Articles | Volume 21, issue 10
Research article 25 May 2021
Research article | 25 May 2021
SO2 and NH3 emissions enhance organosulfur compounds and fine particle formation from the photooxidation of a typical aromatic hydrocarbon
Zhaomin Yang et al.
No articles found.
Qingcai Chen, Zhen Mu, Li Xu, Mamin Wang, Jin Wang, Ming Shan, Xudong Yang, Xingjun Fan, Jianzhong Song, Yuqin Wang, Pengchuan Lin, Lixin Zhang, Zhenxing Shen, and Lin Du
Atmos. Chem. Phys. Discuss.,
Preprint withdrawnShort summary
It is important to study the formation characteristics and mechanism of triplet state in aerosols to quantify the effect of chromophore substances on the global climate and atmospheric environmental quality. The result of this study reveals that chromophore substances contributes significantly to aerosol photochemistry and plays an important role in aerosol aging. The global models may need to include those potential effects in the future.
Xiaotong Jiang, Narcisse T. Tsona, Long Jia, Shijie Liu, Hailiang Zhang, Yongfu Xu, and Lin Du
Atmos. Chem. Phys., 19, 13591–13609,Short summary
Atmospheric furan is a primary and secondary pollutant in the atmosphere, and its emission contributes to the formation of ultrafine particles and ground-level ozone. The present study demonstrates the effect of NOx and humidity on secondary organic aerosol (SOA) formation during the furan–NOx–NaCl photooxidation. Furthermore, the results illustrate the importance of studying SOA formation over a comprehensive range of environmental conditions.
Jun Zhang, Xinfeng Wang, Rui Li, Shuwei Dong, Yingnan Zhang, Penggang Zheng, Min Li, Tianshu Chen, Yuhong Liu, Likun Xue, Wei Nie, Aijun Ding, Mingjin Tang, Xuehua Zhou, Lin Du, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys. Discuss.,
Preprint withdrawnShort summary
This study presents the concentrations, variation characteristics, and key influencing factors of particulate organic nitrates at four urban and rural sites in eastern China. The effects of anthropogenic activities (i.e. biomass burning and coal combustion) and meteorological conditions (in particular the humidity) on the secondary formation of organic nitrates have been investigated. The results highlight the greater role of SO2 in organic nitrate chemistry than previously assumed.
Siyang Li, Xiaotong Jiang, Marie Roveretto, Christian George, Ling Liu, Wei Jiang, Qingzhu Zhang, Wenxing Wang, Maofa Ge, and Lin Du
Atmos. Chem. Phys., 19, 9887–9902,Short summary
We stimulated the photochemical aging of organic film coated on aqueous aerosol in the presence of imidazole-2-carboxaldehyde, humic acid, an atmospheric PM2.5 sample, and a secondary organic aerosol sample from the lab. The unsaturated lipid mixed with photosensitizer under UV irradiation produced hydroperoxides, leading to surface area increase in organic film. Our results reveal the modification of organic film on aqueous aerosol has potential influence on the hygroscopic growth of droplets.
Narcisse Tchinda Tsona and Lin Du
Atmos. Chem. Phys., 19, 649–661,Short summary
We used ab initio calculations to explore a new path for ion-induced SO2 oxidation by ozone in the gas phase. We find that, initiated by the superoxide ion, SO2 can readily oxidize to SO−3. The reaction is facilitated by the presence of water, being ~ 4 orders of magnitude faster than the reaction in the absence of water. Depending on the altitude and temperature, it is estimated that this reaction may contribute to 0.1–2.0 % of the total atmospheric sulfate.
Xiaotong Jiang, Narcisse T. Tsona, Long Jia, Shijie Liu, Yongfu Xu, and Lin Du
Atmos. Chem. Phys. Discuss.,
Revised manuscript not acceptedShort summary
The roles of NOx level and RH on the formation of SOA from the photooxidation of furan in the presence of NaCl seed particles were elucidated. The aerosol liquid water (ALW) effects on SOA mass concentration and yield were also evaluated. The chemical composition of furan SOA was investigated by ESI-Exactive-Orbitrap MS, with focus on the formation of organic nitrates. Strong evidences indicate that both the RH and different NOx levels have a significant effect on SOA formation.
Shijie Liu, Long Jia, Yongfu Xu, Narcisse T. Tsona, Shuangshuang Ge, and Lin Du
Atmos. Chem. Phys., 17, 13329–13343,Short summary
Secondary organic aerosol (SOA) formation from cyclohexene/NOx system with various SO2 concentrations under UV light was investigated to study the effects of cyclic alkenes on the atmospheric environment in polluted urban areas. The composition of organic compounds in SOA was measured using several complementary techniques. We present new evidence that organosulfates were produced from the photooxidation of cyclohexene in the presence of SO2.
