Articles | Volume 19, issue 5
https://doi.org/10.5194/acp-19-2833-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Special issue:
https://doi.org/10.5194/acp-19-2833-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
04 Mar 2019
Research article |
| 04 Mar 2019
| 04 Mar 2019
Understanding the catalytic role of oxalic acid in SO3 hydration to form H2SO4 in the atmosphere
Guochun Lv
Environment Research Institute, Shandong University, Jinan 250100, China
Xiaomin Sun
CORRESPONDING AUTHOR
Environment Research Institute, Shandong University, Jinan 250100, China
Chenxi Zhang
College of Biological and Environmental Engineering, Binzhou University, Binzhou 256600, China
Mei Li
CORRESPONDING AUTHOR
Institute of Mass Spectrometer and Atmospheric Environment, Jinan University, Guangzhou 510632, China
Guangdong Provincial Engineering Research Center for On-line Source Apportionment System Of Air Pollution, Guangzhou 510632, China
Related authors
No articles found.
Liangbin Wu, Cheng Wu, Tao Deng, Dui Wu, Mei Li, Yong Jie Li, and Zhen Zhou
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-245, https://doi.org/10.5194/amt-2023-245, 2023
Revised manuscript accepted for AMT
Short summary
Short summary
Field comparison of dual-spot (AE33) and single-spot (AE31) aethalometers by full-year collocated measurements suggests that site-specific correction factors are needed to ensure the data continuity of long-term measurements for AE31-to-AE33 transition in BC monitoring networks.
Liyuan Zhou, Zhancong Liang, Beatrix Rosette Go Mabato, Rosemarie Ann Infante Cuevas, Rongzhi Tang, Mei Li, Chunlei Cheng, and Chak K. Chan
Atmos. Chem. Phys., 23, 5251–5261, https://doi.org/10.5194/acp-23-5251-2023, https://doi.org/10.5194/acp-23-5251-2023, 2023
Short summary
Short summary
This study reveals the sulfate formation in photosensitized particles from biomass burning under UV and SO2, of which the relative atmospheric importance in sulfate production was qualitatively compared to nitrate photolysis. On the basis of single-particle aerosol mass spectrometry measurements, the number percentage of sulfate-containing particles and relative peak area of sulfate in single-particle spectra exhibited a descending order of 3,4-dimethoxybenzaldehyde > vanillin > syringaldehyde.
Zhancong Liang, Liyuan Zhou, Xinyue Li, Rosemarie Ann Infante Cuevas, Rongzhi Tang, Mei Li, Chunlei Cheng, Yangxi Chu, and Chak Keung Chan
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-838, https://doi.org/10.5194/acp-2022-838, 2022
Preprint withdrawn
Short summary
Short summary
Incense burning is a common religious ritual, especially in Asian and African communities, with massive particles emitted. While previous research mainly focused on the chemical compositions and potential health impacts of fresh incense particles, our work reveals that nitrate, accompanied by SOA, can rapidly form in incense-burning particles upon photochemical oxidation in the atmosphere. This finding could deepen our understanding of air pollution caused by religious activities.
Qi En Zhong, Chunlei Cheng, Zaihua Wang, Lei Li, Mei Li, Dafeng Ge, Lei Wang, Yuanyuan Li, Wei Nie, Xuguang Chi, Aijun Ding, Suxia Yang, Duohong Chen, and Zhen Zhou
Atmos. Chem. Phys., 21, 17953–17967, https://doi.org/10.5194/acp-21-17953-2021, https://doi.org/10.5194/acp-21-17953-2021, 2021
Short summary
Short summary
Particulate amines play important roles in new particle formation, aerosol acidity, and hygroscopicity. Most of the field observations did not distinguish the different behavior of each type amine under the same ambient influencing factors. In this study, two amine-containing single particles exhibited different mixing states and disparate enrichment of secondary organics, which provide insight into the discriminated fates of organics during the formation and evolution processes.
Shengqiang Zhu, Lei Li, Shurong Wang, Mei Li, Yaxi Liu, Xiaohui Lu, Hong Chen, Lin Wang, Jianmin Chen, Zhen Zhou, Xin Yang, and Xiaofei Wang
Atmos. Meas. Tech., 13, 4111–4121, https://doi.org/10.5194/amt-13-4111-2020, https://doi.org/10.5194/amt-13-4111-2020, 2020
Short summary
Short summary
Single-particle aerosol mass spectrometry (SPAMS) is widely used to detect chemical compositions and sizes of individual aerosol particles. However, it has a major issue: the mass accuracy of high-resolution SPAMS is relatively low. Here we developed an automatic linear calibration method to greatly improve the mass accuracy of SPAMS spectra so that the elemental compositions of organic peaks, such as Cx, CxHy, CxHyOz and CxHyNO peaks, can be directly identified just based on their m / z values.
Jia Yin Sun, Cheng Wu, Dui Wu, Chunlei Cheng, Mei Li, Lei Li, Tao Deng, Jian Zhen Yu, Yong Jie Li, Qianni Zhou, Yue Liang, Tianlin Sun, Lang Song, Peng Cheng, Wenda Yang, Chenglei Pei, Yanning Chen, Yanxiang Cen, Huiqing Nian, and Zhen Zhou
Atmos. Chem. Phys., 20, 2445–2470, https://doi.org/10.5194/acp-20-2445-2020, https://doi.org/10.5194/acp-20-2445-2020, 2020
Short summary
Short summary
Atmospheric aging processes (AAPs) can lead to black carbon (BC) light absorption enhancement (Eabs), which remained poorly characterized at a long timescale. By applying a newly developed approach, the minimum R squared method (MRS), this study investigated the temporal variations of BC Eabs at both seasonal and diel scales in an urban environment. Factors affecting the temporal variability of BC Eabs were also analyzed, including variability in emission sources and various types of AAPs.
Danhui Xu, Baozhu Ge, Xueshun Chen, Yele Sun, Nianliang Cheng, Mei Li, Xiaole Pan, Zhiqiang Ma, Yuepeng Pan, and Zifa Wang
Atmos. Chem. Phys., 19, 15569–15581, https://doi.org/10.5194/acp-19-15569-2019, https://doi.org/10.5194/acp-19-15569-2019, 2019
Short summary
Short summary
Wet deposition is one of the most important and efficient removal mechanisms in the evolution of the air pollution. Due to the lack of a localized parameterization scheme and some mechanisms being neglected in theoretical estimations and modeling calculations, below-cloud wet scavenging coefficients (BWSC) have large uncertainties. We compare the BWSCs under the same conditions to perform a multi-method evaluation in order to describe their characteristics.
Qinhao Lin, Yuxiang Yang, Yuzhen Fu, Guohua Zhang, Feng Jiang, Long Peng, Xiufeng Lian, Fengxian Liu, Xinhui Bi, Lei Li, Duohong Chen, Mei Li, Jie Ou, Mingjin Tang, Xinming Wang, Ping'an Peng, and Guoying Sheng
Atmos. Chem. Phys., 19, 10469–10479, https://doi.org/10.5194/acp-19-10469-2019, https://doi.org/10.5194/acp-19-10469-2019, 2019
Short summary
Short summary
The effects of the chemical composition and size of sea-salt-containing particles on their cloud condensation nuclei activity are incompletely understood. Our results showed that submicron sea-salt-containing particles can enrich in small cloud droplets, likely due to change in the chemical composition, while supermicron sea-salt-containing particles tended in the large cloud droplets less affected by chemical composition. This difference might further influence their atmospheric residence time.
Jun Tao, Zhisheng Zhang, Yunfei Wu, Leiming Zhang, Zhijun Wu, Peng Cheng, Mei Li, Laiguo Chen, Renjian Zhang, and Junji Cao
Atmos. Chem. Phys., 19, 8471–8490, https://doi.org/10.5194/acp-19-8471-2019, https://doi.org/10.5194/acp-19-8471-2019, 2019
Short summary
Short summary
Mass-scattering efficiencies (MSE) of dominant chemical species in atmospheric aerosols are important parameters for building the relationships between chemical species and the particle-scattering coefficient. Particle MSE mainly depends on the mass fractions of (NH4)2SO4, NH4NO3, and organic matter and their MSEs in the droplet mode. MSEs of (NH4)2SO4, NH4NO3 and organic matter were determined by their size distributions in the droplet mode.
Xinning Wang, Yin Shen, Yanfen Lin, Jun Pan, Yan Zhang, Peter K. K. Louie, Mei Li, and Qingyan Fu
Atmos. Chem. Phys., 19, 6315–6330, https://doi.org/10.5194/acp-19-6315-2019, https://doi.org/10.5194/acp-19-6315-2019, 2019
Short summary
Short summary
Shipping emissions were measured online at Shanghai Port, and their impacts on local air quality at the port and in the surrounding area were quantitatively assessed. Ship emission plumes were readily detectable before they dissipated. We captured ship emission plumes using synchronized peaks of SO2 and vanadium particles. By measuring the pollutant concentrations during plumes and their occurrence frequency, we made quantitative estimations of ship emission impacts on port air quality.
