Articles | Volume 19, issue 5
Atmos. Chem. Phys., 19, 2833–2844, 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: Multiphase chemistry of secondary aerosol formation under...
Research article 04 Mar 2019
Research article | 04 Mar 2019
Understanding the catalytic role of oxalic acid in SO3 hydration to form H2SO4 in the atmosphere
Guochun Lv et al.
No articles found.
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,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,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,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,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,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,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,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,
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,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,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,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,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,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,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,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.
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)Emission inventory of air pollutants and chemical speciation for specific anthropogenic sources based on local measurements in the Yangtze River Delta region, ChinaPhotochemical environment over Southeast Asia primed for hazardous ozone levels with influx of nitrogen oxides from seasonal biomass burningAtmospheric-methane source and sink sensitivity analysis using Gaussian process emulationCarbon and air pollutant emissions from China's cement industry 1990–2015: trends, evolution of technologies, and driversAssessment of pre-industrial to present-day anthropogenic climate forcing in UKESM1Technical note: A high-resolution inverse modelling technique for estimating surface CO2 fluxes based on the NIES-TM–FLEXPART coupled transport model and its adjointImprovement of the satellite-derived NOx emissions on air quality modeling and its effect on ozone and secondary inorganic aerosol formation in the Yangtze River Delta, ChinaAircraft-based inversions quantify the importance of wetlands and livestock for Upper Midwest methane emissionsTime-resolved emission reductions for atmospheric chemistry modelling in Europe during the COVID-19 lockdownsRapid increase in summer surface ozone over the North China Plain during 2013–2019: a side effect of particulate matter reduction control?Pan-Arctic surface ozone: modelling vs. measurementsInfluence of aerosol copper on HO2 uptake: a novel parameterized equationRole of ammonia in European air quality with changing land and ship emissions between 1990 and 2030Discrepancies between MICS-Asia III simulation and observation for surface ozone in the marine atmosphere over the northwestern Pacific Asian Rim regionCorrecting model biases of CO in East Asia: impact on oxidant distributions during KORUS-AQQuantifying the emission changes and associated air quality impacts during the COVID-19 pandemic on the North China Plain: a response modeling studyDo alternative inventories converge on the spatiotemporal representation of spring ammonia emissions in France?Impacts of global NOx inversions on NO2 and ozone simulationsReactive Organic Carbon Emissions from Volatile Chemical ProductsQuantifying sources of Brazil's CH4 emissions between 2010 and 2018 from satellite dataOn the role of trend and variability in the hydroxyl radical (OH) in the global methane budgetTrends in global tropospheric hydroxyl radical and methane lifetime since 1850 from AerChemMIPEstimation of rate coefficients for the reactions of O3 with unsaturated organic compounds for use in automated mechanism constructionLong-term historical trends in air pollutant emissions in Asia: Regional Emission inventory in ASia (REAS) version 3A Comparison of Long-term Trends in Observations and Emission Inventories of NOxThe impact of weather patterns and related transport processes on aviation's contribution to ozone and methane concentrations from NOx emissionsNorthwestward cropland expansion and growing urea-based fertilizer use enhanced NH3 emission loss in the contiguous United StatesTechnical note: On comparing greenhouse gas emission metricsImpact of reduced anthropogenic emissions during COVID-19 on air quality in IndiaEvaluating China's fossil-fuel CO2 emissions from a comprehensive dataset of nine inventoriesIncreases in surface ozone pollution in China from 2013 to 2019: anthropogenic and meteorological influencesThe impact of inhomogeneous emissions and topography on ozone photochemistry in the vicinity of the Hong Kong islandMeteorology-normalized impact of the COVID-19 lockdown upon NO2 pollution in SpainAttribution of the accelerating increase in atmospheric methane during 2010–2018 by inverse analysis of GOSAT observationsTropospheric ozone radiative forcing uncertainty due to pre-industrial fire and biogenic emissionsCRI-HOM: A novel chemical mechanism for simulating highly oxygenated organic molecules (HOMs) in global chemistry–aerosol–climate modelsGlobal