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)Revisiting the reaction of dicarbonyls in aerosol proxy solutions containing ammonia: the case of butenedialImportance of secondary organic aerosol formation of α-pinene, limonene, and m-cresol comparing day- and nighttime radical chemistrySource apportionment of carbonaceous aerosols in Beijing with radiocarbon and organic tracers: insight into the differences between urban and rural sitesOn the similarities and differences between the products of oxidation of hydrocarbons under simulated atmospheric conditions and cool flamesEnhanced secondary organic aerosol formation from the photo-oxidation of mixed anthropogenic volatile organic compoundsFormation kinetics and mechanisms of ozone and secondary organic aerosols from photochemical oxidation of different aromatic hydrocarbons: dependence on NOx and organic substituentsIncreased primary and secondary H2SO4 showing the opposing roles in secondary organic aerosol formation from ethyl methacrylate ozonolysisWater uptake of subpollen aerosol particles: hygroscopic growth, cloud condensation nuclei activation, and liquid–liquid phase separationLaboratory study of the collection efficiency of submicron aerosol particles by cloud droplets – Part II: Influence of electric chargesHeterogeneous interactions between SO2 and organic peroxides in submicron aerosolTemperature and acidity dependence of secondary organic aerosol formation from α-pinene ozonolysis with a compact chamber systemProduction of HONO from NO2 uptake on illuminated TiO2 aerosol particles and following the illumination of mixed TiO2∕ammonium nitrate particlesCharacterization of secondary organic aerosol from heated-cooking-oil emissions: evolution in composition and volatilityMeasurement report: Diurnal and temporal variations of sugar compounds in suburban aerosols from the northern vicinity of Beijing, China – an influence of biogenic and anthropogenic sourcesPre-deliquescent water uptake in deposited nanoparticles observed with in situ ambient pressure X-ray photoelectron spectroscopyTechnical note: Emission factors, chemical composition, and morphology of particles emitted from Euro 5 diesel and gasoline light-duty vehicles during transient cyclesMeasurement report: Distinct emissions and volatility distribution of intermediate-volatility organic compounds from on-road Chinese gasoline vehicles: implication of high secondary organic aerosol formation potentialEmissions of intermediate-volatility and semi-volatile organic compounds from domestic fuels used in Delhi, IndiaEffects of liquid–liquid phase separation and relative humidity on the heterogeneous OH oxidation of inorganic–organic aerosols: insights from methylglutaric acid and ammonium sulfate particlesMeasurement report: Sulfuric acid nucleation and experimental conditions in a photolytic flow reactorOzonolysis of fatty acid monolayers at the air–water interface: organic films may persist at the surface of atmospheric aerosolsQuantification of the role of stabilized Criegee intermediates in the formation of aerosols in limonene ozonolysisTracer-based source apportioning of atmospheric organic carbon and the influence of anthropogenic emissions on secondary organic aerosol formation in Hong KongPhotochemical degradation of iron(III) citrate/citric acid aerosol quantified with the combination of three complementary experimental techniques and a kinetic process modelThe production and hydrolysis of organic nitrates from OH radical oxidation of β-ocimeneEmission factors for PM10 and polycyclic aromatic hydrocarbons (PAHs) from illegal burning of different types of municipal waste in householdsKinetic modeling of formation and evaporation of secondary organic aerosol from NO3 oxidation of pure and mixed monoterpenesDirect contribution of ammonia to α-pinene secondary organic aerosol formationHygroscopic behavior of aerosols generated from solutions of 3-methyl-1,2,3-butanetricarboxylic acid, its sodium salts, and its mixtures with NaClChemical composition, structures, and light absorption of N-containing aromatic compounds emitted from burning wood and charcoal in household cookstovesChemical composition and light absorption of carbonaceous aerosols emitted from crop residue burning: influence of combustion efficiencyOn mineral dust aerosol hygroscopicityDistinct chemical and mineralogical composition of Icelandic dust compared to northern African and Asian dustSecondary organic aerosol yields from the oxidation of benzyl alcoholThe Aarhus Chamber Campaign on Highly Oxygenated Organic Molecules and Aerosols (ACCHA): particle formation, organic acids, and dimer esters from α-pinene ozonolysis at different temperaturesMolecular understanding of the suppression of new-particle formation by isopreneReactive species formed upon interaction of water with fine particulate matter from remote forest and polluted urban airComplex plant-derived organic aerosol as ice-nucleating particles – more than the sums of their parts?Liquid–liquid phase separation and morphologies in organic particles consisting of α-pinene and β-caryophyllene ozonolysis products and mixtures with commercially available organic compoundsCharacterization of primary and aged wood burning and coal combustion organic aerosols in environmental chamber and its implications for atmospheric aerosolsOligomer and highly oxygenated organic molecule formation from oxidation of oxygenated monoterpenes emitted by California sage plantsLaboratory studies of fresh and aged biomass burning aerosol emitted from east African biomass fuels – Part 2: Chemical properties and characterizationImpact of NOx on secondary organic aerosol (SOA) formation from α-pinene and β-pinene photooxidation: the role of highly oxygenated organic nitratesEvaluation of the chemical composition of gas- and particle-phase products of aromatic oxidationGlyoxal's impact on dry ammonium salts: fast and reversible surface aerosol browningOxygenated products formed from OH-initiated reactions of trimethylbenzene: autoxidation and accretionBiomass-burning-derived particles from a wide variety of fuels – Part 2: Effects of photochemical aging on particle optical and chemical propertiesMeasured solid state and subcooled liquid vapour pressures of nitroaromatics using Knudsen effusion mass spectrometryPolar semivolatile organic compounds in biomass-burning emissions and their chemical transformations during aging in an oxidation flow reactorTemperature effects on optical properties and chemical composition of secondary organic aerosol derived from n-dodecane
Jack C. Hensley, Adam W. Birdsall, Gregory Valtierra, Joshua L. Cox, and Frank N. Keutsch
Atmos. Chem. Phys., 21, 8809–8821,Short summary
We measured reactions of butenedial, an atmospheric dicarbonyl, in aqueous mixtures that mimic the conditions of aerosol particles. Major reaction products and rates were determined to assess their atmospheric relevance and to compare against other well-studied dicarbonyls. We suggest that the structure of the carbon backbone, not just the dominant functional group, plays a major role in dicarbonyl reactivity, influencing the fate and ability of dicarbonyls to produce brown carbon.