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
Short summary
Short summary
Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Qinhao Lin, Xinhui Bi, Guohua Zhang, Yuxiang Yang, Long Peng, Xiufeng Lian, Yuzhen Fu, Mei Li, Duohong Chen, Mark Miller, Ji Ou, Mingjin Tang, Xinming Wang, Ping'an Peng, Guoying Sheng, and Zhen Zhou
Atmos. Chem. Phys., 19, 1195–1206, https://doi.org/10.5194/acp-19-1195-2019, https://doi.org/10.5194/acp-19-1195-2019, 2019
Qian Xiao, Mei Li, Huan Liu, Mingliang Fu, Fanyuan Deng, Zhaofeng Lv, Hanyang Man, Xinxin Jin, Shuai Liu, and Kebin He
Atmos. Chem. Phys., 18, 9527–9545, https://doi.org/10.5194/acp-18-9527-2018, https://doi.org/10.5194/acp-18-9527-2018, 2018
Short summary
Short summary
This study emphasizes the importance of at-berth emissions to understanding the health impact of atmospheric pollutants. The chemical characteristics of both VOCs and PM from 20 container ship's at-berth exhaust emissions were examined using a gas chromatograph coupled to a mass spectrometer, and a single particle aerosol mass spectrometer. The profiles, based on massive samples from this study, complemented the insufficiency of relevant research in key port areas with high density populations.
Chunlei Cheng, Zuzhao Huang, Chak K. Chan, Yangxi Chu, Mei Li, Tao Zhang, Yubo Ou, Duohong Chen, Peng Cheng, Lei Li, Wei Gao, Zhengxu Huang, Bo Huang, Zhong Fu, and Zhen Zhou
Atmos. Chem. Phys., 18, 9147–9159, https://doi.org/10.5194/acp-18-9147-2018, https://doi.org/10.5194/acp-18-9147-2018, 2018
Short summary
Short summary
Particulate amines play an important role for the particle acidity and hygroscopicity. We found amines were internally mixed with sulfate and nitrate at a rural site in the PRD, China, suggesting the formation of aminium sulfate and nitrate salts. The ammonium-poor state of amine particles in summer was associated with the low emission sources of ammonia and a possible contribution of ammonium–amine exchange reactions. Amines could be a buffer for the particle acidity of ammonium-poor particles.
Guohua Zhang, Qinhao Lin, Long Peng, Xinhui Bi, Duohong Chen, Mei Li, Lei Li, Fred J. Brechtel, Jianxin Chen, Weijun Yan, Xinming Wang, Ping'an Peng, Guoying Sheng, and Zhen Zhou
Atmos. Chem. Phys., 17, 14975–14985, https://doi.org/10.5194/acp-17-14975-2017, https://doi.org/10.5194/acp-17-14975-2017, 2017
Short summary
Short summary
The mixing state of black carbon (BC)-containing particles and the mass scavenging efficiency of BC in cloud were investigated at a mountain site (1690 m a.s.l.) in southern China. The measured BC-containing particles were internally mixed extensively with sulfate, and thus the number fraction of scavenged BC-containing particles is close to that of all the measured particles. BC-containing particles with higher fractions of organics were scavenged relatively less.
Guohua Zhang, Qinhao Lin, Long Peng, Yuxiang Yang, Yuzhen Fu, Xinhui Bi, Mei Li, Duohong Chen, Jianxin Chen, Zhang Cai, Xinming Wang, Ping'an Peng, Guoying Sheng, and Zhen Zhou
Atmos. Chem. Phys., 17, 13891–13901, https://doi.org/10.5194/acp-17-13891-2017, https://doi.org/10.5194/acp-17-13891-2017, 2017
Short summary
Short summary
We first reported the size-resolved mixing state of oxalate in the cloud droplet residual, the cloud interstitial, and cloud-free particles by single particle mass spectrometry. Individual particle analysis provides unique insight into the formation and evolution of oxalate during in-cloud processing. The data show that in-cloud aqueous reactions dramatically improved the formation of oxalate from organic acids that were strongly associated with the aged biomass burning particles.
Chunlei Cheng, Mei Li, Chak K. Chan, Haijie Tong, Changhong Chen, Duohong Chen, Dui Wu, Lei Li, Cheng Wu, Peng Cheng, Wei Gao, Zhengxu Huang, Xue Li, Zhijuan Zhang, Zhong Fu, Yanru Bi, and Zhen Zhou
Atmos. Chem. Phys., 17, 9519–9533, https://doi.org/10.5194/acp-17-9519-2017, https://doi.org/10.5194/acp-17-9519-2017, 2017
Short summary
Short summary
Oxalic acid is an abundant and ubiquitous constituent in secondary organic aerosol (SOA) and can be an effective tracer for the oxidative processes leading to the formation of SOA. In this work photochemical reactions have a significant contribution to oxalic acid formation in summer, while in winter the formation of oxalic acid is closely associated with the oxidation of organic precursors in the aqueous phase.
Qinhao Lin, Guohua Zhang, Long Peng, Xinhui Bi, Xinming Wang, Fred J. Brechtel, Mei Li, Duohong Chen, Ping'an Peng, Guoying Sheng, and Zhen Zhou
Atmos. Chem. Phys., 17, 8473–8488, https://doi.org/10.5194/acp-17-8473-2017, https://doi.org/10.5194/acp-17-8473-2017, 2017
Short summary
Short summary
A ground-based counterflow virtual impactor coupled with a single-particle aerosol mass spectrometer (SPAMS) was used to assess the mixing state of individual cloud residue particles. Abundant aged EC cloud residues that internally mixed with inorganic salts were found in air masses from northerly polluted areas. K-rich cloud residues significantly increased within southwesterly air masses. This study increases our understanding of the impacts of aerosols on cloud droplets in southern China.
Yan Lyu, Tingting Xu, Xiang Li, Tiantao Cheng, Xin Yang, Xiaomin Sun, and Jianmin Chen
Atmos. Meas. Tech., 9, 1025–1037, https://doi.org/10.5194/amt-9-1025-2016, https://doi.org/10.5194/amt-9-1025-2016, 2016
Short summary
Short summary
This study presents the particle size distribution of PBDEs in the atmosphere of a megacity and evaluates the contribution of size-fractionated PBDEs' deposition in the human respiratory tract.
G. Zhang, X. Bi, L. Li, L. Y. Chan, M. Li, X. Wang, G. Sheng, J. Fu, and Z. Zhou
Atmos. Chem. Phys., 13, 4723–4735, https://doi.org/10.5194/acp-13-4723-2013, https://doi.org/10.5194/acp-13-4723-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Organosulfate produced from consumption of SO3 speeds up sulfuric acid–dimethylamine atmospheric nucleation
Contribution of expanded marine sulfur chemistry to the seasonal variability of dimethyl sulfide oxidation products and size-resolved sulfate aerosol
Spatial disparities of ozone pollution in the Sichuan Basin spurred by extreme, hot weather
Global impacts of aviation on air quality evaluated at high resolution
Bias correction of OMI HCHO columns based on FTIR and aircraft measurements and impact on top-down emission estimates
Investigation of the renewed methane growth post-2007 with high-resolution 3-D variational inverse modeling and isotopic constraints
Revisiting day-of-week ozone patterns in an era of evolving US air quality
Air quality and radiative impacts of downward-propagating sudden stratospheric warmings (SSWs)
Estimation of the atmospheric hydroxyl radical oxidative capacity using multiple hydrofluorocarbons (HFCs)
Investigating the differences in calculating global mean surface CO2 abundance: the impact of analysis methodologies and site selection
Meteorological characteristics of extreme ozone pollution events in China and their future predictions
Evaluating modelled tropospheric columns of CH4, CO, and O3 in the Arctic using ground-based Fourier transform infrared (FTIR) measurements
The high-resolution Global Aviation emissions Inventory based on ADS-B (GAIA) for 2019–2021
Zonal variability of methane trends derived from satellite data
Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021
Current status of model predictions of volatile organic compounds and impacts on surface ozone predictions during summer in China
Utility of Geostationary Lightning Mapper-derived lightning NO emission estimates in air quality modeling studies
The suitability of atmospheric oxygen measurements to constrain western European fossil-fuel CO2 emissions and their trends
Future tropospheric ozone budget and distribution over east Asia under a net-zero scenario
Comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA: implications for atmospheric oxidative capacity
MIXv2: a long-term mosaic emission inventory for Asia (2010–2017)
Insights into soil NO emissions and the contribution to surface ozone formation in China
Development, intercomparison, and evaluation of an improved mechanism for the oxidation of dimethyl sulfide in the UKCA model
A better representation of VOC chemistry in WRF-Chem and its impact on ozone over Los Angeles
The atmospheric oxidizing capacity in China – Part 1: Roles of different photochemical processes
Benefits of net-zero policies for future ozone pollution in China
Simulating impacts on UK air quality from net-zero forest planting scenarios
Understanding offshore high-ozone events during TRACER-AQ 2021 in Houston: insights from WRF–CAMx photochemical modeling
Opinion: Establishing a science-into-policy process for tropospheric ozone assessment
Atmospheric composition and climate impacts of a future hydrogen economy
Assessment of isoprene and near-surface ozone sensitivities to water stress over the Euro-Mediterranean region
Nighttime ozone in the lower boundary layer: insights from 3-year tower-based measurements in South China and regional air quality modeling
What controls ozone sensitivity in the upper tropical troposphere?