Impact of COVID-19 Restrictions on the Surface Concentrations of Nitrogen Dioxide and OzoneIdentifying forecast uncertainties for biogenic gases in the Po valley related to model configuration in EURAD-IM during PEGASOS 2012The impact of ship emissions on air quality and human health in the Gothenburg area – Part II: Scenarios for 2040Attribution of ground-level ozone to anthropogenic and natural sources of nitrogen oxides and reactive carbon in a global chemical transport modelCharacterizing sources of high surface ozone events in the southwestern US with intensive field measurements and two global modelsAn inversion of NOx and non-methane volatile organic compound (NMVOC) emissions using satellite observations during the KORUS-AQ campaign and implications for surface ozone over East AsiaInfluences of hydroxyl radicals (OH) on top-down estimates of the global and regional methane budgetsEvaluation of nitrogen oxides (NOx) sources and sinks and ozone production in Colombia and surrounding areasThe impact of biomass burning on upper tropospheric carbon monoxide: a study using MOCAGE global model and IAGOS airborne dataTemporal and spatial analysis of ozone concentrations in Europe based on timescale decomposition and a multi-clustering approachWhy is the Indo-Gangetic Plain the region with the largest NH3 column in the globe during pre-monsoon and monsoon seasons?Improving the prediction of an atmospheric chemistry transport model using gradient-boosted regression treesInverse modelling of carbonyl sulfide: implementation, evaluation and implications for the global budgetAttributing ozone and its precursors to land transport emissions in Europe and Germany
Jingyu An, Yiwei Huang, Cheng Huang, Xin Wang, Rusha Yan, Qian Wang, Hongli Wang, Sheng'ao Jing, Yan Zhang, Yiming Liu, Yuan Chen, Chang Xu, Liping Qiao, Min Zhou, Shuhui Zhu, Qingyao Hu, Jun Lu, and Changhong Chen
Atmos. Chem. Phys., 21, 2003–2025,Short summary
This study established a 4 km × 4 km anthropogenic emission inventory in the Yangtze River Delta region, China, for 2017 based on locally measured emission factors and source profiles. There are high-intensity NOx and NMVOC species emissions in the eastern areas of the region. Toluene, 1,2,4-trimethylbenzene, m,p-xylene, propylene, ethylene, o-xylene, and OVOCs from industry and mobile sources have the highest comprehensive potentials for ozone and secondary organic aerosol formation.
Margaret R. Marvin, Paul I. Palmer, Barry G. Latter, Richard Siddans, Brian J. Kerridge, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 21, 1917–1935,Short summary
We use an atmospheric chemistry model in combination with satellite and surface observations to investigate how biomass burning affects tropospheric ozone over Southeast Asia during its fire seasons. We find that nitrogen oxides from biomass burning were responsible for about 30 % of the regional ozone formation potential, and we estimate that ozone from biomass burning caused more than 400 excess premature deaths in Southeast Asia during the peak burning months of March and September 2014.
Angharad C. Stell, Luke M. Western, Tomás Sherwen, and Matthew Rigby
Atmos. Chem. Phys., 21, 1717–1736,Short summary
Although it is the second-most important greenhouse gas, our understanding of the atmospheric-methane budget is limited. The uncertainty highlights the need for new tools to investigate sources and sinks. Here, we use a Gaussian process emulator to efficiently approximate the response of atmospheric-methane observations to changes in the most uncertain emission or loss processes. With this new method, we rigorously quantify the sensitivity of atmospheric observations to budget uncertainties.
Jun Liu, Dan Tong, Yixuan Zheng, Jing Cheng, Xinying Qin, Qinren Shi, Liu Yan, Yu Lei, and Qiang Zhang
Atmos. Chem. Phys., 21, 1627–1647,Short summary
In this study, we investigated the decadal changes in carbon dioxide and air pollutant emissions in China's cement industry for the period 1990–2015 based on intensive unit-based information. We found that from 1990 to 2015, accompanied by a 10.3-fold increase in cement production, CO2, SO2, and NOx emissions from China's cement industry increased by 627 %, 56 %, and 659 %, whereas CO, PM2.5, and PM10 emissions decreased by 9 %, 63 %, and 59 %, respectively.
Fiona M. O'Connor, N. Luke Abraham, Mohit Dalvi, Gerd A. Folberth, Paul T. Griffiths, Catherine Hardacre, Ben T. Johnson, Ron Kahana, James Keeble, Byeonghyeon Kim, Olaf Morgenstern, Jane P. Mulcahy, Mark Richardson, Eddy Robertson, Jeongbyn Seo, Sungbo Shim, João C. Teixeira, Steven T. Turnock, Jonny Williams, Andrew J. Wiltshire, Stephanie Woodward, and Guang Zeng
Atmos. Chem. Phys., 21, 1211–1243,Short summary
This paper calculates how changes in emissions and/or concentrations of different atmospheric constituents since the pre-industrial era have altered the Earth's energy budget at the present day using a metric called effective radiative forcing. The impact of land use change is also assessed. We find that individual contributions do not add linearly, and different Earth system interactions can affect the magnitude of the calculated effective radiative forcing.