Anke Mutzel, Yanli Zhang, Olaf Böge, Maria Rodigast, Agata Kolodziejczyk, Xinming Wang, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 8479–8498,Short summary
This study investigates secondary organic aerosol (SOA) formation and particle growth from α-pinene, limonene, and m-cresol oxidation through NO3 and OH radicals and the effect of relative humidity. The formed SOA is comprehensively characterized with respect to the content of OC / EC, WSOC, SOA-bound peroxides, and SOA marker compounds. The findings present new insights and implications of nighttime chemistry, which can form SOA more efficiently than OH radical reaction during daytime.
Siqi Hou, Di Liu, Jingsha Xu, Tuan V. Vu, Xuefang Wu, Deepchandra Srivastava, Pingqing Fu, Linjie Li, Yele Sun, Athanasia Vlachou, Vaios Moschos, Gary Salazar, Sönke Szidat, André S. H. Prévôt, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 8273–8292,Short summary
This study provides a newly developed method which combines radiocarbon (14C) with organic tracers to enable source apportionment of primary and secondary fossil vs. non-fossil sources of carbonaceous aerosols at an urban and a rural site of Beijing. The source apportionment results were compared with those by chemical mass balance and AMS/ACSM-PMF methods. Correlations of WINSOC and WSOC with different sources of OC were also performed to elucidate the formation mechanisms of SOC.
Roland Benoit, Nesrine Belhadj, Maxence Lailliau, and Philippe Dagaut
Atmos. Chem. Phys., 21, 7845–7862,Short summary
This study compares different modes of limonene oxidation (ozonolysis, photooxidation, and cool flame) on the basis of review articles and experimental results. Although the oxidation conditions are totally different, the results obtained present great similarities in the nature of the products but also specificities related to autooxidation such as the presence of keto-hydroperoxides.
Junling Li, Hong Li, Kun Li, Yan Chen, Hao Zhang, Xin Zhang, Zhenhai Wu, Yongchun Liu, Xuezhong Wang, Weigang Wang, and Maofa Ge
Atmos. Chem. Phys., 21, 7773–7789,Short summary
SOA formation from the mixed anthropogenic volatile organic compounds was enhanced compared to the predicted SOA mass concentration based on the SOA yield of single species; interaction occurred between intermediate products from the two precursors. Interactions between the intermediate products from the mixtures and the effect on SOA formation give us a further understanding of the SOA formed in the atmosphere.
Hao Luo, Jiangyao Chen, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 21, 7567–7578,Short summary
The formation kinetics and mechanism of O3 and SOA from different AHs are still unclear. Thus the photochemical oxidation mechanism of nine AHs with NO2 is studied. Increased formation rate and yield of O3 and SOA are observed via promoting AH content. Raising the number of AH substituents enhances O3 formation but decreases SOA yield, which is promoted by increasing the methyl group number of AHs. Results help show conversion of AHs to secondary pollutants in the real atmospheric environment.
Peng Zhang, Tianzeng Chen, Jun Liu, Guangyan Xu, Qingxin Ma, Biwu Chu, Wanqi Sun, and Hong He
Atmos. Chem. Phys., 21, 7099–7112,Short summary
This work highlights the opposing effects of primary and secondary H2SO4 on both secondary organic aerosol (SOA) formation and constitutes. Our findings revealed that a substantial increase in secondary H2SO4 particles promoted the SOA formation of ethyl methacrylate with increasing SO2 in the absence of seed particles. However, increased primary H2SO4 with seed acidity enhanced ethyl methacrylate uptake but reduced its SOA formation in the presence of seed particles.
Eugene F. Mikhailov, Mira L. Pöhlker, Kathrin Reinmuth-Selzle, Sergey S. Vlasenko, Ovid O. Krüger, Janine Fröhlich-Nowoisky, Christopher Pöhlker, Olga A. Ivanova, Alexey A. Kiselev, Leslie A. Kremper, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 6999–7022,Short summary
Subpollen particles are a relatively new subset of atmospheric aerosol particles. When pollen grains rupture, they release cytoplasmic fragments known as subpollen particles (SPPs). We found that SPPs, containing a broad spectrum of biopolymers and hydrocarbons, exhibit abnormally high water uptake. This effect may influence the life cycle of SPPs and the related direct and indirect impacts on radiation budget as well as reinforce their allergic potential.
Alexis Dépée, Pascal Lemaitre, Thomas Gelain, Marie Monier, and Andrea Flossmann
Atmos. Chem. Phys., 21, 6963–6984,Short summary
The present article describes a new In-Cloud Aerosol Scavenging Experiment (In-CASE) that has been conceived to measure the collection efficiency of submicron aerosol particles by cloud droplets. The present article focuses on the influence of electrostatic effects on the collection efficiency.
