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Atmosphere
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New Insights into Secondary Organic Aerosol Formation
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New Insights into Secondary Organic Aerosol Formation

A special issue of Atmosphere (ISSN 2073-4433). This special issue belongs to the section "Aerosols".

Deadline for manuscript submissions: closed (25 November 2022) | Viewed by 12848

Special Issue Editors

Dr. Xiao Sui

E-Mail Website
Guest Editor
College of Geography and Environment, Shandong Normal University, Jinan 250358, China
Interests: atmospheric chemistry laboratory simulation; secondary aerosol formation; air quality
Special Issues, Collections and Topics in MDPI journals
Prof. Houfeng Liu

E-Mail Website
Guest Editor
Center for Environmental Technology and Policy, Shandong Normal University, Jinan 250113, China
Interests: meteorology; influence of geography on environment; air quality; environmental management

Special Issue Information

Dear Colleagues,

The formation of secondary organic aerosols (SOAs) is recognized as a main source of earth atmospheric compositional change due to industrialization in recent human history, and these compounds directly affect global climate, human health, and the environment. However, great uncertainty surrounding SOA formation still exists because the contributing factors are very complicated, i.e., precursor, meteorological condition, regional terrain, and atmospheric chemistry pathways, which also create difficulties with model simulation and enviromental management. In recognition of this, the open-access journal Atmosphere is hosting a Special Issue to exhibit frontier research related to SOAs and their formation mechanisms. This Special Issue aims to provide new insights into SOA formation and its effect on air pollution. Topics of interest for this Special Issue include, but are not limited to:

  • Laboratory simulation of SOA formation mechanisms;
  • Atmospheric observations showing atomspheric chemistry processes related to SOA formation;
  • The atmospheric physics process of SOA formation, i.e., meteorological condition and terrain;
  • Environmental management of SOA formation control;
  • Models and review papers.

Dr. Xiao Sui
Prof. Houfeng Liu
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Atmosphere is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2400 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

•    Secondary organic aerosol formation
•    Laboratory simulation
•    Air quality
•    PM2.5 and VOCs
•    Pollution mechanism
•    Environmental management

Published Papers (6 papers)