Shamil Maksyutov, Tomohiro Oda, Makoto Saito, Rajesh Janardanan, Dmitry Belikov, Johannes W. Kaiser, Ruslan Zhuravlev, Alexander Ganshin, Vinu K. Valsala, Arlyn Andrews, Lukasz Chmura, Edward Dlugokencky, László Haszpra, Ray L. Langenfelds, Toshinobu Machida, Takakiyo Nakazawa, Michel Ramonet, Colm Sweeney, and Douglas Worthy
Atmos. Chem. Phys., 21, 1245–1266,Short summary
In order to improve the top-down estimation of the anthropogenic greenhouse gas emissions, a high-resolution inverse modelling technique was developed for applications to global transport modelling of carbon dioxide and other greenhouse gases. A coupled Eulerian–Lagrangian transport model and its adjoint are combined with surface fluxes at 0.1° resolution to provide high-resolution forward simulation and inverse modelling of surface fluxes accounting for signals from emission hot spots.
Yang Yang, Yu Zhao, Lei Zhang, Jie Zhang, Xin Huang, Xuefen Zhao, Yan Zhang, Mengxiao Xi, and Yi Lu
Atmos. Chem. Phys., 21, 1191–1209,Short summary
We conducted new NOx emission estimation based on the satellite-derived NO2 column constraint and found reduced emissions compared to previous estimates for a developed region in east China. The subsequent improvement in air quality modeling was demonstrated based on available ground observations. With multiple emission reduction cases for various pollutants, we explored the effective control approaches for ozone and inorganic aerosol pollution.
Xueying Yu, Dylan B. Millet, Kelley C. Wells, Daven K. Henze, Hansen Cao, Timothy J. Griffis, Eric A. Kort, Genevieve Plant, Malte J. Deventer, Randall K. Kolka, D. Tyler Roman, Kenneth J. Davis, Ankur R. Desai, Bianca C. Baier, Kathryn McKain, Alan C. Czarnetzki, and A. Anthony Bloom
Atmos. Chem. Phys., 21, 951–971,Short summary
Methane concentrations have doubled since 1750. The US Upper Midwest is a key region contributing to such trends, but sources are poorly understood. We collected and analyzed aircraft data to resolve spatial and timing biases in wetland and livestock emission estimates and uncover errors in inventory treatment of manure management. We highlight the importance of intensive agriculture for the regional and US methane budgets and the potential for methane mitigation through improved management.
Marc Guevara, Oriol Jorba, Albert Soret, Hervé Petetin, Dene Bowdalo, Kim Serradell, Carles Tena, Hugo Denier van der Gon, Jeroen Kuenen, Vincent-Henri Peuch, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 21, 773–797,Short summary
Most European countries have imposed lockdowns to combat the spread of the COVID-19 pandemic. Such a socioeconomic disruption has resulted in a sudden drop of atmospheric emissions and air pollution levels. This study quantifies the daily reductions in national emissions and associated levels of nitrogen dioxide (NO2) due to the COVID-19 lockdowns in Europe, by making use of multiple open-access measured activity data as well as artificial intelligence and modelling techniques.
Xiaodan Ma, Jianping Huang, Tianliang Zhao, Cheng Liu, Kaihui Zhao, Jia Xing, and Wei Xiao
Atmos. Chem. Phys., 21, 1–16,Short summary
The present work aims at identifying and quantifying the relative contributions of the key factors in driving a rapid increase in summertime surface O3 over the North China Plain during 2013–2019. In addition to anthropogenic emission reduction and meteorological variabilities, our study highlights the importance of inclusion of aerosol absorption and scattering properties rather than aerosol abundance only in accurate assessment of aerosol radiative effect on surface O3 formation and change.
Xin Yang, Anne-M. Blechschmidt, Kristof Bognar, Audra McClure-Begley, Sara Morris, Irina Petropavlovskikh, Andreas Richter, Henrik Skov, Kimberly Strong, David W. Tarasick, Taneil Uttal, Mika Vestenius, and Xiaoyi Zhao
Atmos. Chem. Phys., 20, 15937–15967,Short summary
This is a modelling-based study on Arctic surface ozone, with a particular focus on spring ozone depletion events (i.e. with concentrations < 10 ppbv). Model experiments show that model runs with blowing-snow-sourced sea salt aerosols implemented as a source of reactive bromine can reproduce well large-scale ozone depletion events observed in the Arctic. This study supplies modelling evidence of the proposed mechanism of reactive-bromine release from blowing snow on sea ice (Yang et al., 2008).