Shunyao Wang, Tengyu Liu, Jinmyung Jang, Jonathan P. D. Abbatt, and Arthur W. H. Chan
Atmos. Chem. Phys., 21, 6647–6661,Short summary
Discrepancies between atmospheric modeling and field observations, especially in highly polluted cities, have highlighted the lack of understanding of sulfate formation mechanisms and kinetics. Here, we directly quantify the reactive uptake coefficient of SO2 onto organic peroxides and study the important governing factors. The SO2 uptake rate was observed to depend on RH, peroxide amount and reactivity, pH, and ionic strength, which provides a framework to better predict sulfate formation.
Yange Deng, Satoshi Inomata, Kei Sato, Sathiyamurthi Ramasamy, Yu Morino, Shinichi Enami, and Hiroshi Tanimoto
Atmos. Chem. Phys., 21, 5983–6003,Short summary
The temperature and acidity dependence of yields and chemical compositions of the α-pinene ozonolysis SOA were systematically investigated using a newly developed compact chamber system. Increases in SOA yields were observed with the decrease in temperature and under acidic seed conditions. The differences in chemical compositions between acidic and neutral seed conditions were characterized and explained from the viewpoints of acid-catalyzed reactions. Some organosulfates were newly detected.
Joanna E. Dyson, Graham A. Boustead, Lauren T. Fleming, Mark Blitz, Daniel Stone, Stephen R. Arnold, Lisa K. Whalley, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 5755–5775,Short summary
The hydroxyl radical (OH) dominates the removal of atmospheric pollutants, with nitrous acid (HONO) recognised as a major OH source. For remote regions HONO production through the action of sunlight on aerosol surfaces can provide a source of nitrogen oxides. In this study, HONO production rates at illuminated aerosol surfaces are measured under atmospheric conditions, a model consistent with the data is developed and aerosol production of HONO in the atmosphere is shown to be significant.
Manpreet Takhar, Yunchun Li, and Arthur W. H. Chan
Atmos. Chem. Phys., 21, 5137–5149,Short summary
Our study highlights the importance of molecular composition in constraining the chemical properties of cooking SOA as well as understanding the contribution of aldehydes in formation of SOA from cooking emissions. We show that fragmentation reactions are key in atmospheric processing of cooking SOA, and aldehydes emitted from cooking emissions contribute substantially to SOA formation. Our study provides a framework to better predict SOA formation in and downwind of urban atmospheres.
Santosh Kumar Verma, Kimitaka Kawamura, Fei Yang, Pingqing Fu, Yugo Kanaya, and Zifa Wang
Atmos. Chem. Phys., 21, 4959–4978,Short summary
We studied aerosol samples collected in autumn 2007 with day and night intervals in a rural site of Mangshan, north of Beijing, for sugar compounds (SCs) that are abundant organic aerosol components and can influence the air quality and climate. We found higher concentrations of biomass burning (BB) products at nighttime than daytime, whereas pollen tracers and other SCs showed an opposite diurnal trend, because this site is meteorologically characterized by a mountain/valley breeze.
Jack J. Lin, Kamal Raj R, Stella Wang, Esko Kokkonen, Mikko-Heikki Mikkelä, Samuli Urpelainen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 4709–4727,Short summary
We used surface-sensitive X-ray photoelectron spectroscopy (XPS) to study laboratory-generated nanoparticles of atmospheric interest at 0–16 % relative humidity. XPS gives direct information about changes in the chemical state from the binding energies of probed elements. Our results indicate water adsorption and associated chemical changes at the particle surfaces well below deliquescence, with distinct features for different particle components and implications for atmospheric chemistry.
Evangelia Kostenidou, Alvaro Martinez-Valiente, Badr R'Mili, Baptiste Marques, Brice Temime-Roussel, Amandine Durand, Michel André, Yao Liu, Cédric Louis, Boris Vansevenant, Daniel Ferry, Carine Laffon, Philippe Parent, and Barbara D'Anna
Atmos. Chem. Phys., 21, 4779–4796,Short summary
Passenger vehicle emissions can be a significant source of particulate matter in urban areas. In this study the particle-phase emissions of seven Euro 5 passenger vehicles were characterized. Changes in engine technologies and after-treatment devices can alter the chemical composition and the size of the emitted particulate matter. The condition of the diesel particle filter (DPF) plays an important role in the emitted pollutants.
Rongzhi Tang, Quanyang Lu, Song Guo, Hui Wang, Kai Song, Ying Yu, Rui Tan, Kefan Liu, Ruizhe Shen, Shiyi Chen, Limin Zeng, Spiro D. Jorga, Zhou Zhang, Wenbin Zhang, Shijin Shuai, and Allen L. Robinson
Atmos. Chem. Phys., 21, 2569–2583,Short summary
We performed chassis dynamometer experiments to investigate the emissions and secondary organic aerosol (SOA) formation potential of intermediate volatility organic compounds (IVOCs) from an on-road Chinese gasoline vehicle. High IVOC emission factors (EFs) and distinct volatility distribution were recognized. Our results indicate that vehicular IVOCs contribute significantly to SOA, implying the importance of reducing IVOCs when making air pollution control policies in urban areas of China.
