气候变化领域集成服务门户(CCPortal): Role of Criegee intermediates in the formation of sulfuric acid at a Mediterranean (Cape Corsica) site under influence of biogenic emissions

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DOI	10.5194/acp-21-13333-2021
	Role of Criegee intermediates in the formation of sulfuric acid at a Mediterranean (Cape Corsica) site under influence of biogenic emissions
	Kukui A.; Chartier M.; Wang J.; Chen H.; Dusanter S.; Sauvage S.; Michoud V.; Locoge N.; Gros V.; Bourrianne T.; Sellegri K.; Pichon J.-M.
发表日期	2021
ISSN	1680-7316
起始页码	13333
结束页码	13351
卷号	21 期号:17
英文摘要	Reaction of stabilized Criegee intermediates (SCIs) with SO2 was proposed as an additional pathway of gaseous sulfuric acid (H2SO4) formation in the atmosphere, supplementary to the conventional mechanism of H2SO4 production by oxidation of SO2 in reaction with OH radicals. However, because of a large uncertainty in mechanism and rate coefficients for the atmospheric formation and loss reactions of different SCIs, the importance of this additional source is not well established. In this work, we present an estimation of the role of SCIs in H2SO4 formation at a western Mediterranean (Cape Corsica) remote site, where comprehensive field observations including gas-phase H2SO4, OH radicals, SO2, volatile organic compounds (VOCs) and aerosol size distribution measurements were performed in July-August 2013 as a part of the project ChArMEx (Chemistry-Aerosols Mediterranean Experiment). The measurement site was under strong influence of local emissions of biogenic volatile organic compounds, including monoterpenes and isoprene generating SCIs in reactions with ozone, and, hence, presenting an additional source of H2SO4 via SO2 oxidation by the SCIs. Assuming the validity of a steady state between H2SO4 production and its loss by condensation on existing aerosol particles with a unity accommodation coefficient, about 90g% of the H2SO4 formation during the day could be explained by the reaction of SO2 with OH. During the night the oxidation of SO2 by OH radicals was found to contribute only about 10g% to the H2SO4 formation. The accuracy of the derived values for the contribution of OHg+gSO2 reaction to the H2SO4 formation is limited mostly by a large, at present factor of 2, uncertainty in the OHg+gSO2 reaction rate coefficient. The contribution of the SO2 oxidation by SCIs to the H2SO4 formation was evaluated using available measurements of unsaturated VOCs and steady-state SCI concentrations estimated by adopting rate coefficients for SCI reactions based on structure-activity relationships (SARs). The estimated concentration of the sum of SCIs was in the range of (1-3)g×g103gmolec.gcm-3. During the day the reaction of SCIs with SO2 was found to account for about 10g% and during the night for about 40g% of the H2SO4 production, closing the H2SO4 budget during the day but leaving unexplained about 50g% of the H2SO4 formation during the night. Despite large uncertainties in used kinetic parameters, these results indicate that the SO2 oxidation by SCIs may represent an important H2SO4 source in VOC-rich environments, especially during nighttime. © Copyright:
语种	英语
scopus关键词	accuracy assessment; aerosol composition; aerosol formation; biogenic emission; carbon emission; hydroxyl radical; oxidation; parameter estimation; volatile organic compound; Corse; France; Mediterranean Region
来源期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/246595
作者单位	Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), CNRS, Orleans, France; Resources and Environment Innovation Research Institute, School of Municipal and Environmental Engineering, Shandong Jianzhu University, Jinan, 250101, China; ICARE-CNRS, 1 C Av. de la Recherche Scientifique, Orleans CEDEX 2, 45071, France; IMT Lille Douai, Institut Mines-Telecom, Univ. Lille, Centre for Energy and Environment, Lille, 59000, France; Laboratoire des Sciences du Climat et de l'Environnement (LSCE), UMR CNRS-CEA-UVSQ, IPSL, Univ. Paris-Saclay, Gif-sur-Yvette, 91191, France; Centre National de Recherches Meteorologiques (CNRM), GMEI, MNP, Meteo-France, Toulouse, 31057, France; Laboratoire de Meteorologie Physique Observatoire de Physique du Globe (LAMP), Clermont-Ferrand, France; Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Institute of Atmospheric Sciences, Fudan University, Shanghai, 200438, China; Laboratoire I...
推荐引用方式 GB/T 7714	Kukui A.,Chartier M.,Wang J.,et al. Role of Criegee intermediates in the formation of sulfuric acid at a Mediterranean (Cape Corsica) site under influence of biogenic emissions[J],2021,21(17).
APA	Kukui A..,Chartier M..,Wang J..,Chen H..,Dusanter S..,...&Pichon J.-M..(2021).Role of Criegee intermediates in the formation of sulfuric acid at a Mediterranean (Cape Corsica) site under influence of biogenic emissions.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(17).
MLA	Kukui A.,et al."Role of Criegee intermediates in the formation of sulfuric acid at a Mediterranean (Cape Corsica) site under influence of biogenic emissions".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.17(2021).