Huan Song, Xiaorui Chen, Keding Lu, Qi Zou, Zhaofeng Tan, Hendrik Fuchs, Alfred Wiedensohler, Daniel R. Moon, Dwayne E. Heard, María-Teresa Baeza-Romero, Mei Zheng, Andreas Wahner, Astrid Kiendler-Scharr, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 15835–15850,Short summary
Accurate calculation of the HO2 uptake coefficient is one of the key parameters to quantify the co-reduction of both aerosol and ozone pollution. We modelled various lab measurements of γHO2 based on a gas-liquid phase kinetic model and developed a state-of-the-art parameterized equation. Based on a dataset from a comprehensive field campaign in the North China Plain, we proposed that the determination of the heterogeneous uptake process for HO2 should be included in future field campaigns.
Sebnem Aksoyoglu, Jianhui Jiang, Giancarlo Ciarelli, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 15665–15680,Short summary
We investigated the role of ammonia in European air quality between 1990 and 2030 under varying land and ship emissions. If ship emissions will be regulated more strictly in the future, particulate nitrate will decrease in coastal areas in northern Europe, while sulfate aerosol will decrease in the Mediterranean region. We predict a shift in the sensitivity of aerosol formation from NH3 towards NOx emissions between 1990 and 2030 in most of Europe except the eastern part of the model domain.
Hajime Akimoto, Tatsuya Nagashima, Natsumi Kawano, Li Jie, Joshua S. Fu, and Zifa Wang
Atmos. Chem. Phys., 20, 15003–15014,Short summary
In order to perform proper model simulation of ozone near the ground in the coastal area of northeastern Asia, it has been found that it is very important to select appropriate dry deposition velocities of ozone on the oceanic water of specific area of the northwestern Pacific. Empirical measurement of the mixing ratios and dry deposition flux of ozone over the ocean in this area is highly recommended.
Benjamin Gaubert, Louisa K. Emmons, Kevin Raeder, Simone Tilmes, Kazuyuki Miyazaki, Avelino F. Arellano Jr., Nellie Elguindi, Claire Granier, Wenfu Tang, Jérôme Barré, Helen M. Worden, Rebecca R. Buchholz, David P. Edwards, Philipp Franke, Jeffrey L. Anderson, Marielle Saunois, Jason Schroeder, Jung-Hun Woo, Isobel J. Simpson, Donald R. Blake, Simone Meinardi, Paul O. Wennberg, John Crounse, Alex Teng, Michelle Kim, Russell R. Dickerson, Hao He, Xinrong Ren, Sally E. Pusede, and Glenn S. Diskin
Atmos. Chem. Phys., 20, 14617–14647,Short summary
This study investigates carbon monoxide pollution in East Asia during spring using a numerical model, satellite remote sensing, and aircraft measurements. We found an underestimation of emission sources. Correcting the emission bias can improve air quality forecasting of carbon monoxide and other species including ozone. Results also suggest that controlling VOC and CO emissions, in addition to widespread NOx controls, can improve ozone pollution over East Asia.
Jia Xing, Siwei Li, Yueqi Jiang, Shuxiao Wang, Dian Ding, Zhaoxin Dong, Yun Zhu, and Jiming Hao
Atmos. Chem. Phys., 20, 14347–14359,Short summary
Quantifying emission changes is a prerequisite for assessment of control effectiveness in improving air quality. However, traditional bottom-up methods usually take months to perform and limit timely assessments. A novel method was developed by using a response model that provides real-time estimation of emission changes based on air quality observations. It was successfully applied to quantify emission changes on the North China Plain due to the COVID-19 pandemic shutdown.
Audrey Fortems-Cheiney, Gaëlle Dufour, Karine Dufossé, Florian Couvidat, Jean-Marc Gilliot, Guillaume Siour, Matthias Beekmann, Gilles Foret, Frederik Meleux, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Cathy Clerbaux, and Sophie Génermont
Atmos. Chem. Phys., 20, 13481–13495,Short summary
Studies have suggested the importance of ammonia emissions on pollution particle formation over Europe, whose main atmospheric source is agriculture. In this study, we performed an inter-comparison of two alternative inventories, both with a reference inventory, that quantify the French ammonia emissions during spring 2011. Over regions with large mineral fertilizer use, like over northeastern France, NH3 emissions are probably considerably underestimated by the reference inventory.