Gareth J. Stewart, Beth S. Nelson, W. Joe F. Acton, Adam R. Vaughan, Naomi J. Farren, James R. Hopkins, Martyn W. Ward, Stefan J. Swift, Rahul Arya, Arnab Mondal, Ritu Jangirh, Sakshi Ahlawat, Lokesh Yadav, Sudhir K. Sharma, Siti S. M. Yunus, C. Nicholas Hewitt, Eiko Nemitz, Neil Mullinger, Ranu Gadi, Lokesh K. Sahu, Nidhi Tripathi, Andrew R. Rickard, James D. Lee, Tuhin K. Mandal, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 2407–2426,Short summary
Biomass burning releases many lower-molecular-weight organic species which are difficult to analyse but important for the formation of organic aerosol. This study examined a new high-resolution technique to better characterise these difficult-to-analyse organic components. Some burning sources analysed in this study, such as cow dung cake and municipal solid waste, released extremely complex mixtures containing many thousands of different lower-volatility organic compounds.
Hoi Ki Lam, Rongshuang Xu, Jack Choczynski, James F. Davies, Dongwan Ham, Mijung Song, Andreas Zuend, Wentao Li, Ying-Lung Steve Tse, and Man Nin Chan
Atmos. Chem. Phys., 21, 2053–2066,Short summary
This work demonstrates that organic compounds present at or near the surface of aerosols can be subjected to oxidation initiated by gas-phase oxidants, such as hydroxyl radicals (OH). The heterogeneous reactivity is sensitive to their surface concentrations, which are determined by the phase separation behavior. This results of this work emphasize the effects of phase separation and potentially distinct aerosol morphologies on the chemical transformation of atmospheric aerosols.
David R. Hanson, Seakh Menheer, Michael Wentzel, and Joan Kunz
Atmos. Chem. Phys., 21, 1987–2001,Short summary
We report experimental measurements of particle formation in a flow reactor that extend the results from this experiment to a total of more than 270 runs over a time period of ~3 years. This has allowed us to detect a general increase in the cleanliness of the system and improve our knowledge of its chemistry. In-house simulations allowed us to construct phenomenological free energies of molecular clusters of sulfuric acid and ammonia that are appropriate for application to the atmosphere.
Benjamin Woden, Maximilian W. A. Skoda, Adam Milsom, Curtis Gubb, Armando Maestro, James Tellam, and Christian Pfrang
Atmos. Chem. Phys., 21, 1325–1340,Short summary
Atmospheric aerosols contain a large amount of organic compounds, whose oxidation affects their physical properties through a process known as ageing. We have simulated atmospheric ageing experimentally to elucidate the nature and behaviour of residual surface films. Our results show an increasing amount of residue at near-zero temperatures, demonstrating that an inert product film may build up during droplet ageing, even if only ordinarily short-lived reactive species are initially emitted.
Yiwei Gong and Zhongming Chen
Atmos. Chem. Phys., 21, 813–829,Short summary
Stabilized Criegee intermediates (SCIs) are important factors in estimating aerosol formation in the atmosphere. Here the results show that SCIs account for more than 60 % of aerosol formation in limonene ozonolysis and water is an uncertainty in SCI performances. The aerosol formation potential of SCIs under high-humidity conditions is double that under dry and low-humidity conditions, suggesting SCI reactions are still important in contributing to aerosols at high relative humidity.
Yubo Cheng, Yiqiu Ma, and Di Hu
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
We conducted comprehensive chemical characterization and source apportionment of PM2.5 samples collected in Hong Kong. Secondary formation was the leading contributor to OC throughout the year, and monoterpenes were the most significant SOA precursors in the region. Isoprene SOA was mainly formed from the aerosol phase reaction of isoprene epoxydiols. NOx processing played a key role in both daytime and nighttime SOA production, especially the nighttime NO3 oxidation of biogenic VOCs.
Jing Dou, Peter A. Alpert, Pablo Corral Arroyo, Beiping Luo, Frederic Schneider, Jacinta Xto, Thomas Huthwelker, Camelia N. Borca, Katja D. Henzler, Jörg Raabe, Benjamin Watts, Hartmut Herrmann, Thomas Peter, Markus Ammann, and Ulrich K. Krieger
Atmos. Chem. Phys., 21, 315–338,Short summary
Photochemistry of iron(III) complexes plays an important role in aerosol aging, especially in the lower troposphere. Ensuing radical chemistry leads to decarboxylation, and the production of peroxides, and oxygenated volatile compounds, resulting in particle mass loss due to release of the volatile products to the gas phase. We investigated kinetic transport limitations due to high particle viscosity under low relative humidity conditions. For quantification a numerical model was developed.
Ana C. Morales, Thilina Jayarathne, Jonathan H. Slade, Alexander Laskin, and Paul B. Shepson
Atmos. Chem. Phys., 21, 129–145,Short summary
Organic nitrates formed from the oxidation of biogenic volatile organic compounds impact both ozone and particulate matter as they remove nitrogen oxides, but they represent important aerosol precursors. We conducted a series of reaction chamber experiments that quantified the total organic nitrate and secondary organic aerosol yield from the OH-radical-initiated oxidation of ocimene, and also measured their hydrolysis lifetimes in the aqueous phase, as a function of pH.