The CO anthropogenic emissions in Europe from 2011 to 2021: insights from the MOPITT satellite data
Summertime tropospheric ozone source apportionment study in Madrid (Spain)
Modelling the impacts of emission changes on O3 sensitivity, atmospheric oxidation capacity, and pollution transport over the Catalonia region
A regional modelling study of halogen chemistry within a volcanic plume of Mt Etna's Christmas 2018 eruption
Analysis of an intense O3 pollution episode in the Atlantic Coast of the Iberian Peninsula using photochemical modelling: characterization of transport pathways and accumulation processes
Constraining the budget of atmospheric carbonyl sulfide using a 3-D chemical transport model
Atmospheric CO2 inversion reveals the Amazon as a minor carbon source caused by fire emissions, with forest uptake offsetting about half of these emissions
Rapid O3 assimilations – Part 2: Tropospheric O3 changes accompanied by declining NOx emissions in the USA and Europe in 2005–2020
High-resolution air quality simulations of ozone exceedance events during the Lake Michigan Ozone Study
Simulations of winter ozone in the Upper Green River basin, Wyoming, using WRF-Chem
Measurement report: Assessment of Asian emissions of ethane and propane with a chemistry transport model based on observations from the island of Hateruma
Sensitivity of northeastern US surface ozone predictions to the representation of atmospheric chemistry in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMMv1.0)
Daytime isoprene nitrates under changing NOx and O3
Atmospheric data support a multi-decadal shift in the global methane budget towards natural tropical emissions
Air quality and related health impact in the UNECE region: source attribution and scenario analysis
East Asian methane emissions inferred from high-resolution inversions of GOSAT and TROPOMI observations: a comparative and evaluative analysis
Towards near-real-time air pollutant and greenhouse gas emissions: lessons learned from multiple estimates during the COVID-19 pandemic
Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin
Atmos. Chem. Phys., 24, 3593–3612, https://doi.org/10.5194/acp-24-3593-2024, https://doi.org/10.5194/acp-24-3593-2024, 2024
Short summary
Short summary
Atmospheric new particle formation (NPF) has a significant influence on the global climate, local air quality and human health. Using a combination of quantum chemical calculations and kinetics modeling, we find that thhe gas-phase organosulfate produced from consumption of SO3 can significantly enhance SA–DMA nucleation in the polluted boundary layer, resulting in non-negligible contributions to NPF. Our findings provide important insights into organic sulfur in atmospheric aerosol formation.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
Short summary
Short summary
Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Nan Wang, Yunsong Du, Dongyang Chen, Haiyan Meng, Xi Chen, Li Zhou, Guangming Shi, Yu Zhan, Miao Feng, Wei Li, Mulan Chen, Zhenliang Li, and Fumo Yang
Atmos. Chem. Phys., 24, 3029–3042, https://doi.org/10.5194/acp-24-3029-2024, https://doi.org/10.5194/acp-24-3029-2024, 2024
Short summary
Short summary
In the scorching August 2022 heatwave, China's Sichuan Basin saw a stark contrast in ozone (O3) levels between Chengdu and Chongqing. The regional disparities were studied considering meteorology, precursors, photochemistry, and transportation. The study highlighted the importance of tailored pollution control measures and underlined the necessity for region-specific strategies to combat O3 pollution on a regional scale.
Sebastian D. Eastham, Guillaume P. Chossière, Raymond L. Speth, Daniel J. Jacob, and Steven R. H. Barrett
Atmos. Chem. Phys., 24, 2687–2703, https://doi.org/10.5194/acp-24-2687-2024, https://doi.org/10.5194/acp-24-2687-2024, 2024
Short summary
Short summary
Emissions from aircraft are known to cause air quality impacts worldwide, but the scale and mechanisms of this impact are not well understood. This work uses high-resolution computational modeling of the atmosphere to show that air pollution changes from aviation are mostly the result of emissions during cruise (high-altitude) operations, that these impacts are related to how much non-aviation pollution is present, and that prior regional assessments have underestimated these impacts.
Jean-François Müller, Trissevgeni Stavrakou, Glenn-Michael Oomen, Beata Opacka, Isabelle De Smedt, Alex Guenther, Corinne Vigouroux, Bavo Langerock, Carlos Augusto Bauer Aquino, Michel Grutter, James Hannigan, Frank Hase, Rigel Kivi, Erik Lutsch, Emmanuel Mahieu, Maria Makarova, Jean-Marc Metzger, Isamu Morino, Isao Murata, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Amelie Röhling, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, and Alan Fried
Atmos. Chem. Phys., 24, 2207–2237, https://doi.org/10.5194/acp-24-2207-2024, https://doi.org/10.5194/acp-24-2207-2024, 2024
Short summary
Short summary
Formaldehyde observations from satellites can be used to constrain the emissions of volatile organic compounds, but those observations have biases. Using an atmospheric model, aircraft and ground-based remote sensing data, we quantify these biases, propose a correction to the data, and assess the consequence of this correction for the evaluation of emissions.
Joël Thanwerdas, Marielle Saunois, Antoine Berchet, Isabelle Pison, and Philippe Bousquet
Atmos. Chem. Phys., 24, 2129–2167, https://doi.org/10.5194/acp-24-2129-2024, https://doi.org/10.5194/acp-24-2129-2024, 2024
Short summary
Short summary
We investigate the causes of the renewed growth of atmospheric methane (CH4) after 2007 using inverse modeling. We use the additional information provided by observations of CH4 isotopic compositions to better differentiate between the emission categories. Accounting for the large uncertainties in source signatures, our results suggest that the post-2007 increase in atmospheric CH4 was caused by similar increases in emissions from (1) fossil fuels and (2) agriculture and waste.
Heather Simon, Christian Hogrefe, Andrew Whitehill, Kristen M. Foley, Jennifer Liljegren, Norm Possiel, Benjamin Wells, Barron H. Henderson, Lukas C. Valin, Gail Tonnesen, K. Wyat Appel, and Shannon Koplitz
Atmos. Chem. Phys., 24, 1855–1871, https://doi.org/10.5194/acp-24-1855-2024, https://doi.org/10.5194/acp-24-1855-2024, 2024
Short summary
Short summary
We assess observed and modeled ozone weekend–weekday differences in the USA from 2002–2019. A subset of urban areas that were NOx-saturated at the beginning of the period transitioned to NOx-limited conditions. Multiple rural areas of California were NOx-limited for the entire period but become less influenced by local day-of-week emission patterns in more recent years. The model produces more NOx-saturated conditions than the observations but captures trends in weekend–weekday ozone patterns.
Ryan S. Williams, Michaela I. Hegglin, Patrick Jöckel, Hella Garny, and Keith P. Shine
Atmos. Chem. Phys., 24, 1389–1413, https://doi.org/10.5194/acp-24-1389-2024, https://doi.org/10.5194/acp-24-1389-2024, 2024
Short summary
Short summary
During winter, a brief but abrupt reversal of the mean stratospheric westerly flow (~30 km high) around the Arctic occurs ~6 times a decade. Using a chemistry–climate model, about half of these events are shown to induce large anomalies in Arctic ozone (>25 %) and water vapour (>±25 %) around ~8–12 km altitude for up to 2–3 months, important for weather forecasting. We also calculate a doubling to trebling of the risk in breaches of mid-latitude surface air quality (ozone) standards (~60 ppbv).
Rona L. Thompson, Stephen A. Montzka, Martin K. Vollmer, Jgor Arduini, Molly Crotwell, Paul B. Krummel, Chris Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Stefan Reimann, Isaac Vimont, Hsiang Wang, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 24, 1415–1427, https://doi.org/10.5194/acp-24-1415-2024, https://doi.org/10.5194/acp-24-1415-2024, 2024
Short summary
Short summary
The hydroxyl radical determines the atmospheric lifetimes of numerous species including methane. Since OH is very short-lived, it is not possible to directly measure its concentration on scales relevant for understanding its effect on other species. Here, OH is inferred by looking at changes in hydrofluorocarbons (HFCs). We find that OH levels have been fairly stable over our study period (2004 to 2021), suggesting that OH is not the main driver of the recent increase in atmospheric methane.
Zhendong Wu, Alex Vermeulen, Yousuke Sawa, Ute Karstens, Wouter Peters, Remco de Kok, Xin Lan, Yasuyuki Nagai, Akinori Ogi, and Oksana Tarasova
Atmos. Chem. Phys., 24, 1249–1264, https://doi.org/10.5194/acp-24-1249-2024, https://doi.org/10.5194/acp-24-1249-2024, 2024
Short summary
Short summary
This study focuses on exploring the differences in calculating global surface CO2 and its growth rate, considering the impact of analysis methodologies and site selection. Our study reveals that the current global CO2 network has a good capacity to represent global surface CO2 and its growth rate, as well as trends in atmospheric CO2 mass changes. However, small differences exist in different analyses due to the impact of methodology and site selection.
Yang Yang, Yang Zhou, Hailong Wang, Mengyun Li, Huimin Li, Pinya Wang, Xu Yue, Ke Li, Jia Zhu, and Hong Liao
Atmos. Chem. Phys., 24, 1177–1191, https://doi.org/10.5194/acp-24-1177-2024, https://doi.org/10.5194/acp-24-1177-2024, 2024
Short summary
Short summary
This study reveals that extreme ozone pollution over the North China Plain and Yangtze River Delta is due to the chemical production related to hot and dry conditions, and the regional transport explains the ozone pollution over the Sichuan Basin and Pearl River Delta. The frequency of meteorological conditions of the extreme ozone pollution increases from the past to the future. The sustainable scenario is the optimal path to retaining clean air in China in the future.
