V., Brown, S., McDuffie, E., Tevlin, A., and Farmer, D. K.: Tropospheric sources and sinks of gas-phase acids in the Colorado Front Range, Atmos. Chem. Phys., 18, 12315–12327, https://doi.org/10.5194/acp-18-12315-2018, 2018.
Mauldin III, R., Berndt, T., Sipilä, M., Paasonen, P., Petäjä, T., Kim, S., Kurtén, T., Stratmann, F., Kerminen, V.-M., and Kulmala, M.:
A new atmospherically relevant oxidant of sulphur dioxide,
Nature,
488, 193–196, https://doi.org/10.1038/nature11278, 2012.
McGrath, M. J., Olenius, T., Ortega, I. K., Loukonen, V., Paasonen, P., Kurtén, T., Kulmala, M., and Vehkamäki, H.: Atmospheric Cluster Dynamics Code: a flexible method for solution of the birth-death equations, Atmos. Chem. Phys., 12, 2345–2355, https://doi.org/10.5194/acp-12-2345-2012, 2012.
Mellouki, A. and Mu, Y.:
On the atmospheric degradation of pyruvic acid in the gas phase,
J. Photoch. Photobio. A,
157, 295–300, https://doi.org/10.1016/S1010-6030(03)00070-4, 2003.
Morokuma, K. and Muguruma, C.:
Ab initio Molecular Orbital Study of the Mechanism of the Gas Phase Reaction SO3 + H2O: Importance of the Second Water Molecule,
J. Am. Chem. Soc.,
116, 10316–10317, https://doi.org/10.1021/ja00101a068, 1994.
Nair, A. A. and Yu, F.:
Quantification of Atmospheric Ammonia Concentrations: A Review of Its Measurement and Modeling,
Atmosphere,
11, 1092, https://doi.org/10.3390/atmos11101092, 2020.
Olenius, T., Kupiainen-Määttä, O., Ortega, I. K., Kurtén, T., and Vehkamäki, H.:
Free energy barrier in the growth of sulfuric acid–ammonia and sulfuric acid–dimethylamine clusters,
J. Chem. Phys.,
139, 084312, https://doi.org/10.1063/1.4819024, 2013a.
Olenius, T., Schobesberger, S., Kupiainen-Määttä, O., Franchin, A., Junninen, H., Ortega, I. K., Kurtén, T., Loukonen, V., Worsnop, D. R., Kulmala, M., and Vehkamäki, H.:
Comparing simulated and experimental molecular cluster distributions,
Faraday Discuss.,
165, 75–89, https://doi.org/10.1039/C3FD00031A, 2013b.
Ortega, I. K., Kupiainen, O., Kurtén, T., Olenius, T., Wilkman, O., McGrath, M. J., Loukonen, V., and Vehkamäki, H.: From quantum chemical formation free energies to evaporation rates, Atmos. Chem. Phys., 12, 225–235, https://doi.org/10.5194/acp-12-225-2012, 2012.
Paulot, F., Crounse, J. D., Kjaergaard, H. G., Kroll, J. H., Seinfeld, J. H., and Wennberg, P. O.: Isoprene photooxidation: new insights into the production of acids and organic nitrates, Atmos. Chem. Phys., 9, 1479–1501, https://doi.org/10.5194/acp-9-1479-2009, 2009.
Peng, C., Ayala, P. Y., Schlegel, H. B., and Frisch, M. J.:
Using redundant internal coordinates to optimize equilibrium geometries and transition states,
J. Comput. Chem.,
17, 49–56, https://doi.org/10.1002/(SICI)1096-987X(19960115)17:1<49::AID-JCC5>3.0.CO;2-0, 1996.
Praplan, A. P., Hegyi-Gaeggeler, K., Barmet, P., Pfaffenberger, L., Dommen, J., and Baltensperger, U.: Online measurements of water-soluble organic acids in the gas and aerosol phase from the photooxidation of 1,3,5-trimethylbenzene, Atmos. Chem. Phys., 14, 8665–8677, https://doi.org/10.5194/acp-14-8665-2014, 2014.