András Hoffer, Beatrix Jancsek-Turóczi, Ádám Tóth, Gyula Kiss, Anca Naghiu, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 20, 16135–16144,Short summary
Emission factors for PM10 and polycyclic aromatic hydrocarbons (PAHs) are reported for the first time ever for the indoor combustion of 12 common types of municipal solid waste that are frequently burned in households worldwide. We have found that waste burning emits up to 40 times more PM10 and 800 times more PAHs than the combustion of dry firewood. Our finding highlights the need for coordinated actions against illegal waste combustion and the extreme health hazard associated with it.
Thomas Berkemeier, Masayuki Takeuchi, Gamze Eris, and Nga L. Ng
Atmos. Chem. Phys., 20, 15513–15535,Short summary
This paper presents how environmental chamber data of secondary organic aerosol (SOA) formation can be interpreted using kinetic modeling techniques. Utilizing pure and mixed precursor experiments, we show that SOA formation and evaporation can be understood by explicitly treating gas-phase chemistry, gas–particle partitioning, and, notably, particle-phase oligomerization, but some of the non-linear, non-equilibrium effects must be accredited to diffusion limitations in the particle phase.
Liqing Hao, Eetu Kari, Ari Leskinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 20, 14393–14405,Short summary
Our work presents the observational results of secondary organic aerosol (SOA) formation in the presence of ammonia. The particle-phase ammonium was continuously produced even after SOA formation had ceased. The gas-phase organic acids were observed to contribute to the formed particle-phase ammonium salts. This study suggests that the presence of ammonia may change the mass and chemical composition of large-size SOA particles and can potentially alter the aerosol impact on climate change.
Li Wu, Clara Becote, Sophie Sobanska, Pierre-Marie Flaud, Emilie Perraudin, Eric Villenave, Young-Chul Song, and Chul-Un Ro
Atmos. Chem. Phys., 20, 14103–14122,Short summary
MBTCA (3-methyl-1,2,3-butanetricarboxylic acid), a second-generation product of monoterpenes, is one of the most relevant tracer compounds for biogenic secondary organic aerosols (SOAs). Laboratory-generated, micrometer-sized, pure-MBTCA, mono-/di-/trisodium MBTCA salts and MBTCA–NaCl mixture aerosol particles were examined systematically to observe their hygroscopic behavior, and it was also observed that the monosodium MBTCA salt aerosols were formed through a reaction between MBTCA and NaCl.
Mingjie Xie, Zhenzhen Zhao, Amara L. Holder, Michael D. Hays, Xi Chen, Guofeng Shen, James J. Jetter, Wyatt M. Champion, and Qin'geng Wang
Atmos. Chem. Phys., 20, 14077–14090,Short summary
This study investigated the composition, structures, and light absorption of N-containing aromatic compounds (NACs) in PM2.5 emitted from burning red oak and charcoal in a variety of cookstoves. The results suggest that the identified NACs might have substantial fractions remaining in the gas phase. In comparison to other sources, cookstove emissions from red oak or charcoal fuels did not exhibit unique NAC structural features but had distinct NAC composition.
Yujue Wang, Min Hu, Nan Xu, Yanhong Qin, Zhijun Wu, Liwu Zeng, Xiaofeng Huang, and Lingyan He
Atmos. Chem. Phys., 20, 13721–13734,Short summary
Field straw residue burning is a widespread type of biomass burning in Asia, while its emissions are poorly understood. In this study, we designed lab-controlled experiments to comprehensively investigate the emission factors, chemical compositions and light absorption properties of both water-soluble and water-insoluble carbonaceous aerosols emitted from straw burning. The results clearly highlight the significant influences of burning conditions and combustion efficiency on the emissions.
Lanxiadi Chen, Chao Peng, Wenjun Gu, Hanjing Fu, Xing Jian, Huanhuan Zhang, Guohua Zhang, Jianxi Zhu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13611–13626,Short summary
We investigated hygroscopic properties of a number of mineral dust particles in a quantitative manner, via measuring the sample mass at different relative humidities. The robust and comprehensive data obtained would significantly improve our knowledge of hygroscopicity of mineral dust and its impacts on atmospheric chemistry and climate.
Clarissa Baldo, Paola Formenti, Sophie Nowak, Servanne Chevaillier, Mathieu Cazaunau, Edouard Pangui, Claudia Di Biagio, Jean-Francois Doussin, Konstantin Ignatyev, Pavla Dagsson-Waldhauserova, Olafur Arnalds, A. Robert MacKenzie, and Zongbo Shi
Atmos. Chem. Phys., 20, 13521–13539,Short summary
We showed that Icelandic dust has a fundamentally different chemical and mineralogical composition from low-latitude dust. In particular, magnetite is as high as 1 %–2 % of the total dust mass. Our results suggest that Icelandic dust may have an important impact on the radiation balance in the subpolar and polar regions.
Sophia M. Charan, Reina S. Buenconsejo, and John H. Seinfeld
Atmos. Chem. Phys., 20, 13167–13190,Short summary
In urban areas, the emissions from volatile chemical products may be responsible for the formation of as much particulate matter as motor vehicles. Since exposure to particulate matter is a public health crisis, understanding its formation is critical. In this work, we investigate the secondary organic aerosol formation potential of benzyl alcohol, an important compound that is representative of some of these new emission sources, and find that more particulate matter forms than is expected.