Victoria A. Flood, Kimberly Strong, Cynthia H. Whaley, Kaley A. Walker, Thomas Blumenstock, James W. Hannigan, Johan Mellqvist, Justus Notholt, Mathias Palm, Amelie N. Röhling, Stephen Arnold, Stephen Beagley, Rong-You Chien, Jesper Christensen, Makoto Deushi, Srdjan Dobricic, Xinyi Dong, Joshua S. Fu, Michael Gauss, Wanmin Gong, Joakim Langner, Kathy S. Law, Louis Marelle, Tatsuo Onishi, Naga Oshima, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Manu A. Thomas, Svetlana Tsyro, and Steven Turnock
Atmos. Chem. Phys., 24, 1079–1118, https://doi.org/10.5194/acp-24-1079-2024, https://doi.org/10.5194/acp-24-1079-2024, 2024
Short summary
Short summary
It is important to understand the composition of the Arctic atmosphere and how it is changing. Atmospheric models provide simulations that can inform policy. This study examines simulations of CH4, CO, and O3 by 11 models. Model performance is assessed by comparing results matched in space and time to measurements from five high-latitude ground-based infrared spectrometers. This work finds that models generally underpredict the concentrations of these gases in the Arctic troposphere.
Roger Teoh, Zebediah Engberg, Marc Shapiro, Lynnette Dray, and Marc E. J. Stettler
Atmos. Chem. Phys., 24, 725–744, https://doi.org/10.5194/acp-24-725-2024, https://doi.org/10.5194/acp-24-725-2024, 2024
Short summary
Short summary
Emissions from aircraft contribute to climate change and degrade air quality. We describe an up-to-date 4D emissions inventory of global aviation from 2019 to 2021 based on actual flown trajectories. In 2019, 40.2 million flights collectively travelled 61 billion kilometres using 283 Tg of fuel. Long-haul flights were responsible for 43 % of CO2. The emissions inventory is made available for use in future studies to evaluate the negative externalities arising from global aviation.
Jonas Hachmeister, Oliver Schneising, Michael Buchwitz, John P. Burrows, Justus Notholt, and Matthias Buschmann
Atmos. Chem. Phys., 24, 577–595, https://doi.org/10.5194/acp-24-577-2024, https://doi.org/10.5194/acp-24-577-2024, 2024
Short summary
Short summary
We quantified changes in atmospheric methane concentrations using satellite data and a dynamic linear model approach. We calculated global annual methane increases for the years 2019–2022, which are in good agreement with other sources. For zonal methane growth rates, we identified strong inter-hemispheric differences in 2019 and 2022. For 2022, we could attribute decreases in the global growth rate to the Northern Hemisphere, possibly related to a reduction in anthropogenic emissions.
Glenn-Michael Oomen, Jean-François Müller, Trissevgeni Stavrakou, Isabelle De Smedt, Thomas Blumenstock, Rigel Kivi, Maria Makarova, Mathias Palm, Amelie Röhling, Yao Té, Corinne Vigouroux, Martina M. Friedrich, Udo Frieß, François Hendrick, Alexis Merlaud, Ankie Piters, Andreas Richter, Michel Van Roozendael, and Thomas Wagner
Atmos. Chem. Phys., 24, 449–474, https://doi.org/10.5194/acp-24-449-2024, https://doi.org/10.5194/acp-24-449-2024, 2024
Short summary
Short summary
Natural emissions from vegetation have a profound impact on air quality for their role in the formation of harmful tropospheric ozone and organic aerosols, yet these emissions are highly uncertain. In this study, we quantify emissions of organic gases over Europe using high-quality satellite measurements of formaldehyde. These satellite observations suggest that emissions from vegetation are much higher than predicted by models, especially in southern Europe.
Yongliang She, Jingyi Li, Xiaopu Lyu, Hai Guo, Momei Qin, Xiaodong Xie, Kangjia Gong, Fei Ye, Jianjiong Mao, Lin Huang, and Jianlin Hu
Atmos. Chem. Phys., 24, 219–233, https://doi.org/10.5194/acp-24-219-2024, https://doi.org/10.5194/acp-24-219-2024, 2024
Short summary
Short summary
In this study, we use multi-site volatile organic compound (VOC) measurements to evaluate the CMAQ-model-predicted VOCs and assess the impacts of VOC bias on O3 simulation. Our results demonstrate that current modeling setups and emission inventories are likely to underpredict VOC concentrations, and this underprediction of VOCs contributes to lower O3 predictions in China.
Peiyang Cheng, Arastoo Pour-Biazar, Yuling Wu, Shi Kuang, Richard T. McNider, and William J. Koshak
Atmos. Chem. Phys., 24, 41–63, https://doi.org/10.5194/acp-24-41-2024, https://doi.org/10.5194/acp-24-41-2024, 2024
Short summary
Short summary
Lightning-induced nitrogen monoxide (LNO) emission can be estimated from geostationary satellite observations. The present study uses the LNO emission estimates derived from geostationary satellite observations in an air quality modeling system to investigate the impact of LNO on air quality. Results indicate that significant ozone increase could be due to long-distance chemical transport, lightning activity in the upwind direction, and the mixing of high LNO (or ozone) plumes.
Christian Rödenbeck, Karina E. Adcock, Markus Eritt, Maksym Gachkivskyi, Christoph Gerbig, Samuel Hammer, Armin Jordan, Ralph F. Keeling, Ingeborg Levin, Fabian Maier, Andrew C. Manning, Heiko Moossen, Saqr Munassar, Penelope A. Pickers, Michael Rothe, Yasunori Tohjima, and Sönke Zaehle
Atmos. Chem. Phys., 23, 15767–15782, https://doi.org/10.5194/acp-23-15767-2023, https://doi.org/10.5194/acp-23-15767-2023, 2023
Short summary
Short summary
The carbon dioxide content of the Earth atmosphere is increasing due to human emissions from burning of fossil fuels, causing global climate change. The strength of the fossil-fuel emissions is estimated by inventories based on energy data, but independent validation of these inventories has been recommended by the Intergovernmental Panel on Climate Change. Here we investigate the potential to validate inventories based on measurements of small changes in the atmospheric oxygen content.
Xuewei Hou, Oliver Wild, Bin Zhu, and James Lee
Atmos. Chem. Phys., 23, 15395–15411, https://doi.org/10.5194/acp-23-15395-2023, https://doi.org/10.5194/acp-23-15395-2023, 2023
Short summary
Short summary
In response to the climate crisis, many countries have committed to net zero in a certain future year. The impacts of net-zero scenarios on tropospheric O3 are less well studied and remain unclear. In this study, we quantified the changes of tropospheric O3 budgets, spatiotemporal distributions of future surface O3 in east Asia and regional O3 source contributions for 2060 under a net-zero scenario using the NCAR Community Earth System Model (CESM) and online O3-tagging methods.
Meghna Soni, Rolf Sander, Lokesh K. Sahu, Domenico Taraborrelli, Pengfei Liu, Ankit Patel, Imran A. Girach, Andrea Pozzer, Sachin S. Gunthe, and Narendra Ojha
Atmos. Chem. Phys., 23, 15165–15180, https://doi.org/10.5194/acp-23-15165-2023, https://doi.org/10.5194/acp-23-15165-2023, 2023
Short summary
Short summary
The study presents the implementation of comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA. Simulations for contrasting urban environments of Asia and Europe highlight the significant impacts of chlorine on atmospheric oxidation capacity and composition. Chemical processes governing the production and loss of chlorine-containing species has been discussed. The updated chemical mechanism will be useful to interpret field measurements and for future air quality studies.
Meng Li, Junichi Kurokawa, Qiang Zhang, Jung-Hun Woo, Tazuko Morikawa, Satoru Chatani, Zifeng Lu, Yu Song, Guannan Geng, Hanwen Hu, Jinseok Kim, Owen R. Cooper, and Brian C. McDonald
EGUsphere, https://doi.org/10.5194/egusphere-2023-2283, https://doi.org/10.5194/egusphere-2023-2283, 2023
Short summary
Short summary
In this work, we developed MIXv2, an innovative Asian emission inventory for 2010–2017. With high spatial (0.1 degree) and monthly temporal resolution, MIXv2 integrates anthropogenic and open biomass burning emissions across seven sectors following a mosaic methodology. It provides CO2 emissions data alongside nine key pollutants and three chemical mechanisms. Our publicly accessible gridded monthly emissions data can facilitate long-term atmospheric and climate model analyses.
Ling Huang, Jiong Fang, Jiaqiang Liao, Greg Yarwood, Hui Chen, Yangjun Wang, and Li Li
Atmos. Chem. Phys., 23, 14919–14932, https://doi.org/10.5194/acp-23-14919-2023, https://doi.org/10.5194/acp-23-14919-2023, 2023
Short summary
Short summary
Surface ozone concentrations have emerged as a major environmental issue in China. Although control strategies aimed at reducing NOx emissions from conventional combustion sources are widely recognized, soil NOx emissions have received little attention. The impact of soil NO emissions on ground-level ozone concentration is yet to be evaluated. In this study, we estimated the soil NO emissions and evaluated its impact on ozone formation in China.