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Research

13 pages, 2141 KiB  
Article
Relative Humidity Impact on Organic New Particle Formation from Ozonolysis of α- and β-Pinene at Atmospherically Relevant Mixing Ratios
by Christopher N. Snyder, Austin C. Flueckiger and Giuseppe A. Petrucci
Atmosphere 2023, 14(1), 173; https://doi.org/10.3390/atmos14010173 - 13 Jan 2023
Cited by 2 | Viewed by 1681
Abstract
The impact of relative humidity (RH) on organic new particle formation (NPF) from ozonolysis of monoterpenes remains an area of active debate. Previous reports provide contradictory results indicating both depression and enhancement of NPF under conditions of moderate RH, while others do not [...] Read more.
The impact of relative humidity (RH) on organic new particle formation (NPF) from ozonolysis of monoterpenes remains an area of active debate. Previous reports provide contradictory results indicating both depression and enhancement of NPF under conditions of moderate RH, while others do not indicate a potential impact. Only several reports have suggested that the effect may depend on absolute mixing ratio of the precursor volatile organic compound (VOC, ppbv). Herein we report on the impact of RH on NPF from dark ozonolysis of α- and β-pinene at mixing ratios ranging from 0.2 to 80 ppbv. We show that RH enhances NPF (by a factor of eight) at the lowest α-pinene mixing ratio, with a very strong dependence on α-pinene mixing ratio from 4 to 22 ppbv. At higher mixing ratios, the effect of RH plateaus, with resulting modest decreases in NPF. In the case of α- and β-pinene, NPF is enhanced at low mixing ratios due to a combination of chemistry, accelerated kinetics, and reduced partitioning of semi-volatile oxidation products to the particulate phase. Reduced partitioning would limit particle growth, permitting increased gas-phase concentrations of semi- and low-volatility products, which could favor NPF. Full article
(This article belongs to the Special Issue New Insights into Secondary Organic Aerosol Formation)
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13 pages, 2619 KiB  
Article
HONO Formation from the Oxidation Reactions of ClO, NO, and Water in the Gas-Phase and at the Air-Water Interface
by Qi Zhang, Mohammad Hassan Hadizadeh, Xiaotong Wang, Xianwei Zhao, Xurong Bai, Fei Xu and Yanhui Sun
Atmosphere 2023, 14(1), 30; https://doi.org/10.3390/atmos14010030 - 24 Dec 2022
Cited by 1 | Viewed by 1761
Abstract
Nitrous acid (HONO) plays a key role in atmospheric chemistry. Nevertheless, the HONO formation mechanism in the atmosphere, especially in the marine boundary layer, remains to be fully understood. Here, Born–Oppenheimer molecular dynamic and metadynamics simulations were performed to study the formation mechanism [...] Read more.
Nitrous acid (HONO) plays a key role in atmospheric chemistry. Nevertheless, the HONO formation mechanism in the atmosphere, especially in the marine boundary layer, remains to be fully understood. Here, Born–Oppenheimer molecular dynamic and metadynamics simulations were performed to study the formation mechanism of HONO from the oxidation reactions of ClO radical and NO with the addition of (H2O)1–2, considering a monohydrated system ((ClO)(NO)(H2O)1) and dihydrated system ((ClO)(NO)(H2O)2), as well as at the air-water interface. This study shows that HONO formation follows a single-water mechanism in gas-phase and air-water interface systems. The free-energy barrier of the (ClO)(NO)(H2O)1 system was 9.66 kJ mol−1, whereas the (ClO)(NO)(H2O)2 system was a barrierless reaction. HONO formation at the air-water interface was faster than that in monohydrated and dihydrated systems. Although the concentration of ClO radical in the marine boundary layer is two orders higher than that of Cl radical, the production rates of HONO from the (ClO)(NO)(H2O)1 system are six orders lower than that from the (Cl)(NO)(H2O)1 system, which means that Cl radical dominates HONO formation rather than ClO radical in the marine boundary layer. These results can deepen our understanding of the HONO formation mechanism and be used to reduce HONO emissions and establish HONO-control strategies. Full article
(This article belongs to the Special Issue New Insights into Secondary Organic Aerosol Formation)
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17 pages, 6367 KiB  
Article
Theoretical Perspectives on the Gas-Phase Oxidation Mechanism and Kinetics of Carbazole Initiated by OH Radical in the Atmosphere
by Zhuochao Teng, Xiaotong Wang, Mohammad Hassan Hadizadeh, Yanan Han, Xianwei Zhao, Qi Zhang, Hetong Wang, Ying Li, Fei Xu and Yanhui Sun
Atmosphere 2022, 13(7), 1129; https://doi.org/10.3390/atmos13071129 - 18 Jul 2022
Cited by 3 | Viewed by 1664
Abstract
