Aerosol high water contents favor sulfate and secondary organic aerosol formation from fossil fuel combustion emissions DOI Creative Commons
Huang Xiao-juan, Zhe Liu,

Yanzhen Ge

et al.

npj Climate and Atmospheric Science, Journal Year: 2023, Volume and Issue: 6(1)

Published: Oct. 27, 2023

Abstract Fine-particle pollution associated with high sulfate and secondary organic aerosol (SOA) contents still occurs in winter, despite considerable reductions precursor emissions China. The chemical mechanisms involved are consistently acknowledged to be linked water but remain poorly understood. Here, we present findings demonstrating that the synergistic effect of elevated content particles originating from fossil fuel combustion significantly enhanced rapid formation SOAs under humidity conditions during winter northern presence promoted aging process containing elemental carbon (EC) facilitated SOAs. Evidence single reveals an increased potential for SOA primary aerosols (POAs) combustion, increasing water. Under relative exceeding 85%, multiphase oxidation SO 2 by in-particle nitrite/nitrous acid, generated through reactions involving aged EC-containing iron-rich particles, as well aqueous-phase hydroxymethanesulfonate (HMS), led a substantial increase production. This study emphasizes critical role chemistry concerning SOAs, highlighting urgent necessity mitigate combustion.

Language: Английский

Organic Peroxides in Aerosol: Key Reactive Intermediates for Multiphase Processes in the Atmosphere DOI

Shunyao Wang,

Yue Zhao, Arthur W. H. Chan

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(4), P. 1635 - 1679

Published: Jan. 11, 2023

Organic peroxides (POs) are organic molecules with one or more peroxide (−O–O−) functional groups. POs commonly regarded as chemically labile termination products from gas-phase radical chemistry and therefore serve temporary reservoirs for oxidative radicals (HOx ROx) in the atmosphere. Owing to their ubiquity, active gas-particle partitioning behavior, reactivity, key reactive intermediates atmospheric multiphase processes determining life cycle (formation, growth, aging), climate, health impacts of aerosol. However, there remain substantial gaps origin, molecular diversity, fate due complex nature dynamic behavior. Here, we summarize current understanding on POs, a focus identification quantification, state-of-the-art analytical developments, molecular-level formation mechanisms, chemical transformation pathways, well environmental impacts. We find that interactions SO2 transition metal ions generally fast PO pathways liquid water, lifetimes estimated be minutes hours, while hydrolysis is particularly important α-substituted hydroperoxides. Meanwhile, photolysis thermolysis likely minor sinks POs. These distinctly different fates, such reaction OH radicals, which highlights need understand By summarizing advances remaining challenges investigation propose future research priorities regarding fate,

Language: Английский

Citations

95
Imaging of pH distribution inside individual microdroplet by stimulated Raman microscopy DOI Creative Commons
Kedong Gong, Jianpeng Ao, Kejian Li

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(20)

Published: May 8, 2023

Aerosol microdroplets as microreactors for many important atmospheric reactions are ubiquitous in the atmosphere. pH largely regulates chemical processes within them; however, how and species spatially distribute an microdroplet is still under intense debate. The challenge to measure distribution a tiny volume without affecting distribution. We demonstrate method based on stimulated Raman scattering microscopy visualize three-dimensional inside single of varying sizes. find that surface all more acidic, monotonic trend decreasing observed 2.9-μm aerosol from center edge, which well supported by molecular dynamics simulation. However, bigger cloud differs small This size-dependent can be related surface-to-volume ratio. work presents noncontact measurement imaging microdroplets, filling gap our understanding spatial aerosol.

Language: Английский

Citations

45
Washable and flexible gas sensor based on UiO-66-NH2 nanofibers membrane for highly detecting SO2 DOI
Zhenyu Zhai, Xiuling Zhang,

Jiaona Wang

et al.

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 428, P. 131720 - 131720

Published: Aug. 10, 2021

Language: Английский

Citations

78
A critical review of sulfate aerosol formation mechanisms during winter polluted periods DOI Open Access
Can Ye,

Keding Lu,

Huan Song

et al.

Journal of Environmental Sciences, Journal Year: 2022, Volume and Issue: 123, P. 387 - 399

Published: July 16, 2022

Language: Английский

Citations

52
Sulfate Formation Apportionment during Winter Haze Events in North China DOI
Tiantian Wang, Mingxu Liu, Mingyuan Liu

et al.

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(12), P. 7771 - 7778

Published: May 24, 2022

There is a large gap between the simulated and observed sulfate concentrations during winter haze events in North China. Although multiphase formation mechanisms have been proposed, they not evaluated using chemical transport models. In this study, Weather Research Forecasting model coupled with Chemistry (WRF-Chem) was used to apportion formation. It found that Mn-catalyzed oxidation on aerosol surfaces dominant pathway, accounting for 92.3 ± 3.5% of events. Gas-phase contributed 3.1 0.5% due low OH levels. The H2O2 water accounted 4.2 3.6% formation, caused by rapid consumption H2O2. contributions O3, NO2 oxidation, transition metal ion-catalyzed reactions could be negligible owing content, pH, high ionic strength. from in-cloud were barrier provided stable stratification

Language: Английский

Citations

49
Single-particle Raman spectroscopy for studying physical and chemical processes of atmospheric particles DOI Creative Commons
Zhancong Liang, Yangxi Chu, Masao Gen

et al.

