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DOI10.1016/j.atmosenv.2021.118541
Role of ecosystem-atmosphere exchanges of semi-volatile organic compounds in organic aerosol formation
Couvidat F.; Bessagnet B.
发表日期2021
ISSN1352-2310
卷号263
英文摘要Deposition of the gas fraction of Semi-Volatile Organic Compounds (SVOC) may be an important removal pathway and may strongly influence concentrations of organic aerosols due to the gas-particle partitioning of SVOC. All the studies on this process are based on the classic Wesely resistance approach that uses Henry's law constants to calculate a deposition rate scaled on the deposition rate of SO2. However, even highly hydrophobic SVOC could be efficiently removed by the vegetation and soils as shown by numerous studies on Persistent Organic Pollutant (POP) modeling. Moreover, the re-volatilization of deposited SVOC is possible and could influence organic aerosol concentrations. An atmosphere-soil-vegetation module was developed and implemented in the 3D air quality model CHIMERE 2017β to represent the accumulation of compounds in the different compartments of the biosphere and the exchanges between them. The soil compartment was represented with a multi-layer approach (the layers corresponding to different in-soil depths) to simulate the multiphase diffusion of compounds inside the soil. Exchanges of SVOC between the air, soil and vegetation compartments were simulated using bi-directional approaches based on Rg (the gas-phase partitioning in the soil compartment) and Kva the vegetation-air partitioning coefficient. Parameters were estimated based on the physical properties of the compounds and their molecular structure. Simulations performed over Europe show that air-vegetation-soil exchanges may be a more efficient removal pathway than dry deposition of particles for SVOC with a gas-phase fraction above 10%. Considering air-vegetation-soil exchanges in the simulations lead to a decrease of organic aerosol concentrations by 15% and primary SVOC (considered as hydrophobic compounds) may be efficiently removed by those pathways (contrary to what is calculated with the Wesely approach). This decrease of concentrations is mainly due to air-vegetation exchanges. During summer, the use of the Wesely approach may lead to a slight overestimation of deposition fluxes (leading to an underestimation of concentration by 1%). Re-volatilization may limit the amount of deposited SVOC. Depending on assumptions, simulations showed that re-emissions (inversion of exchanges toward the emissions) in summer of SVOC accumulated during winter is theoretically possible and may be a minor source of organic aerosol. © 2021 The Author(s)
关键词Air quality modelingDepositionExchangesOrganic aerosol
语种英语
scopus关键词Aerosols; Air quality; Deposition rates; Gases; Hydrophobicity; Organic pollutants; Rate constants; Soils; Vegetation; Aerosol concentration; Air quality modelling; Air-vegetation; Exchange; Gas fraction; Gas-phases; Organic aerosol; Organic aerosol formation; Re-volatilization; Volatile organics; Volatile organic compounds; aerosol formation; air quality; atmosphere-biosphere interaction; concentration (composition); dry deposition; volatile organic compound; Europe
来源期刊ATMOSPHERIC ENVIRONMENT
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/248253
作者单位INERIS, Institut National de l'Environnement Industriel et des Risques, Parc Technologique ALATA, Verneuil-en-Halatte60550, France; Now at European Commission, Joint Research Centre (JRC), Ispra, Italy
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Couvidat F.,Bessagnet B.. Role of ecosystem-atmosphere exchanges of semi-volatile organic compounds in organic aerosol formation[J],2021,263.
APA Couvidat F.,&Bessagnet B..(2021).Role of ecosystem-atmosphere exchanges of semi-volatile organic compounds in organic aerosol formation.ATMOSPHERIC ENVIRONMENT,263.
MLA Couvidat F.,et al."Role of ecosystem-atmosphere exchanges of semi-volatile organic compounds in organic aerosol formation".ATMOSPHERIC ENVIRONMENT 263(2021).
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