Zhen Qu, Daven K. Henze, Owen R. Cooper, and Jessica L. Neu
Atmos. Chem. Phys., 20, 13109–13130,Short summary
We use satellite observations and chemical transport modeling to quantify sources of NOx, a major air pollutant, over the past decade. We find improved simulations of the magnitude, seasonality, and trends of NO2 and ozone concentrations using these derived emissions. Changes in ozone pollution driven by human and natural sources are identified in different regions. This work shows the benefits of remote-sensing data and inverse modeling for more accurate ozone simulations.
Karl M. Seltzer, Elyse Pennington, Venkatesh Rao, Benjamin N. Murphy, Madeleine Strum, Kristin K. Isaacs, and Havala O. T. Pye
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon emissions. Here, we develop VCPy, a new framework to model organic emissions from VCPs throughout the United States. At the national-level, VCPy emissions are broadly consistent with the US EPA's 2017 National Emission Inventory, however county-level and categorical estimates can differ substantially. An observational evaluation indicates high fidelity in the methods employed here.
Rachel L. Tunnicliffe, Anita L. Ganesan, Robert J. Parker, Hartmut Boesch, Nicola Gedney, Benjamin Poulter, Zhen Zhang, Jošt V. Lavrič, David Walter, Matthew Rigby, Stephan Henne, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 20, 13041–13067,Short summary
This study quantifies Brazil’s emissions of a potent atmospheric greenhouse gas, methane. This is in the field of atmospheric modelling and uses remotely sensed data and surface measurements of methane concentrations as well as an atmospheric transport model to interpret the data. Because of Brazil’s large emissions from wetlands, agriculture and biomass burning, these emissions affect global methane concentrations and thus are of global significance.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 20, 13011–13022,Short summary
Decadal trends and variations in OH are critical for understanding atmospheric CH4 evolution. We quantify the impacts of OH trends and variations on the CH4 budget by conducting CH4 inversions on a decadal scale with an ensemble of OH fields. We find the negative OH anomalies due to enhanced fires can reduce the optimized CH4 emissions by up to 10 Tg yr−1 during El Niño years and the positive OH trend from 1986 to 2010 results in a ∼ 23 Tg yr−1 additional increase in optimized CH4 emissions.
David S. Stevenson, Alcide Zhao, Vaishali Naik, Fiona M. O'Connor, Simone Tilmes, Guang Zeng, Lee T. Murray, William J. Collins, Paul T. Griffiths, Sungbo Shim, Larry W. Horowitz, Lori T. Sentman, and Louisa Emmons
Atmos. Chem. Phys., 20, 12905–12920,Short summary
We present historical trends in atmospheric oxidizing capacity (OC) since 1850 from the latest generation of global climate models and compare these with estimates from measurements. OC controls levels of many key reactive gases, including methane (CH4). We find small model trends up to 1980, then increases of about 9 % up to 2014, disagreeing with (uncertain) measurement-based trends. Major drivers of OC trends are emissions of CH4, NOx, and CO; these will be important for future CH4 trends.
Michael E. Jenkin, Richard Valorso, Bernard Aumont, Mike J. Newland, and Andrew R. Rickard
Atmos. Chem. Phys., 20, 12921–12937,Short summary
Unsaturated organic compounds are emitted in large quantities from natural and human-influenced sources. Atmospheric removal occurs significantly by reaction with ozone, initiating reaction sequences forming free radicals and organic pollutants in the gaseous and particulate phases. Due to their very large number, it is impossible to study the reaction rate for every compound, and most have to be estimated. Updated and extended estimation methods are reported for use in atmospheric models.
Junichi Kurokawa and Toshimasa Ohara
Atmos. Chem. Phys., 20, 12761–12793,Short summary
A long historical emission inventory of major air pollutants in Asia during 1950–2015 was developed as Regional Emission inventory in ASia version 3 (REASv3). Trends of emissions and changes in source contributions in countries and regions in Asia during these 6 decades were analyzed. REASv3 provides monthly gridded data with 0.25° by 0.25° resolution for major source categories as well as table of emissions by countries and sub-regions for major sectors and fuel types.
Elena Macdonald, Noelia Otero Felipe, and Tim Butler
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
NO2 limit values are still regularly exceeded in many European cities despite decreasing emissions. Measurements of NOx concentrations from stations across Europe were systematically analysed to assess long-term changes observed in urban areas. We compared trends in concentration increments to trends in total and traffic emissions to find potential discrepancies. The results can help with evaluating inaccuracies in emission inventories and with improving spatial imbalances in data availability.