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(5), P. 3017 - 3044

Published: March 7, 2022

Abstract. Atmospheric particles experience various physical and chemical processes change their properties during lifetime. Most studies on atmospheric particles, both in laboratory field measurements, rely analyzing an ensemble of particles. Because different mixing states individual only average can be obtained from using ensembles To better understand the fate environmental impacts investigations at a single-particle level are valuable. Among wealth analytic techniques, Raman spectroscopy provides unambiguous characterization under pressure non-destructive situ manner. This paper comprehensively reviews application such technique including particle hygroscopicity, phase transition separation, solute–water interactions, pH, multiphase reactions. Investigations enhanced bioaerosols basis also reviewed. For each application, we describe principle representative examples studies. Finally, present our views future directions development further applications studying

Language: Английский

Citations

47
Sulfate Formation in Incense Burning Particles: A Single-Particle Mass Spectrometric Study DOI
Zhancong Liang, Liyuan Zhou, Rosemarie Ann Infante Cuevas

et al.

Environmental Science & Technology Letters, Journal Year: 2022, Volume and Issue: 9(9), P. 718 - 725

Published: Aug. 26, 2022

Incense burning is a common ritual in Asian communities, and it emits massive amounts of particles. These particles can undergo atmospheric aging upon exposure to sunlight other pollutants. In this work, we observed sulfate formation fresh incense SO2, using single-particle aerosol mass spectrometer (SPAMS). Analysis the positive spectra classified as K-type OC-type. both dark light experiments, SO2 uptake oxidation were found preferentially OC-type over Sulfate formation, represented by number fraction sulfate-containing (FS), under was likely due gaseous oxidants. FS increased with UV, mainly attributable photosensitization reactions. While more formed at higher relative humidity (RH) dark, independent RH. The increase photochemistry effective lower RH, where photoactive compounds concentrated generated photo-oxidants. This effect outweighed that reduced dissolution. Since contain organic photosensitizers have also been biomass particles, our findings could shed on potential trigger formation.

Language: Английский

Citations

47
Targeting Atmospheric Oxidants Can Better Reduce Sulfate Aerosol in China: H2O2 Aqueous Oxidation Pathway Dominates Sulfate Formation in Haze DOI
Jie Gao, Guoliang Shi, Zhongcheng Zhang

et al.

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(15), P. 10608 - 10618

Published: July 5, 2022

Particulate sulfate is one of the most important components in atmosphere. The observation rapid aerosol production during haze events provoked scientific interest multiphase oxidation SO2 aqueous particles. Diverse pathways can be enhanced or suppressed under different acidity levels and high ionic strength conditions atmospheric aerosol. importance to chemistry has been verified laboratory conditions, though studies actual atmosphere are still limited. By utilizing online observations developing an improved solute strength-dependent chemical thermodynamics kinetics model (EF-T&K model, EF enhancement factor that represents effect on aqueous-phase reaction), we provided quantitative evidence H2O2 pathway was nearly 100 times dominated formation for entire years (66%) Tianjin (a northern city China). TMI (oxygen catalyzed by transition-metal ions) (14%) NO2 got second-highest contributions. Machine learning supported result more affected pathway. collaborative effects oxidants were further investigated using EF-T&K model. Our findings highlight effectiveness adopting target oxidant control as a new direction sustainable mitigation sulfate, given already low concentrations China.

Language: Английский

Citations

44
Rapid Sulfate Formation via Uncatalyzed Autoxidation of Sulfur Dioxide in Aerosol Microdroplets DOI

Zhe Chen,

Pai Liu, Weigang Wang

et al.

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(12), P. 7637 - 7646

Published: May 31, 2022

Severe winter haze events in Beijing and North China Plain are characterized by rapid production of sulfate aerosols with unresolved mechanisms. Oxidation SO2 O2 the absence metal catalysts (uncatalyzed autoxidation) represents most ubiquitous conversion pathway atmosphere. However, this reaction has long been regarded as too slow to be atmospherically meaningful. This traditional view was based on kinetic studies conducted bulk dilute solutions that mimic cloudwater but deviate from urban aerosols. Here, we directly measure formation rate via uncatalyzed autoxidation single (NH4)2SO4 microdroplets, using an aerosol optical tweezer coupled a cavity-enhanced Raman spectroscopy technique. We find aqueous is accelerated two orders magnitude at high ionic strength (∼36 molal) conditions supersaturated water. Furthermore, acidic (pH 3.5–4.5), predominately occurs droplet surface, unconstrained solubility. With these enhancements, estimate can produce up 0.20 μg m–3 hr–1, under air pollution condition Beijing.

Language: Английский

Citations

40
Significant formation of sulfate aerosols contributed by the heterogeneous drivers of dust surface DOI Creative Commons
Tao Wang, Yangyang Liu,

Hanyun Cheng

et al.

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(20), P. 13467 - 13493

Published: Oct. 19, 2022

Abstract. The importance of dust heterogeneous oxidation in the removal atmospheric SO2 and formation sulfate aerosols is not adequately understood. In this study, Fe-, Ti-, Al-bearing components, Na+, Cl−, K+, Ca2+ surface, were discovered to be closely associated with sulfate. Regression models then developed make a reliable prediction reactivity based on particle chemical compositions. Further, recognized gas-phase, aqueous-phase, routes quantitatively assessed kinetically compared by combining laboratory work modelling study. presence 55 µg m−3 airborne dust, accounts for approximately 28.6 % secondary during nighttime, while proportion decreases 13.1 solar irradiation. On drivers (e.g. transition metal constituents, water-soluble ions) are more efficient than surface-adsorbed oxidants H2O2, NO2, O3) conversion SO2, particularly nighttime. Dust offers an opportunity explain missing source severe haze pollution events, its contribution complex environments could even higher current calculation results. Overall, surface responsible significant have profound impacts sulfur cycling.

Language: Английский

Citations

40