Kasper Kristensen, Louise N. Jensen, Lauriane L. J. Quéléver, Sigurd Christiansen, Bernadette Rosati, Jonas Elm, Ricky Teiwes, Henrik B. Pedersen, Marianne Glasius, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 20, 12549–12567,Short summary
Atmospheric particles are important in relation to human health and the global climate. As the global temperature changes, so may the atmospheric chemistry controlling the formation of particles from reactions of naturally emitted volatile organic compounds (VOCs). In the current work, we show how temperatures influence the formation and chemical composition of atmospheric particles from α-pinene: a biogenic VOC largely emitted in high-latitude environments such as the boreal forests.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821,Short summary
With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction (RF) of •OH among detected radicals, but negatively correlated with the RF of C-centered radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Isabelle Steinke, Naruki Hiranuma, Roger Funk, Kristina Höhler, Nadine Tüllmann, Nsikanabasi Silas Umo, Peter G. Weidler, Ottmar Möhler, and Thomas Leisner
Atmos. Chem. Phys., 20, 11387–11397,Short summary
In this study, we highlight the potential impact of particles from certain terrestrial sources on the formation of ice crystals in clouds. In particular, we focus on biogenic particles consisting of various organic compounds, which makes it very difficult to predict the ice nucleation properties of complex ambient particles. We find that these ambient particles are often more ice active than individual components.
Young-Chul Song, Ariana G. Bé, Scot T. Martin, Franz M. Geiger, Allan K. Bertram, Regan J. Thomson, and Mijung Song
Atmos. Chem. Phys., 20, 11263–11273,Short summary
We report the liquid–liquid phase separation (LLPS) of organic aerosol consisting of α-pinene- and β-caryophyllene-derived ozonolysis products and commercial organic compounds. As compositional complexity increased from one to two organic species, LLPS occurred over a wider range of average O : C values (increasing from 0.44 to 0.67). These results provide further evidence that LLPS is likely frequent in organic aerosol particles in the troposphere, even in the absence of inorganic salt.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Functional group composition of primary and aged aerosols from wood burning and coal combustion sources from chamber experiments are interpreted through compounds present in the fuels and known gas-phase oxidation products. Infrared spectra of aged wood burning in the chamber and ambient biomass burning samples reveal striking similarities, and a new method for identifying burning-impacted samples in monitoring network measurements is presented.
Archit Mehra, Jordan E. Krechmer, Andrew Lambe, Chinmoy Sarkar, Leah Williams, Farzaneh Khalaj, Alex Guenther, John Jayne, Hugh Coe, Douglas Worsnop, Celia Faiola, and Manjula Canagaratna
Atmos. Chem. Phys., 20, 10953–10965,Short summary
Emissions of volatile organic compounds (VOCs) from plants are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Real plant emissions are much more diverse than the few proxies widely used for studies of plant SOA. Here we present the first study of SOA from Californian sage plants and the oxygenated monoterpenes representing their major emissions. We identify SOA products and show the importance of the formation of highly oxygenated organic molecules and oligomers.
Damon M. Smith, Tianqu Cui, Marc N. Fiddler, Rudra P. Pokhrel, Jason D. Surratt, and Solomon Bililign
Atmos. Chem. Phys., 20, 10169–10191,Short summary
Biomass fuels used for domestic purposes in east Africa produce a significant atmospheric burden of aerosols and volatile organic compounds. The chemical properties and composition of these aerosols have not been investigated in the laboratory. In this work methanol extracts from filter samples of aerosol collected from an indoor smog chamber were analyzed to determine the chemical composition and identify the light absorption properties of organic aerosol constituents.
Iida Pullinen, Sebastian Schmitt, Sungah Kang, Mehrnaz Sarrafzadeh, Patrick Schlag, Stefanie Andres, Einhard Kleist, Thomas F. Mentel, Franz Rohrer, Monika Springer, Ralf Tillmann, Jürgen Wildt, Cheng Wu, Defeng Zhao, Andreas Wahner, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 20, 10125–10147,Short summary
Biogenic and anthropogenic air masses mix in the atmosphere, bringing plant-emitted monoterpenes and traffic-related nitrogen oxides together. There is debate whether the presence of nitrogen oxides reduces or increases secondary aerosol formation. This is important as secondary aerosols have cooling effects in the climate system but also constitute a health risk in populated areas. We show that the presence of NOx alone should not much affect the mass yields of secondary organic aerosols.
Archit Mehra, Yuwei Wang, Jordan E. Krechmer, Andrew Lambe, Francesca Majluf, Melissa A. Morris, Michael Priestley, Thomas J. Bannan, Daniel J. Bryant, Kelly L. Pereira, Jacqueline F. Hamilton, Andrew R. Rickard, Mike J. Newland, Harald Stark, Philip Croteau, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, Lin Wang, and Hugh Coe
Atmos. Chem. Phys., 20, 9783–9803,Short summary
Aromatic volatile organic compounds (VOCs) emitted from anthropogenic activity are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Here we present a detailed chemical characterisation of SOA from four C9-aromatic isomers and a polycyclic aromatic hydrocarbon (PAH). We identify and compare their oxidation products in the gas and particle phases, showing the different relative importance of oxidation pathways and proportions of highly oxygenated organic molecules.