Ben A. Cala, Scott Archer-Nicholls, James Weber, N. Luke Abraham, Paul T. Griffiths, Lorrie Jacob, Y. Matthew Shin, Laura E. Revell, Matthew Woodhouse, and Alexander T. Archibald
Atmos. Chem. Phys., 23, 14735–14760, https://doi.org/10.5194/acp-23-14735-2023, https://doi.org/10.5194/acp-23-14735-2023, 2023
Short summary
Short summary
Dimethyl sulfide (DMS) is an important trace gas emitted from the ocean recognised as setting the sulfate aerosol background, but its oxidation is complex. As a result representation in chemistry-climate models is greatly simplified. We develop and compare a new mechanism to existing mechanisms via a series of global and box model experiments. Our studies show our updated DMS scheme is a significant improvement but significant variance exists between mechanisms.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, Andy Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
EGUsphere, https://doi.org/10.5194/egusphere-2023-2742, https://doi.org/10.5194/egusphere-2023-2742, 2023
Short summary
Short summary
Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represent VOCs chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from Volatile Chemical Products and other anthropogenic sources to total VOC reactivity and O3.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 23, 14127–14158, https://doi.org/10.5194/acp-23-14127-2023, https://doi.org/10.5194/acp-23-14127-2023, 2023
Short summary
Short summary
In this study, we used a regional chemical transport model to characterize the different parameters of atmospheric oxidative capacity in recent chemical environments in China. These parameters include the production and destruction rates of ozone and other oxidants, the ozone production efficiency, the OH reactivity, and the length of the reaction chain responsible for the formation of ozone and ROx. They are also affected by the aerosol burden in the atmosphere.
Zhenze Liu, Oliver Wild, Ruth M. Doherty, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 23, 13755–13768, https://doi.org/10.5194/acp-23-13755-2023, https://doi.org/10.5194/acp-23-13755-2023, 2023
Short summary
Short summary
We investigate the impact of net-zero policies on surface ozone pollution in China. A chemistry–climate model is used to simulate ozone changes driven by local and external emissions, methane, and warmer climates. A deep learning model is applied to generate more robust ozone projection, and we find that the benefits of net-zero policies may be overestimated with the chemistry–climate model. Nevertheless, it is clear that the policies can still substantially reduce ozone pollution in future.
Gemma Purser, Mathew R. Heal, Edward J. Carnell, Stephen Bathgate, Julia Drewer, James I. L. Morison, and Massimo Vieno
Atmos. Chem. Phys., 23, 13713–13733, https://doi.org/10.5194/acp-23-13713-2023, https://doi.org/10.5194/acp-23-13713-2023, 2023
Short summary
Short summary
Forest expansion is a ″net-zero“ pathway, but change in land cover alters air quality in many ways. This study combines tree planting suitability data with UK measured emissions of biogenic volatile organic compounds to simulate spatial and temporal changes in atmospheric composition for planting scenarios of four species. Decreases in fine particulate matter are relatively larger than increases in ozone, which may indicate a net benefit of tree planting on human health aspects of air quality.
Wei Li, Yuxuan Wang, Xueying Liu, Ehsan Soleimanian, Travis Griggs, James Flynn, and Paul Walter
Atmos. Chem. Phys., 23, 13685–13699, https://doi.org/10.5194/acp-23-13685-2023, https://doi.org/10.5194/acp-23-13685-2023, 2023
Short summary
Short summary
This study examined high offshore ozone events in Galveston Bay and the Gulf of Mexico, using boat data and WRF–CAMx modeling during the TRACER-AQ 2021 field campaign. On average, high ozone is caused by chemistry due to the regional transport of volatile organic compounds and downwind advection of NOx from the ship channel. Two case studies show advection of ozone can be another process leading to high ozone, and accurate wind prediction is crucial for air quality forecasting in coastal areas.
Richard G. Derwent, David D. Parrish, and Ian C. Faloona
Atmos. Chem. Phys., 23, 13613–13623, https://doi.org/10.5194/acp-23-13613-2023, https://doi.org/10.5194/acp-23-13613-2023, 2023
Short summary
Short summary
Elevated tropospheric ozone concentrations driven by anthropogenic precursor emissions are a world-wide health and environmental concern; however, this issue lacks a generally accepted understanding of the scientific issues. Here, we briefly outline the elements required to conduct an international assessment process to establish a conceptual model of the underpinning science and motivate international policy forums for regulating ozone production over hemispheric and global scales.
Nicola J. Warwick, Alex T. Archibald, Paul T. Griffiths, James Keeble, Fiona M. O'Connor, John A. Pyle, and Keith P. Shine
Atmos. Chem. Phys., 23, 13451–13467, https://doi.org/10.5194/acp-23-13451-2023, https://doi.org/10.5194/acp-23-13451-2023, 2023
Short summary
Short summary
A chemistry–climate model has been used to explore the atmospheric response to changes in emissions of hydrogen and other species associated with a shift from fossil fuel to hydrogen use. Leakage of hydrogen results in indirect global warming, offsetting greenhouse gas emission reductions from reduced fossil fuel use. To maximise the benefit of hydrogen as an energy source, hydrogen leakage and emissions of methane, carbon monoxide and nitrogen oxides should be minimised.
Susanna Strada, Andrea Pozzer, Graziano Giuliani, Erika Coppola, Fabien Solmon, Xiaoyan Jiang, Alex Guenther, Efstratios Bourtsoukidis, Dominique Serça, Jonathan Williams, and Filippo Giorgi
Atmos. Chem. Phys., 23, 13301–13327, https://doi.org/10.5194/acp-23-13301-2023, https://doi.org/10.5194/acp-23-13301-2023, 2023
Short summary
Short summary
Water deficit modifies emissions of isoprene, an aromatic compound released by plants that influences the production of an air pollutant such as ozone. Numerical modelling shows that, during the warmest and driest summers, isoprene decreases between −20 and −60 % over the Euro-Mediterranean region, while near-surface ozone only diminishes by a few percent. Decreases in isoprene emissions not only happen under dry conditions, but also could occur after prolonged or repeated water deficits.
Guowen He, Cheng He, Haofan Wang, Xiao Lu, Chenglei Pei, Xiaonuan Qiu, Chenxi Liu, Yiming Wang, Nanxi Liu, Jinpu Zhang, Lei Lei, Yiming Liu, Haichao Wang, Tao Deng, Qi Fan, and Shaojia Fan
Atmos. Chem. Phys., 23, 13107–13124, https://doi.org/10.5194/acp-23-13107-2023, https://doi.org/10.5194/acp-23-13107-2023, 2023
Short summary
Short summary
We analyze nighttime ozone in the lower boundary layer (up to 500 m) from the 2017–2019 measurements at the Canton Tower and the WRF-CMAQ model. We identify a strong ability of the residual layer to store daytime ozone in the convective mixing layer, investigate the chemical and meteorological factors controlling nighttime ozone in the residual layer, and quantify the contribution of nighttime ozone in the residual layer to both the nighttime and the following day’s surface ozone air quality.
Clara M. Nussbaumer, Horst Fischer, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 23, 12651–12669, https://doi.org/10.5194/acp-23-12651-2023, https://doi.org/10.5194/acp-23-12651-2023, 2023
Short summary
Short summary
Ozone is a greenhouse gas and contributes to the earth’s radiative energy budget and therefore to global warming. This effect is the largest in the upper troposphere. In this study, we investigate the processes controlling ozone formation and the sensitivity to its precursors in the upper tropical troposphere based on model simulations by the ECHAM5/MESSy2 Atmospheric Chemistry (EMAC) model. We find that NO𝑥 emissions from lightning most importantly affect ozone chemistry at these altitudes.
Audrey Fortems-Cheiney, Gregoire Broquet, Elise Potier, Robin Plauchu, Antoine Berchet, Isabelle Pison, Hugo A. C. Denier van der Gon, and Stijn N. C. Dellaert
EGUsphere, https://doi.org/10.5194/egusphere-2023-1981, https://doi.org/10.5194/egusphere-2023-1981, 2023
Short summary
Short summary
We have estimated the carbon monixide (CO) European emissions from satellite observations of the MOPITT instrument , at the relatively high resolution of 0.5°, for a period of over 10 years from 2011 to 2021. The analysis of the inversion results reveals the challenges associated with the inversion of CO emissions at the regional scale over Europe.
David de la Paz, Rafael Borge, Juan Manuel de Andrés, Luis Miguel Tovar, Golam Sarwar, and Sergey L. Napelenok
EGUsphere, https://doi.org/10.5194/egusphere-2023-2056, https://doi.org/10.5194/egusphere-2023-2056, 2023
Short summary
Short summary
This modelling study shows that around 70 % of ground-level ozone (O3) in Madrid (Spain) is transported from other regions. Nonetheless, local sources, mainly road traffic, play a significant role, specially under stagnation conditions associated to regional air recirculation. Our results suggest that local measures may be effective to reduce O3 peaks (potentially, up to 30 %) and thus, reduce impacts from high-O3 episodes in the Madrid metropolitan area.
Alba Badia, Veronica Vidal, Sergi Ventura, Roger Curcoll, Ricard Segura, and Gara Villalba
Atmos. Chem. Phys., 23, 10751–10774, https://doi.org/10.5194/acp-23-10751-2023, https://doi.org/10.5194/acp-23-10751-2023, 2023
Short summary
Short summary
Improving air quality is a top priority in urban areas. In this study, we used an air quality model to analyse the air quality changes occurring over the metropolitan area of Barcelona and other rural areas affected by transport of the atmospheric plume from the city during mobility restrictions. Our results show that mitigation strategies intended to reduce O3 should be designed according to the local meteorology, air transport, and particular ozone chemistry of the urban area.
Herizo Narivelo, Paul David Hamer, Virginie Marécal, Luke Surl, Tjarda Roberts, Sophie Pelletier, Béatrice Josse, Jonathan Guth, Mickaël Bacles, Simon Warnach, Thomas Wagner, Stefano Corradini, Giuseppe Salerno, and Lorenzo Guerrieri
Atmos. Chem. Phys., 23, 10533–10561, https://doi.org/10.5194/acp-23-10533-2023, https://doi.org/10.5194/acp-23-10533-2023, 2023
Short summary
Short summary
Volcanic emissions emit large quantities of gases and primary aerosols that can play an important role in atmospheric chemistry. We present a study of the fate of volcanic bromine emissions from the eruption of Mount Etna around Christmas 2018. Using a numerical model and satellite observations, we analyse the impact of the volcanic plume and how it modifies the composition of the air over the whole Mediterranean basin, in particular on tropospheric ozone through the bromine-explosion cycle.