Simon Rosanka, Christine Frömming, and Volker Grewe
Atmos. Chem. Phys., 20, 12347–12361,Short summary
Aviation-attributed nitrogen oxide (NOx) emissions lead to an increase in ozone and a depletion of methane. We investigate the impact of weather-related transport processes on these induced composition changes. Subsidence in high-pressure systems leads to earlier ozone maxima due to an enhanced chemical activity. Background NOx and hydroperoxyl radicals limit the total ozone change during summer and winter, respectively. High water vapour concentrations lead to a high methane depletion.
Peiyu Cao, Chaoqun Lu, Jien Zhang, and Avani Khadilkar
Atmos. Chem. Phys., 20, 11907–11922,Short summary
In this study, we estimate monthly ammonia emission from synthetic nitrogen fertilizer use across the contiguous US from 1900 to 2015. The results indicate the important role that cropland expansion and nitrogen fertilizer enrichment played in enhancing NH3 emissions. It shows such long-term human activities have dramatically changed the spatiotemporal and seasonal patterns of NH3 emission, impacting air pollution and public health in the US.
Ian Enting and Nathan Clisby
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
We provide a new framework for comparing short-lived greenhouse gases, using methane as an example, to long-lived greenhouse gases such as carbon dioxide. This can clarify the differences between various proposals that have been introduced in order to overcome the use of Global Warming Potentials as a measure of greenhouse gas equivalence.
Mengyuan Zhang, Apit Katiyar, Shengqiang Zhu, Juanyong Shen, Men Xia, Jinlong Ma, Sri Harsha Kota, Peng Wang, and Hongliang Zhang
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
We studied changes in air quality in India induced by the lockdown of COVID-19 through both surface observations and the CMAQ model. Our results show that emission reductions have improved the air quality across India during the lockdown. On average, the levels of PM2.5 and O3 have decreased by 28% and 15%, indicating positive effects of lockdown measures. We suggest that more stringent and localized emissions control strategies should be implemented in India to mitigate air pollutions.
Pengfei Han, Ning Zeng, Tom Oda, Xiaohui Lin, Monica Crippa, Dabo Guan, Greet Janssens-Maenhout, Xiaolin Ma, Zhu Liu, Yuli Shan, Shu Tao, Haikun Wang, Rong Wang, Lin Wu, Xiao Yun, Qiang Zhang, Fang Zhao, and Bo Zheng
Atmos. Chem. Phys., 20, 11371–11385,Short summary
An accurate estimation of China’s fossil-fuel CO2 emissions (FFCO2) is significant for quantification of carbon budget and emissions reductions towards the Paris Agreement goals. Here we assessed 9 global and regional inventories. Our findings highlight the significance of using locally measured coal emission factors. We call on the enhancement of physical measurements for validation and provide comprehensive information for inventory, monitoring, modeling, assimilation, and reducing emissions.
Ke Li, Daniel J. Jacob, Lu Shen, Xiao Lu, Isabelle De Smedt, and Hong Liao
Atmos. Chem. Phys., 20, 11423–11433,Short summary
Surface summer ozone increased in China from 2013 to 2019 despite new governmental efforts targeting ozone pollution. We find that the ozone increase is mostly due to anthropogenic drivers, although meteorology also plays a role. Further analysis for the North China Plain shows that PM2.5 continued to decrease through 2019, while emissions of volatile organic compounds (VOCs) stayed flat. This could explain the anthropogenic increase in ozone, as PM2.5 scavenges the radical precursors of ozone.
Yuting Wang, Yong-Feng Ma, Domingo Muñoz-Esparza, Cathy W. Y. Li, Mary Barth, Tao Wang, and Guy P. Brasseur
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Large-eddy simulations (LES) were performed in the mountainous region of the Hong Kong island to investigate the degree to which the rates of chemical reactions between two reactive species are reduced due to the segregation of species within the convective boundary layer. We show that the inhomogeneity in emissions plays an important role in the segregation effect. Topography also has a significant influence on the segregation locally.
Hervé Petetin, Dene Bowdalo, Albert Soret, Marc Guevara, Oriol Jorba, Kim Serradell, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 20, 11119–11141,Short summary
To control the spread of the COVID-19 coronavirus, the Spanish Government recently implemented a strict lockdown of the population, which strongly reduced the levels of nitrogen dioxide (NO2), one of the most critical air pollutants in Spain. This study quantifies the contribution of the lockdown on these reduced NO2 levels in Spain, taking the confounding effect of meteorology on artificial intelligence techniques into account.