Reed Harris, A. E., Doussin, J.-F., Carpenter, B. K., and Vaida, V.:
Gas-Phase Photolysis of Pyruvic Acid: The Effect of Pressure on Reaction Rates and Products,
J. Phys. Chem. A,
120, 10123–10133, https://doi.org/10.1021/acs.jpca.6b09058, 2016.
Reed Harris, A. E., Cazaunau, M., Gratien, A., Pangui, E., Doussin, J.-F., and Vaida, V.:
Atmospheric Simulation Chamber Studies of the Gas-Phase Photolysis of Pyruvic Acid,
J. Phys. Chem. A,
121, 8348–8358, https://doi.org/10.1021/acs.jpca.7b05139, 2017a.
Reed Harris, A. E., Pajunoja, A., Cazaunau, M., Gratien, A., Pangui, E., Monod, A., Griffith, E. C., Virtanen, A., Doussin, J.-F., and Vaida, V.:
Multiphase Photochemistry of Pyruvic Acid under Atmospheric Conditions,
J. Phys. Chem. A,
121, 3327–3339, https://doi.org/10.1021/acs.jpca.7b01107, 2017b.
Riplinger, C. and Neese, F.:
An efficient and near linear scaling pair natural orbital based local coupled cluster method,
J. Chem. Phys.,
138, 034106, https://doi.org/10.1063/1.4773581, 2013.
Riplinger, C., Sandhoefer, B., Hansen, A., and Neese, F.:
Natural triple excitations in local coupled cluster calculations with pair natural orbitals,
J. Chem. Phys.,
139, 134101, https://doi.org/10.1063/1.4821834, 2013.
Shampine, L. F. and Reichelt, M. W.:
The MATLAB ODE Suite,
SIAM J. Sci. Comput.,
18, 1–22, https://doi.org/10.1137/S1064827594276424, 1997.
Sihto, S.-L., Kulmala, M., Kerminen, V.-M., Dal Maso, M., Petäjä, T., Riipinen, I., Korhonen, H., Arnold, F., Janson, R., Boy, M., Laaksonen, A., and Lehtinen, K. E. J.: Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms, Atmos. Chem. Phys., 6, 4079–4091, https://doi.org/10.5194/acp-6-4079-2006, 2006.
Sipila, M., Berndt, T., Petaja, T., Brus, D., Vanhanen, J., Stratmann, F., Patokoski, J., Mauldin III, R. L., Hyvarinen, A.-P., Lihavainen, H., and Kulmala, M.:
The Role of Sulfuric Acid in Atmospheric Nucleation,
Science,
327, 1243–1246, https://doi.org/10.1126/science.1180315, 2010.
Stocker, T. F, Qin, D., Plattner, G.-K., Tignor, M., Allen, S. K.,
Boschung, J., Nauels, A., Xia, Y., Bex, V., Midgley, P. M. (Eds.): IPCC, 2013: Climate Change 2013: The Physical Science Basis. Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 1585 pp., 2013.
Talbot, R. W., Andreae, M. O., Berresheim, H., Jacob, D. J., and Beecher, K. M.:
Sources and sinks of formic, acetic, and pyruvic acids over central Amazonia: 2. Wet season,
J. Geophys. Res.-Atmos.,
95, 16799–16811, https://doi.org/10.1029/JD095iD10p16799, 1990.
Talbot, R. W., Mosher, B. W., Heikes, B. G., Jacob, D. J., Munger, J. W., Daube, B. C., Keene, W. C., Maben, J. R., and Artz, R. S.:
Carboxylic acids in the rural continental atmosphere over the eastern United States during the Shenandoah Cloud and Photochemistry Experiment,
J. Geophys. Res.-Atmos.,
100, 9335–9343, https://doi.org/10.1029/95JD00507, 1995.
Temelso, B., Morrell, T. E., Shields, R. M., Allodi, M. A., Wood, E. K., Kirschner, K. N., Castonguay, T. C., Archer, K. A., and Shields, G. C.:
Quantum Mechanical Study of Sulfuric Acid Hydration: Atmospheric Implications,
J. Phys. Chem. A,
116, 2209–2224, https://doi.org/10.1021/jp2119026, 2012a.
Temelso, B., Phan, T. N., and Shields, G. C.:
Computational Study of the Hydration of Sulfuric Acid Dimers: Implications for Acid Dissociation and Aerosol Formation,
J. Phys. Chem. A,
116, 9745–9758, https://doi.org/10.1021/jp3054394, 2012b.