Carbazole is one of the typical heterocyclic aromatic compounds (NSO-HETs) observed in polluted urban atmosphere, which has become a serious environmental concern. The most important atmospheric loss process of carbazole is the reaction with OH radical. The present work investigated the mechanism of [...] Read more.
Carbazole is one of the typical heterocyclic aromatic compounds (NSO-HETs) observed in polluted urban atmosphere, which has become a serious environmental concern. The most important atmospheric loss process of carbazole is the reaction with OH radical. The present work investigated the mechanism of OH-initiated atmospheric oxidation degradation of carbazole by using density functional theory (DFT) calculations at the M06-2X/6-311++G(3df,2p)//M06-2X/6-311+G(d,p) level. The rate constants were determined by the Rice–Ramsperger–Kassel–Marcus (RRKM) theory. The lifetime of carbazole determined by OH was compared with other typical NSO-HETs. The theoretical results show that the degradation of carbazole initiated by OH radical includes four types of reactions: OH additions to “bend” C atoms, OH additions to “benzene ring” C atoms, H abstractions from C-H bonds and the H abstraction from N-H bond. The OH addition to C1 atom and the H abstraction from N-H bond are energetically favorable. The main oxidation products are hydroxycarbazole, dialdehyde, carbazolequinone, carbazole-ol, hydroxy-carbazole-one and hydroperoxyl-carbazole-one. The calculated overall rate constant of carbazole oxidation by OH radical is 6.52 × 10−12 cm3 molecule−1 s−1 and the atmospheric lifetime is 37.70 h under the condition of 298 K and 1 atm. The rate constant of carbazole determined by OH radical is similar with that of dibenzothiophene oxidation but lower than those of pyrrole, indole, dibenzofuran and fluorene. This work provides a theoretical investigation of the oxygenated mechanism of NSO-HETs in the atmosphere and should help to clarify their potential health risk for determining the reaction pathways and environmental influence of carbazole. Full article
(This article belongs to the Special Issue New Insights into Secondary Organic Aerosol Formation)
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19 pages, 5006 KiB  
Article
Characterization of Imidazole Compounds in Aqueous Secondary Organic Aerosol Generated from Evaporation of Droplets Containing Pyruvaldehyde and Inorganic Ammonium
by Xin Lin, Mingqiang Huang, Tingting Lu, Weixiong Zhao, Changjin Hu, Xuejun Gu and Weijun Zhang
Atmosphere 2022, 13(6), 970; https://doi.org/10.3390/atmos13060970 - 15 Jun 2022
Cited by 10 | Viewed by 2598
Abstract
Imidazole compounds are important constituents of atmospheric brown carbon. The imidazole components of aqueous secondary organic aerosol (aqSOA) that are generated from the evaporation of droplets containing pyruvaldehyde and inorganic ammonium are on-line characterized by an aerosol laser time-of-flight mass spectrometer (ALTOFMS) and [...] Read more.
Imidazole compounds are important constituents of atmospheric brown carbon. The imidazole components of aqueous secondary organic aerosol (aqSOA) that are generated from the evaporation of droplets containing pyruvaldehyde and inorganic ammonium are on-line characterized by an aerosol laser time-of-flight mass spectrometer (ALTOFMS) and off-line detected by optical spectrometry in this study. The results demonstrated that the laser desorption/ionization mass spectra of aqSOA particles that were detected by ALTOFMS contained the characteristic mass peaks of imidazoles at m/z = 28 (CH2N+), m/z = 41 (C2H3N+) and m/z = 67 (C3H4N2+). Meanwhile, the extraction solution of the aqSOA particles that were measured by off-line techniques showed that the characteristic absorption peaks at 217 nm and 282 nm appeared in the UV-Vis spectrum, and the stretching vibration peaks of C-N bond and C=N bond emerged in the infrared spectrum. Based on these spectral information, 4-methyl-imidazole and 4-methyl-imidazole-2-carboxaldehyde are identified as the main products of the reaction between pyruvaldehyde and ammonium ions. The water evaporation accelerates the formation of imidazoles inside the droplets, possibly owing to the highly concentrated environment. Anions, such as F−, CO32−, NO3−, SO42− and Cl− in the aqueous phase promote the reaction of pyruvaldehyde and ammonium ions to produce imidazole products, resulting in the averaged mass absorption coefficient (<MAC>) in the range of 200–600 nm of aqSOA increases, and the order of promotion is: F− > CO32− > SO42− ≈ NO3− ≈ Cl−. These results will help to analyze the constituents and optics of imidazoles and provide a useful basis for evaluating the formation process and radiative forcing of aqSOA particles. Full article
(This article belongs to the Special Issue New Insights into Secondary Organic Aerosol Formation)
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16 pages, 2004 KiB  