Eduardo Torre-Pascual, Gotzon Gangoiti, Ana Rodríguez-García, Estíbaliz Sáez de Cámara, Joana Ferreira, Carla Gama, María Carmen Gómez, Iñaki Zuazo, Jose Antonio García, and Maite de Blas
EGUsphere, https://doi.org/10.5194/egusphere-2023-387, https://doi.org/10.5194/egusphere-2023-387, 2023
Short summary
Short summary
We present an analysis of an intense air pollution episode of tropospheric ozone over the Atlantic coast of the Iberian Peninsula, with measured and simulated parameters. Our analysis based not only on surface parameters but also on altitude parameters shows that the described episode may occur due to the accumulation of O3 in the upper layers of the atmosphere during previous days. That air mass will be transported to surface layers producing a sharp increase in O3 concentrations.
Michael P. Cartwright, Richard J. Pope, Jeremy J. Harrison, Martyn P. Chipperfield, Chris Wilson, Wuhu Feng, David P. Moore, and Parvadha Suntharalingam
Atmos. Chem. Phys., 23, 10035–10056, https://doi.org/10.5194/acp-23-10035-2023, https://doi.org/10.5194/acp-23-10035-2023, 2023
Short summary
Short summary
A 3-D chemical transport model, TOMCAT, is used to simulate global atmospheric carbonyl sulfide (OCS) distribution. Modelled OCS compares well with satellite observations of OCS from limb-sounding satellite observations. Model simulations also compare adequately with surface and atmospheric observations and suitably capture the seasonality of OCS and background concentrations.
Luana S. Basso, Chris Wilson, Martyn P. Chipperfield, Graciela Tejada, Henrique L. G. Cassol, Egídio Arai, Mathew Williams, T. Luke Smallman, Wouter Peters, Stijn Naus, John B. Miller, and Manuel Gloor
Atmos. Chem. Phys., 23, 9685–9723, https://doi.org/10.5194/acp-23-9685-2023, https://doi.org/10.5194/acp-23-9685-2023, 2023
Short summary
Short summary
The Amazon’s carbon balance may have changed due to forest degradation, deforestation and warmer climate. We used an atmospheric model and atmospheric CO2 observations to quantify Amazonian carbon emissions (2010–2018). The region was a small carbon source to the atmosphere, mostly due to fire emissions. Forest uptake compensated for ~ 50 % of the fire emissions, meaning that the remaining forest is still a small carbon sink. We found no clear evidence of weakening carbon uptake over the period.
Rui Zhu, Zhaojun Tang, Xiaokang Chen, Xiong Liu, and Zhe Jiang
Atmos. Chem. Phys., 23, 9745–9763, https://doi.org/10.5194/acp-23-9745-2023, https://doi.org/10.5194/acp-23-9745-2023, 2023
Short summary
Short summary
Ozone Monitoring Instrument (OMI) and surface O3 observations are used to investigate the changes in tropospheric O3 in the USA and Europe in 2005–2020. The surface-based assimilations show limited changes in surface and tropospheric column O3. The OMI-based assimilations show larger decreases in tropospheric O3 columns in 2010–2014, related to a decline in free-tropospheric NO2. Analysis suggests limited impacts of local emissions decline on tropospheric O3 over the USA and Europe in 2005–2020.
R. Bradley Pierce, Monica Harkey, Allen Lenzen, Lee M. Cronce, Jason A. Otkin, Jonathan L. Case, David S. Henderson, Zac Adelman, Tsengel Nergui, and Christopher R. Hain
Atmos. Chem. Phys., 23, 9613–9635, https://doi.org/10.5194/acp-23-9613-2023, https://doi.org/10.5194/acp-23-9613-2023, 2023
Short summary
Short summary
We evaluate two high-resolution model simulations with different meteorological inputs but identical chemistry and anthropogenic emissions, with the goal of identifying a model configuration best suited for characterizing air quality in locations where lake breezes commonly affect local air quality along the Lake Michigan shoreline. This analysis complements other studies in evaluating the impact of meteorological inputs and parameterizations on air quality in a complex environment.
Shreta Ghimire, Zachary J. Lebo, Shane Murphy, Stefan Rahimi, and Trang Tran
Atmos. Chem. Phys., 23, 9413–9438, https://doi.org/10.5194/acp-23-9413-2023, https://doi.org/10.5194/acp-23-9413-2023, 2023
Short summary
Short summary
High wintertime ozone levels have occurred often in recent years in mountain basins with oil and gas production facilities. Photochemical modeling of ozone production serves as a basis for understanding the mechanism by which it occurs and for predictive capability. We present photochemical model simulations of ozone formation and accumulation in the Upper Green River basin, Wyoming, demonstrating the model's ability to simulate wintertime ozone and the sensitivity of ozone to its precursors.
Adedayo R. Adedeji, Stephen J. Andrews, Matthew J. Rowlinson, Mathew J. Evans, Alastair C. Lewis, Shigeru Hashimoto, Hitoshi Mukai, Hiroshi Tanimoto, Yasunori Tohjima, and Takuya Saito
Atmos. Chem. Phys., 23, 9229–9244, https://doi.org/10.5194/acp-23-9229-2023, https://doi.org/10.5194/acp-23-9229-2023, 2023
Short summary
Short summary
We use the GEOS-Chem model to interpret observations of CO, C2H6, C3H8, NOx, NOy and O3 made from Hateruma Island in 2018. The model captures many synoptic-scale events and the seasonality of most pollutants at the site but underestimates C2H6 and C3H8 during the winter. These underestimates are unlikely to be reconciled by increases in biomass burning emissions but could be reconciled by increasing the Asian anthropogenic source of C2H6 and C3H8 by factors of around 2 and 3, respectively.
Bryan K. Place, William T. Hutzell, K. Wyat Appel, Sara Farrell, Lukas Valin, Benjamin N. Murphy, Karl M. Seltzer, Golam Sarwar, Christine Allen, Ivan R. Piletic, Emma L. D'Ambro, Emily Saunders, Heather Simon, Ana Torres-Vasquez, Jonathan Pleim, Rebecca H. Schwantes, Matthew M. Coggon, Lu Xu, William R. Stockwell, and Havala O. T. Pye
Atmos. Chem. Phys., 23, 9173–9190, https://doi.org/10.5194/acp-23-9173-2023, https://doi.org/10.5194/acp-23-9173-2023, 2023
Short summary
Short summary
Ground-level ozone is a pollutant with adverse human health and ecosystem effects. Air quality models allow scientists to understand the chemical production of ozone and demonstrate impacts of air quality management plans. In this work, the role of multiple systems in ozone production was investigated for the northeastern US in summer. Model updates to chemical reaction rates and monoterpene chemistry were most influential in decreasing predicted ozone and improving agreement with observations.
Alfred W. Mayhew, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 23, 8473–8485, https://doi.org/10.5194/acp-23-8473-2023, https://doi.org/10.5194/acp-23-8473-2023, 2023
Short summary
Short summary
Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper investigates modelled changes to daytime isoprene nitrate concentrations resulting from changes in NOx and O3. The results highlight the complex, nonlinear chemistry of this group of species under typical conditions for megacities such as Beijing, with many species showing increased concentrations when NOx is decreased and/or ozone is increased.
Alice Drinkwater, Paul I. Palmer, Liang Feng, Tim Arnold, Xin Lan, Sylvia E. Michel, Robert Parker, and Hartmut Boesch
Atmos. Chem. Phys., 23, 8429–8452, https://doi.org/10.5194/acp-23-8429-2023, https://doi.org/10.5194/acp-23-8429-2023, 2023
Short summary
Short summary
Changes in atmospheric methane over the last few decades are largely unexplained. Previous studies have proposed different hypotheses to explain short-term changes in atmospheric methane. We interpret observed changes in atmospheric methane and stable isotope source signatures (2004–2020). We argue that changes over this period are part of a large-scale shift from high-northern-latitude thermogenic energy emissions to tropical biogenic emissions, particularly from North Africa and South America.
Claudio A. Belis and Rita Van Dingenen
Atmos. Chem. Phys., 23, 8225–8240, https://doi.org/10.5194/acp-23-8225-2023, https://doi.org/10.5194/acp-23-8225-2023, 2023
Short summary
Short summary
The study assesses the influence that abating emissions in the rest of the world have on exposure and mortality due to ozone and fine particulate matter in the region covered by the Gothenburg protocol (UNECE, mainly Europe and North America). To that end, the impacts of pollutants derived from different geographic areas and anthropogenic sources are analysed in a series of scenarios including measures to abate air pollutants and greenhouse gas emissions with different levels of ambition.
Ruosi Liang, Yuzhong Zhang, Wei Chen, Peixuan Zhang, Jingran Liu, Cuihong Chen, Huiqin Mao, Guofeng Shen, Zhen Qu, Zichong Chen, Minqiang Zhou, Pucai Wang, Robert J. Parker, Hartmut Boesch, Alba Lorente, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 8039–8057, https://doi.org/10.5194/acp-23-8039-2023, https://doi.org/10.5194/acp-23-8039-2023, 2023
Short summary
Short summary
We compare and evaluate East Asian methane emissions inferred from different satellite observations (GOSAT and TROPOMI). The results show discrepancies over northern India and eastern China. Independent ground-based observations are more consistent with TROPOMI-derived emissions in northern India and GOSAT-derived emissions in eastern China.