Yuzhong Zhang, Daniel J. Jacob, Xiao Lu, Joannes D. Maasakkers, Tia R. Scarpelli, Jian-Xiong Sheng, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Jinfeng Chang, Anthony A. Bloom, Shuang Ma, John Worden, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
We use 2010–2018 satellite observations of atmospheric methane to interpret the factors controlling atmospheric methane and its accelerating increase during the period. The 2010–2018 increase in global methane emissions is driven by tropical (Amazon, tropical Africa) and boreal wetlands (Eurasia), and tropical livestock (South Asia, Africa, Brazil), with no significant trend in oil/gas emissions. The peak methane growth rates in 2014–2015 are also contributed by low OH and high fire emissions.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951,Short summary
Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
James Weber, Scott Archer-Nicholls, Paul Griffiths, Torsten Berndt, Michael Jenkin, Hamish Gordon, Christoph Knote, and Alexander T. Archibald
Atmos. Chem. Phys., 20, 10889–10910,Short summary
Highly oxygenated organic molecules (HOMs) are important for aerosol growth and new particle formation, particularly in air masses with less sulphuric acid. This new chemical mechanism reproduces measured [HOM] and [HOM precursors] and is concise enough for use in global climate models. The mechanism also reproduces the observed suppression of HOMs by isoprene, suggesting enhanced emissions may not necessarily lead to more aerosols. Greater HOM importance in the pre-industrial era is also shown.
Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the compounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Annika Vogel and Hendrik Elbern
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Forecasts of biogenic trace gases highly depend on the model setup and input fields. This study identifies sources of related forecast uncertainties for biogenic gases. Exceptionally high differences in both, biogenic emissions and pollutant transport in the Po valley are identified to be caused by the representation of the land surface and boundary layer dynamics. Consequently, changes in the model configuration are shown to induce significantly different local concentrations of biogenic gases.
Martin O. P. Ramacher, Lin Tang, Jana Moldanová, Volker Matthias, Matthias Karl, Erik Fridell, and Lasse Johansson
Atmos. Chem. Phys., 20, 10667–10686,Short summary
The effects of shipping emissions on air quality and health in the harbour city of Gothenburg were simulated for different scenarios for the year 2040 with coupled regional and city-scale chemistry transport models to evaluate the impact of regional emission regulations and onshore electricity for ships at berth. The results show that contributions of shipping to exposure and associated health impacts from particulate matter and NO2 decrease significantly compared to 2012 in all scenarios.
Tim Butler, Aurelia Lupascu, and Aditya Nalam
Atmos. Chem. Phys., 20, 10707–10731,Short summary
Ground-level ozone (O3) is not directly emitted; it is formed chemically in the atmosphere. Some ground-level O3 is transported from the stratosphere, but most O3 is produced from reactive precursors that are emitted by both natural and anthropogenic sources. We present the results of a novel source apportionment method for ground-level O3. Our results are consistent with previous work and also provide new insights. In particular, we highlight the roles of methane and international shipping.
Li Zhang, Meiyun Lin, Andrew O. Langford, Larry W. Horowitz, Christoph J. Senff, Elizabeth Klovenski, Yuxuan Wang, Raul J. Alvarez II, Irina Petropavlovskikh, Patrick Cullis, Chance W. Sterling, Jeff Peischl, Thomas B. Ryerson, Steven S. Brown, Zachary C. J. Decker, Guillaume Kirgis, and Stephen Conley
Atmos. Chem. Phys., 20, 10379–10400,Short summary
Measuring and quantifying the sources of elevated springtime ozone in the southwestern US is challenging but relevant to the implications for control policy. Here we use intensive field measurements and two global models to study ozone sources in the region. We find that ozone from the stratosphere, wildfires, and Asia is an important source of high-ozone events in the region. Our analysis also helps understand the uncertainties in ozone simulations with individual models.
Amir H. Souri, Caroline R. Nowlan, Gonzalo González Abad, Lei Zhu, Donald R. Blake, Alan Fried, Andrew J. Weinheimer, Armin Wisthaler, Jung-Hun Woo, Qiang Zhang, Christopher E. Chan Miller, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 20, 9837–9854,Short summary
For the first time, we provide a joint nonlinear optimal estimate of NOx and NMVOC emissions during the KORUS-AQ campaign by simultaneously incorporating SAO's new product of HCHO columns from OMPS and OMI tropospheric NO2 columns into a regional model. Results demonstrate a promising improvement in the performance of the model in terms of HCHO and NO2 concentrations, which in turn enables us to quantify the impact of the emission changes on different pathways of ozone formation and loss.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Edward J. Dlugokencky, Ray L. Langenfelds, Michel Ramonet, Doug Worthy, and Bo Zheng
Atmos. Chem. Phys., 20, 9525–9546,Short summary
The hydroxyl radical (OH), which is the dominant sink of methane (CH4), plays a key role in closing the global methane budget. This study quantifies how uncertainties in the hydroxyl radical can influence top-down estimates of CH4 emissions based on 4D Bayesian inversions with different OH fields and the same surface observations. We show that uncertainties in CH4 emissions driven by different OH fields are comparable to the uncertainties given by current bottom-up and top-down estimations.