David O. De Haan, Lelia N. Hawkins, Kevin Jansen, Hannah G. Welsh, Raunak Pednekar, Alexia de Loera, Natalie G. Jimenez, Margaret A. Tolbert, Mathieu Cazaunau, Aline Gratien, Antonin Bergé, Edouard Pangui, Paola Formenti, and Jean-François Doussin
Atmos. Chem. Phys., 20, 9581–9590,Short summary
When exposed to glyoxal in chamber experiments, dry ammonium or methylammonium sulfate particles turn brown immediately and reversibly without increasing in size. Much less browning was observed on wet aerosol particles, and no browning was observed with sodium sulfate aerosol. While estimated dry aerosol light absorption caused by background glyoxal (70 ppt) is insignificant compared to that of secondary brown carbon overall, in polluted regions this process could be a source of brown carbon.
Yuwei Wang, Archit Mehra, Jordan E. Krechmer, Gan Yang, Xiaoyu Hu, Yiqun Lu, Andrew Lambe, Manjula Canagaratna, Jianmin Chen, Douglas Worsnop, Hugh Coe, and Lin Wang
Atmos. Chem. Phys., 20, 9563–9579,Short summary
A series of OH-initiated oxidation experiments of trimethylbenzene were investigated in the absence and presence of NOx. Many C9 products with 1–11 oxygen atoms and C18 products presumably formed from dimerization of C9 peroxy radicals were observed, hinting at the extensive existence of autoxidation and accretion reaction pathways. The presence of NOx would suppress the formation of highly oxygenated C18 molecules and enhance the formation of organonitrates and even dinitrate compounds.
Christopher D. Cappa, Christopher Y. Lim, David H. Hagan, Matthew Coggon, Abigail Koss, Kanako Sekimoto, Joost de Gouw, Timothy B. Onasch, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 8511–8532,Short summary
Smoke from combustion of a wide range of biomass fuels (e.g., leaves, twigs, logs, peat, and dung) was photochemically aged in a small chamber for up to 8 d of equivalent atmospheric aging. Upon aging, the particle chemical composition and ability to absorb sunlight changed owing to reactions in both the gas and particulate phases. We developed a model to explain the observations and used this to derive insights into the aging of smoke in the atmosphere.
Petroc D. Shelley, Thomas J. Bannan, Stephen D. Worrall, M. Rami Alfarra, Ulrich K. Krieger, Carl J. Percival, Arthur Garforth, and David Topping
Atmos. Chem. Phys., 20, 8293–8314,Short summary
The methods used to estimate the vapour pressures of compounds in the atmosphere typically perform poorly when applied to organic compounds found in the atmosphere. New measurements have been made and compared to previous experimental data and estimated values so that the limitations within the estimation methods can be identified and in the future be rectified.
Deep Sengupta, Vera Samburova, Chiranjivi Bhattarai, Adam C. Watts, Hans Moosmüller, and Andrey Y. Khlystov
Atmos. Chem. Phys., 20, 8227–8250,Short summary
This paper presents important results on the atmospheric chemistry of combustion emissions. Organic compounds from these emissions can contribute significantly to chemical and physical properties of atmospheric aerosols. In this paper, a detailed chemical analysis of gas- and particle-phase polar organic compounds from the laboratory combustion of globally important fuels is presented. The aging experiments were performed to understand the fate of biomass-burning organics in the atmosphere.
Junling Li, Weigang Wang, Kun Li, Wenyu Zhang, Chao Peng, Li Zhou, Bo Shi, Yan Chen, Mingyuan Liu, Hong Li, and Maofa Ge
Atmos. Chem. Phys., 20, 8123–8137,Short summary
Long-chain alkanes (a large fraction of diesel fuel and its exhaust) are important potential contributors of SOA. Through the analysis of the components of formed SOA, we found that low-temperature conditions promote the oligomerization of n-dodecane, and the degree of oligomerization can reach tetramerization. The presence of the oligomers enhances the light extinction of the particles. UV-scattering particles in the boundary layer can accelerate photochemical reactions and haze production.
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Fuzzi, S., Baltensperger, U., Carslaw, K., Decesari, S., Denier van der Gon, H., Facchini, M. C., Fowler, D., Koren, I., Langford, B., Lohmann, U., Nemitz, E., Pandis, S., Riipinen, I., Rudich, Y., Schaap, M., Slowik, J. G., Spracklen, D. V., Vignati, E., Wild, M., Williams, M., and Gilardoni, S.: Particulate matter, air quality and climate: lessons learned and future needs, Atmos. Chem. Phys., 15, 8217–8299, https://doi.org/10.5194/acp-15-8217-2015, 2015.
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Han, Y., Gong, Z., Liu, P., de Sá, S. S., McKinney, K. A., and Martin, S. T.: Influence of Particle Surface Area Concentration on the Production of Organic Particulate Matter in a Continuously Mixed Flow Reactor, Environ. Sci. Technol., 53, 4968–4976, https://doi.org/10.1021/acs.est.8b07302, 2019.
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The promotion effects of SO2 and NH3 on particle and organosulfur compound formation from 1,2,4-trimethylbenzene (TMB) photooxidation were observed for the first time. The enhanced organosulfur compounds included hitherto unidentified aromatic sulfonates and organosulfates (OSs). OSs were produced via acid-driven heterogeneous chemistry of hydroperoxides. The production of organosulfur compounds might provide a new pathway for the fate of TMB in regions with considerable SO2 emissions.
The promotion effects of SO2 and NH3 on particle and organosulfur compound formation from...