Marc Guevara, Hervé Petetin, Oriol Jorba, Hugo Denier van der Gon, Jeroen Kuenen, Ingrid Super, Claire Granier, Thierno Doumbia, Philippe Ciais, Zhu Liu, Robin D. Lamboll, Sabine Schindlbacher, Bradley Matthews, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 8081–8101, https://doi.org/10.5194/acp-23-8081-2023, https://doi.org/10.5194/acp-23-8081-2023, 2023
Short summary
Short summary
This study provides an intercomparison of European 2020 emission changes derived from official inventories, which are reported by countries under the framework of several international conventions and directives, and non-official near-real-time estimates, the use of which has significantly grown since the COVID-19 outbreak. The results of the work are used to produce recommendations on how best to approach and make use of near-real-time emissions for modelling and monitoring applications.
Cited articles
Alvarez-Idaboy, J. R., Mora-Diez, N., Boyd, R. J., and Vivier-Bunge, A.: On
the Importance of Prereactive Complexes in Molecule-Radical Reactions:
Hydrogen Abstraction from Aldehydes by OH, J. Am. Chem. Soc., 123,
2018–2024, https://doi.org/10.1021/ja003372g, 2001.
Arquero, K. D., Xu, J., Gerber, R. B., and Finlayson-Pitts, B. J.: Particle
formation and growth from oxalic acid, methanesulfonic acid, trimethylamine
and water: a combined experimental and theoretical study, Phys. Chem. Chem.
Phys., 19, 28286–28301, https://doi.org/10.1039/C7CP04468B, 2017.
Atkinson, R.: Rate constants for the atmospheric reactions of alkoxy
radicals: An updated estimation method, Atmos. Environ., 41, 8468–8485,
https://doi.org/10.1016/j.atmosenv.2007.07.002, 2007.
Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F.,
Hynes, R. G., Jenkin, M. E., Rossi, M. J., Troe, J., and IUPAC Subcommittee:
Evaluated kinetic and photochemical data for atmospheric chemistry: Volume II
– gas phase reactions of organic species, Atmos. Chem. Phys., 6, 3625–4055,
https://doi.org/10.5194/acp-6-3625-2006, 2006.
Bandyopadhyay, B., Kumar, P., and Biswas, P.: Ammonia Catalyzed Formation of
Sulfuric Acid in Troposphere: The Curious Case of a Base Promoting Acid
Rain, J. Phys. Chem. A, 121, 3101–3108, https://doi.org/10.1021/acs.jpca.7b01172, 2017.
Bannan, T. J., Murray Booth, A., Le Breton, M., Bacak, A., Muller, J. B. A.,
Leather, K. E., Khan, M. A. H., Lee, J. D., Dunmore, R. E., Hopkins, J. R.,
Fleming, Z. L., Sheps, L., Taatjes, C. A., Shallcross, D. E., and Percival,
C. J.: Seasonality of Formic Acid (HCOOH) in London during the ClearfLo
Campaign, J. Geophys. Res.-Atmos., 122, 12488–12498,
https://doi.org/10.1002/2017JD027064, 2017.
Bao, L., Matsumoto, M., Kubota, T., Sekiguchi, K., Wang, Q., and Sakamoto,
K.: Gas/particle partitioning of low-molecular-weight dicarboxylic acids at
a suburban site in Saitama, Japan, Atmos. Environ., 47, 546–553,
https://doi.org/10.1016/j.atmosenv.2009.09.014, 2012.
Buemi, G.: DFT study of the hydrogen bond strength and IR spectra of formic,
oxalic, glyoxylic and pyruvic acids in vacuum, acetone and water solution,
J. Phys. Org. Chem., 22, 933–947, https://doi.org/10.1002/poc.1543, 2009.
Cameron, M., Sivakumaran, V., Dillon, T. J., and Crowley, J. N.: Reaction
between OH and CH3CHO Part 1. Primary product yields of CH3 (296 K),
CH3CO (296 K), and H (237–296 K), Phys. Chem. Chem. Phys., 4,
3628–3638, https://doi.org/10.1039/B202586H, 2002.
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.
Chen, J., Jiang, S., Liu, Y.-R., Huang, T., Wang, C.-Y., Miao, S.-K., Wang,
Z.-Q., Zhang, Y., and Huang, W.: Interaction of oxalic acid with
dimethylamine and its atmospheric implications, RSC Adv., 7,
6374–6388, https://doi.org/10.1039/C6RA27945G, 2017.
Courmier, D., Gardebien, F., Minot, C., and St-Amant, A.: A computational
study of the water-catalyzed formation of NH2CH2OH, Chem. Phys. Lett., 405,
357–363, https://doi.org/10.1016/j.cplett.2004.12.121, 2005.
Curtiss, L. A., Redfern, P. C., and Raghavachari, K.: Gaussian-4 theory, J.
Chem. Phys., 126, 084108, https://doi.org/10.1063/1.2436888, 2007.
da Silva, G.: Carboxylic Acid Catalyzed Keto-Enol Tautomerizations in the
Gas Phase, Angew. Chem. Int. Ed., 49, 7523–7525, https://doi.org/10.1002/anie.201003530, 2010.
Deshmukh, D. K., Kawamura, K., Lazaar, M., Kunwar, B., and Boreddy, S. K.
R.: Dicarboxylic acids, oxoacids, benzoic acid, α-dicarbonyls, WSOC,
OC, and ions in spring aerosols from Okinawa Island in the western North
Pacific Rim: size distributions and formation processes, Atmos. Chem. Phys.,
16, 5263–5282, https://doi.org/10.5194/acp-16-5263-2016, 2016.
Fukui, K.: The path of chemical reactions – the IRC approach, Acc. Chem.
Res., 14, 363–368, https://doi.org/10.1021/ar00072a001, 1981.
Gonzalez, J., Torrent-Sucarrat, M., and Anglada, J. M.: The reactions of
SO3 with HO2 radical and H2O⋯HO2
radical complex. Theoretical study on the atmospheric formation of
HSO5 and H2SO4, Phys. Chem. Chem. Phys., 12, 2116–2125,
https://doi.org/10.1039/B916659A, 2010.
Gutbrod, R., Schindler, R. N., Kraka, E., and Cremer, D.: Formation of OH
radicals in the gas phase ozonolysis of alkenes: the unexpected role of
carbonyl oxides, Chem. Phys. Lett., 252, 221–229, https://doi.org/10.1016/0009-2614(96)00126-1, 1996.
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.
Ho, K. F., Huang, R.-J., Kawamura, K., Tachibana, E., Lee, S. C., Ho, S. S.
H., Zhu, T., and Tian, L.: Dicarboxylic acids, ketocarboxylic acids,
α-dicarbonyls, fatty acids and benzoic acid in PM2.5 aerosol collected during
CAREBeijing-2007: an effect of traffic restriction on air quality, Atmos.
Chem. Phys., 15, 3111–3123, https://doi.org/10.5194/acp-15-3111-2015, 2015.
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.
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.
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.
Hratchian, H. P. and Schlegel, H. B.: Accurate reaction paths using a Hessian
based predictor–corrector integrator, J. Chem. Phys., 120, 9918–9924,
https://doi.org/10.1063/1.1724823, 2004.
Hratchian, H. P. and Schlegel, H. B.: Using Hessian Updating To Increase
the Efficiency of a Hessian Based Predictor-Corrector Reaction Path
Following Method, J. Chem. Theory Comput., 1, 61–69, https://doi.org/10.1021/ct0499783,
2005.
Ji, Y., Zhao, J., Terazono, H., Misawa, K., Levitt, N. P., Li, Y., Lin, Y.,
Peng, J., Wang, Y., Duan, L., Pan, B., Zhang, F., Feng, X., An, T.,
Marrero-Ortiz, W., Secrest, J., Zhang, A. L., Shibuya, K., Molina, M. J., and
Zhang, R.: Reassessing the atmospheric oxidation mechanism of toluene, P.
Natl. Acad. Sci. USA, 114, 8169, https://doi.org/10.1073/pnas.1705463114, 2017.
Ji, Y. M., Wang, H. H., Gao, Y. P., Li, G. Y., and An, T. C.: A theoretical
model on the formation mechanism and kinetics of highly toxic air pollutants
from halogenated formaldehydes reacted with halogen atoms, Atmos. Chem.
Phys., 13, 11277–11286, https://doi.org/10.5194/acp-13-11277-2013, 2013.
Kawamura, K. and Ikushima, K.: Seasonal changes in the distribution of
dicarboxylic acids in the urban atmosphere, Environ. Sci. Technol., 27,
2227–2235, https://doi.org/10.1021/es00047a033, 1993.
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.
Klopper, W., van Duijneveldt-van de Rijdt, J. G. C. M., and van Duijneveldt,
F. B.: Computational determination of equilibrium geometry and dissociation
energy of the water dimer, Phys. Chem. Chem. Phys., 2, 2227–2234, https://doi.org/10.1039/A910312K, 2000.
Kumar, M. and Francisco, J. S.: Red-Light-Induced Decomposition of an
Organic Peroxy Radical: A New Source of the HO2 Radical, Angew. Chem. Int.
Ed., 54, 15711–15714, https://doi.org/10.1002/anie.201509311, 2015.