Johannes G. M. Barten, Laurens N. Ganzeveld, Auke J. Visser, Rodrigo Jiménez, and Maarten C. Krol
Atmos. Chem. Phys., 20, 9441–9458,Short summary
Combining satellite and urban air pollution measurements with a meteorology and air quality model, we present the state of air quality in Colombia. We found four distinctly different emission regimes. The simulated pollution levels compare well with satellite data, but the comparison also indicates misrepresentation of prescribed fire emissions and simulated lightning emissions. Comparison of urban measurements requires careful consideration of (nocturnal) boundary layer dynamics and advection.
Martin Cussac, Virginie Marécal, Valérie Thouret, Béatrice Josse, and Bastien Sauvage
Atmos. Chem. Phys., 20, 9393–9417,Short summary
Biomass burning emissions are a major source of carbon monoxide in the atmosphere. Here, the vertical transport that these emissions can undergo until the upper troposphere is investigated, as well as their contribution to carbon monoxide concentrations. It was found that boreal forest emissions were specific to the occurrence of pyroconvection directly above the fires, whereas biomass burning emissions from other regions of the globe relied more on the occurrence of deep convection.
Eirini Boleti, Christoph Hueglin, Stuart K. Grange, André S. H. Prévôt, and Satoshi Takahama
Atmos. Chem. Phys., 20, 9051–9066,Short summary
Long-term temporal evolution of ozone concentrations between 2000 and 2015 in Europe was estimated using a signal decomposition technique. The seasonal cycles are correlated with local climate conditions and vary according to geographic region, while ozone levels are indicative of distance to emission sources. The site's environment plays a key role in ozone trends, with the most polluted environments showing the least reduction in ozone, while in less polluted areas ozone has decreased.
Tiantian Wang, Yu Song, Zhenying Xu, Mingxu Liu, Tingting Xu, Wenling Liao, Lifei Yin, Xuhui Cai, Ling Kang, Hongsheng Zhang, and Tong Zhu
Atmos. Chem. Phys., 20, 8727–8736,Short summary
Satellite measurements have revealed that the Indo-Gangetic Plain (IGP) has the global maximum ammonia concentrations, with a peak from June to August. Here, we studied the reasons for this phenomenon through computer simulations. Low sulfur dioxide and nitrogen oxides emissions and high air temperature over the IGP weaken the swallowing of gaseous ammonia by acidic gases. Additionally, the barrier effects of the Himalayas, like a windshield, are also conducive to the accumulation of ammonia.
Peter D. Ivatt and Mathew J. Evans
Atmos. Chem. Phys., 20, 8063–8082,Short summary
We investigate the potential of using a decision tree algorithm to identify and correct the tropospheric ozone bias in a chemical transport model. We train the algorithm on 2010–2015 ground and column observation data and test the algorithm on the 2016–2017 data using the ground data as well as independent flight data. We find the algorithm is successfully able to identify and correct the bias, improving the model performance.
Jin Ma, Linda M. J. Kooijmans, Ara Cho, Stephen A. Montzka, Norbert Glatthor, John R. Worden, Le Kuai, Elliot L. Atlas, and Maarten C. Krol
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Carbonyl sulfide is an important trace gas in the atmosphere and useful to estimate gross primary productivity in ecosystem, but its sources and sinks remain highly uncertain. Therefore, we applied inverse model system TM5-4DVAR to better constrain the global budget. Our finding is in line with earlier studies, pointing to missing sources in tropics and more uptake in high latitudes. We also stress on the necessity of more ground-based observations and satellite data assimilation in future.
Mariano Mertens, Astrid Kerkweg, Volker Grewe, Patrick Jöckel, and Robert Sausen
Atmos. Chem. Phys., 20, 7843–7873,Short summary
We investigate the contribution of land transport emissions to ozone and ozone precursors in Europe and Germany. Our results show that land transport emissions are one of the most important contributors to reactive nitrogen in Europe. The contribution to ozone is in the range of 8 % to 16 % and varies strongly for different seasons. The hots-pots with the largest ozone concentrations are the Po Valley, while the largest concentration to reactive nitrogen is located mainly in western Europe.
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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...