Article
Effect of Water Molecule on the Complete Series Reactions of Chlorothiobenzenes with H/·OH: A Theoretical Study
by Yanan Han, Siyuan Zheng, Zhuochao Teng, Mohammad Hassan Hadizadeh, Qi Zhang, Fei Xu and Yanhui Sun
Atmosphere 2022, 13(5), 849; https://doi.org/10.3390/atmos13050849 - 23 May 2022
Cited by 3 | Viewed by 1402
Abstract
The chlorothiobenzenes (CTBs) are the principal precursors for the formation of polychlorinated thianthrene/dibenzothiophenes (PCTA/DTs), which have high toxicity and wide distribution in the environment. Under the pyrolysis or combustion conditions, CTBs can react with H/·OH radicals to form the chlorothiobenzyl radicals (CTBRs) through [...] Read more.
The chlorothiobenzenes (CTBs) are the principal precursors for the formation of polychlorinated thianthrene/dibenzothiophenes (PCTA/DTs), which have high toxicity and wide distribution in the environment. Under the pyrolysis or combustion conditions, CTBs can react with H/·OH radicals to form the chlorothiobenzyl radicals (CTBRs) through abstraction of the chlorothiobenzyl-hydrogen. The water molecule can play an important role in this process. The coupling of CTBRs is the essential first step in forming PCTA/DTs. In this paper, quantum chemical calculations were carried out to investigate the formation of CTBRs from the complete series reactions of 19 chlorothiobenzene (CTB) congeners with H/·OH radicals in the presence of the water molecule. Using the MPWB1K/6-311 + G(3df,2p)//MPWB1K/6-31 + G(d,p) energy level, schematic energy profiles were constructed with the water molecule and then compared with the non-hydrated case. The present study shows that structural parameters and thermal data, as well as CTBRs formation potential from CTBs, are strongly dominated by the chlorine substitution at the ortho-position of CTBs. Meanwhile, the water molecule can promote the CTBR formation from CTBs abstracted by H/·OH, which has a stronger catalysis effect on the H abstraction from CTBs by OH than from CTBs by H. This study may provide reference parameters for future experimental research, which would enhance measures to reduce dioxin emission and establish dioxin control strategies. Full article
(This article belongs to the Special Issue New Insights into Secondary Organic Aerosol Formation)
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15 pages, 2104 KiB  
Article
Interfacial Dark Aging Is an Overlooked Source of Aqueous Secondary Organic Aerosol
by Fei Zhang, Manh Thuong Nguyen, Yao Fu and Xiao-Ying Yu
Atmosphere 2022, 13(2), 188; https://doi.org/10.3390/atmos13020188 - 24 Jan 2022
Cited by 1 | Viewed by 2756
Abstract
In this work, the relative yields of aqueous secondary organic aerosols (aqSOAs) at the air–liquid (a–l) interface are investigated between photochemical and dark aging using in situ time-of-flight secondary ion mass spectrometry (ToF-SIMS). Our results show that dark aging is an important source [...] Read more.
In this work, the relative yields of aqueous secondary organic aerosols (aqSOAs) at the air–liquid (a–l) interface are investigated between photochemical and dark aging using in situ time-of-flight secondary ion mass spectrometry (ToF-SIMS). Our results show that dark aging is an important source of aqSOAs despite a lack of photochemical drivers. Photochemical reactions of glyoxal and hydroxyl radicals (•OH) produce oligomers and cluster ions at the aqueous surface. Interestingly, different oligomers and cluster ions form intensely in the dark at the a–l interface, contrary to the notion that oligomer formation mainly depends on light irradiation. Furthermore, cluster ions form readily during dark aging and have a higher water molecule adsorption ability. This finding is supported by the observation of more frequent organic water cluster ion formation. The relative yields of water clusters in the form of protonated and hydroxide ions are presented using van Krevelen diagrams to explore the underlying formation mechanisms of aqSOAs. Large protonated and hydroxide water clusters (e.g., (H2O)nH+, 17 < n ≤ 44) have reasonable yields during UV aging. In contrast, small protonated and hydroxide water clusters (e.g., (H2O)nH+, 1 ≤ n ≤ 17) form after several hours of dark aging. Moreover, cluster ions have higher yields in dark aging, indicating the overlooked influence of dark aging interfacial products on aerosol optical properties. Molecular dynamic simulation shows that cluster ions form stably in UV and dark aging. AqSOAs molecules produced from dark and photochemical aging can enhance UV absorption of the aqueous surface, promote cloud condensation nuclei (CCN) activities, and affect radiative forcing. Full article
(This article belongs to the Special Issue New Insights into Secondary Organic Aerosol Formation)
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