Kumar, M., Sinha, A., and Francisco, J. S.: Role of Double Hydrogen Atom
Transfer Reactions in Atmospheric Chemistry, Acc. Chem. Res., 49, 877–883,
https://doi.org/10.1021/acs.accounts.6b00040, 2016.
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,
https://doi.org/10.1063/1.481532, 2000.
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, 8874–8878, https://doi.org/10.1073/pnas.97.16.8874, 2000.
Long, B., Long, Z.-W., Wang, Y.-B., Tan, X.-F., Han, Y.-H., Long, C.-Y.,
Qin, S.-J., and Zhang, W.-J.: Formic Acid Catalyzed Gas-Phase Reaction of
H2O with SO3 and the Reverse Reaction: A Theoretical Study, Chem. Phys. Chem.,
13, 323–329, https://doi.org/10.1002/cphc.201100558, 2012.
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.
Martinelango, P. K., Dasgupta, P. K., and Al-Horr, R. S.: Atmospheric
production of oxalic acid/oxalate and nitric acid/nitrate in the Tampa Bay
airshed: Parallel pathways, Atmos. Environ., 41, 4258–4269,
https://doi.org/10.1016/j.atmosenv.2006.05.085, 2007.
Miao, S.-K., Jiang, S., Chen, J., Ma, Y., Zhu, Y.-P., Wen, Y., Zhang, M.-M.,
and Huang, W.: Hydration of a sulfuric acid-oxalic acid complex: acid
dissociation and its atmospheric implication, RSC Adv., 5, 48638–48646, https://doi.org/10.1039/C5RA06116D, 2015.
Millet, D. B., Baasandorj, M., Farmer, D. K., Thornton, J. A., Baumann, K.,
Brophy, P., Chaliyakunnel, S., de Gouw, J. A., Graus, M., Hu, L., Koss, A.,
Lee, B. H., Lopez-Hilfiker, F. D., Neuman, J. A., Paulot, F., Peischl, J.,
Pollack, I. B., Ryerson, T. B., Warneke, C., Williams, B. J., and Xu, J.: A
large and ubiquitous source of atmospheric formic acid, Atmos. Chem. Phys.,
15, 6283–6304, https://doi.org/10.5194/acp-15-6283-2015, 2015.
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.
NASA and NOAA: Technical Report, available at:
https://ntrs.nasa.gov/archive/nasa/casi.ntrs.nasa.gov/19770009539.pdf
(last access: 17 August 2018), 1976.
Nieminen, J., Rasanen, M., and Murto, J.: Matrix-isolation and ab initio
studies of oxalic acid, J. Phys. Chem., 96, 5303–5308,
https://doi.org/10.1021/j100192a024, 1992.
Peng, X.-Q., Liu, Y.-R., Huang, T., Jiang, S., and Huang, W.: Interaction of
gas phase oxalic acid with ammonia and its atmospheric implications, Phys.
Chem. Chem. Phys., 17, 9552–9563, https://doi.org/10.1039/C5CP00027K, 2015.
Pople, J. A., Gordon, M., and Raghavachari, K.: Quadratic configuration
interaction. A general technique for determining electron correlation
energies, J. Chem. Phys., 87, 5968–5975, https://doi.org/10.1063/1.453520, 1987.
Purvis, G. D. and Bartlett, R. J.: A full coupled cluster singles and
doubles model: The inclusion of disconnected triples, J. Chem. Phys., 76,
1910–1918, https://doi.org/10.1063/1.443164, 1982.
Rayez, M.-T., Picquet-Varrault, B., Caralp, F., and Rayez, J.-C.:
CH3C(O)OCH(O⚫)CH3 alkoxy radical derived from ethyl
acetate: Novel rearrangement confirmed by computational chemistry, Phys.
Chem. Chem. Phys., 4, 5789–5794, https://doi.org/10.1039/B207511N, 2002.
Rocher-Casterline, B. E., Ch'ng, L. C., Mollner, A. K., and Reisler, H.:
Communication: Determination of the bond dissociation energy (D0) of the
water dimer, (H2O)2, by velocity map imaging, J. Chem. Phys., 134,
211101, https://doi.org/10.1063/1.3598339, 2011.
Steckler, R., Thurman, G. M., Watts, J. D., and Bartlett, R. J.: Ab initio
direct dynamics study of OH + HCl → Cl + H2O, J. Chem.
Phys., 106, 3926–3933, https://doi.org/10.1063/1.473981, 1997.
Steudel, R.: Sulfuric Acid from Sulfur Trioxide and Water – A Surprisingly
Complex Reaction, Angew. Chem. Int. Ed. Engl., 34, 1313–1315,
https://doi.org/10.1002/anie.199513131, 1995.
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.
Vöhringer-Martinez, E., Hansmann, B., Hernandez, H., Francisco, J. S.,
Troe, J., and Abel, B.: Water Catalysis of a Radical-Molecule Gas-Phase
Reaction, Science, 315, 497–501, https://doi.org/10.1126/science.1134494, 2007.
van Pinxteren, D., Neusüß, C., and Herrmann, H.: On the abundance and
source contributions of dicarboxylic acids in size-resolved aerosol particles
at continental sites in central Europe, Atmos. Chem. Phys., 14, 3913–3928,
https://doi.org/10.5194/acp-14-3913-2014, 2014.
Wang, G., Zhang, R., Gomez, M. E., Yang, L., Levy Zamora, M., Hu, M., Lin,
Y., Peng, J., Guo, S., Meng, J., Li, J., Cheng, C., Hu, T., Ren, Y., Wang,
Y., Gao, J., Cao, J., An, Z., Zhou, W., Li, G., Wang, J., Tian, P.,
Marrero-Ortiz, W., Secrest, J., Du, Z., Zheng, J., Shang, D., Zeng, L., Shao,
M., Wang, W., Huang, Y., Wang, Y., Zhu, Y., Li, Y., Hu, J., Pan, B., Cai, L.,
Cheng, Y., Ji, Y., Zhang, F., Rosenfeld, D., Liss, P. S., Duce, R. A., Kolb,
C. E., and Molina, M. J.: Persistent sulfate formation from London Fog to
Chinese haze, P. Natl. Acad. Sci. USA, 113, 13630,
https://doi.org/10.1073/pnas.1616540113, 2016.
Weber, K. H., Morales, F. J., and Tao, F.-M.: Theoretical Study on the
Structure and Stabilities of Molecular Clusters of Oxalic Acid with Water, J.
Phys. Chem. A, 116, 11601–11617, https://doi.org/10.1021/jp308499f, 2012.
Weber, K. H., Liu, Q., and Tao, F.-M.: Theoretical Study on Stable Small
Clusters of Oxalic Acid with Ammonia and Water, J. Phys. Chem. A, 118,
1451–1468, https://doi.org/10.1021/jp4128226, 2014.
Williams, I. H., Spangler, D., Femec, D. A., Maggiora, G. M., and Schowen, R.
L.: Theoretical models for solvation and catalysis in carbonyl addition, J.
Am. Chem. Soc., 105, 31–40, https://doi.org/10.1021/ja00339a008, 1983.
Xu, J., Finlayson-Pitts, B. J., and Gerber, R. B.: Proton Transfer in Mixed
Clusters of Methanesulfonic Acid, Methylamine, and Oxalic Acid: Implications
for Atmospheric Particle Formation, J. Phys. Chem. A, 121, 2377–2385,
https://doi.org/10.1021/acs.jpca.7b01223, 2017.
Xu, W. and Zhang, R.: Theoretical Investigation of Interaction of
Dicarboxylic Acids with Common Aerosol Nucleation Precursors, J. Phys. Chem.
A, 116, 4539–4550, https://doi.org/10.1021/jp301964u, 2012.
Xu, Y., Nadykto, A. B., Yu, F., Jiang, L., and Wang, W.: Formation and
properties of hydrogen-bonded complexes of common organic oxalic acid with
atmospheric nucleation precursors, J. Mol. Struct. Theochem., 951, 28–33,
https://doi.org/10.1016/j.theochem.2010.04.004, 2010.
Zhang, D. and Zhang, R.: Mechanism of OH Formation from Ozonolysis of
Isoprene: A Quantum-Chemical Study, J. Am. Chem. Soc., 124, 2692–2703,
https://doi.org/10.1021/ja011518l, 2002.
Zhang, R.: Getting to the Critical Nucleus of Aerosol Formation, Science,
328, 1366, https://doi.org/10.1126/science.1189732, 2010.
Zhao, H., Zhang, Q., and Du, L.: Hydrogen bonding in cyclic complexes of
carboxylic acid-sulfuric acid and their atmospheric implications, RSC Adv.,
6, 71733–71743, https://doi.org/10.1039/C6RA16782A, 2016.
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.
Zheng, J. and Truhlar, D. G.: Kinetics of hydrogen-transfer isomerizations of
butoxyl radicals, Phys. Chem. Chem. Phys., 12, 7782–7793,
https://doi.org/10.1039/B927504E, 2010.
Short summary
The hydration of SO3 to produce H2SO4 is an important process in the atmosphere. Using quantum chemical calculations, we investigated the catalytic role of oxalic acid in the SO3 hydration reaction. The results show that oxalic acid is effective in facilitating the hydration of SO3 to form H2SO4. The kinetic analysis result indicates that the oxalic-acid-catalyzed SO3 hydration can play an important role in the upper troposphere.
The hydration of SO3 to produce H2SO4 is an important process in the atmosphere. Using quantum...
Altmetrics
Final-revised paper
Preprint