Torrent-Sucarrat, M., Francisco, J. S., and Anglada, J. M.:
Sulfuric acid as autocatalyst in the formation of sulfuric acid,
J. Am. Chem. Soc.,
134, 20632–20644, https://doi.org/10.1021/ja307523b, 2012.
Truhlar, D. G., Garrett, B. C., and Klippenstein, S. J.:
Current Status of Transition-State Theory,
J. Phys. Chem.,
100, 12771–12800, https://doi.org/10.1021/jp953748q, 1996.
Tsona, N. T. and Du, L.: A potential source of atmospheric sulfate from
Tsona, N. T., Bork, N., and Vehkamäki, H.: Exploring the chemical fate of the sulfate radical anion by reaction with sulfur dioxide in the gas phase, Atmos. Chem. Phys., 15, 495–503, https://doi.org/10.5194/acp-15-495-2015, 2015a.
Tsona, N. T., Henschel, H., Bork, N., Loukonen, V., and Vehkamäki, H.:
Structures, Hydration, and Electrical Mobilities of Bisulfate Ion–Sulfuric Acid–Ammonia/Dimethylamine Clusters: A Computational Study,
J. Phys. Chem. A,
119, 9670–9679, 2015b.
Tsona, N. T., Bork, N., Loukonen, V., and Vehkamäki, H.:
A Closure Study of the Reaction between Sulfur Dioxide and the Sulfate Radical Ion from First-Principles Molecular Dynamics Simulations,
J. Phys. Chem. A,
120, 1046–1050, 2016.
Warneck, P.:
Multi-Phase Chemistry of C2 and C3 Organic Compounds in the Marine Atmosphere, J. Atmos. Chem., 51, 119–159, https://doi.org/10.1007/s10874-005-5984-7, 2005.
Weber, R. J., Chen, G., Davis, D. D., Mauldin III, R. L., Tanner, D. J., Eisele, F. L., Clarke, A. D., Thornton, D. C., and Bandy, A. R.:
Measurements of enhanced H2SO4 and 3–4 nm particles near a frontal cloud during the First Aerosol Characterization Experiment (ACE 1),
J. Geophys. Res.-Atmos.,
106, 24107–24117, https://doi.org/10.1029/2000JD000109, 2001.
Welz, O., Savee, J. D., Osborn, D. L., Vasu, S. S., Percival, C. J., Shallcross, D. E., and Taatjes, C. A.:
Direct kinetic measurements of Criegee intermediate (CH2OO) formed by reaction of CH2I with O2,
Science,
335, 204–207, 2012.
Yao, X. and Zhang, L.:
Causes of Large Increases in Atmospheric Ammonia in the Last Decade across North America,
ACS Omega,
4, 22133–22142, https://doi.org/10.1021/acsomega.9b03284, 2019.
Zhang, Y., Liu, X., Fang, Y., Liu, D., Tang, A., and Collett, J. L.:
Atmospheric Ammonia in Beijing during the COVID-19 Outbreak: Concentrations, Sources, and Implications,
Environ. Sci. Tech. Let.,
8, 32–38, https://doi.org/10.1021/acs.estlett.0c00756, 2021.
Zhao, Y. and Truhlar, D. G.:
The M06 suite of density functionals for main group thermochemistry, thermochemical kinetics, noncovalent interactions, excited states, and transition elements: two new functionals and systematic testing of four M06-class functionals and 12 other functionals,
Theor. Chem. Acc.,
120, 215–241, https://doi.org/10.1007/s00214-007-0310-x, 2008.
Short summary
This study explores the effect of pyruvic acid (PA) both in the SO3 hydrolysis and in sulfuric-acid-based aerosol formation. Results show that in dry and polluted areas, PA-catalyzed SO3 hydrolysis is about 2 orders of magnitude more efficient at forming sulfuric acid than the water-catalyzed reaction. Moreover, PA can effectively enhance the ternary SA-PA-NH3 particle formation rate by up to 4.7×102 relative to the binary SA-NH3 particle formation rate at cold temperatures.
This study explores the effect of pyruvic acid (PA) both in the SO3 hydrolysis and in...
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