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Role of ecosystem-atmosphere exchanges of semi-volatile organic compounds in organic aerosol formation
Atmospheric Environment ( IF 5 ) Pub Date : 2021-06-22 , DOI: 10.1016/j.atmosenv.2021.118541
Florian Couvidat , Bertrand Bessagnet

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.



中文翻译:

半挥发性有机化合物的生态系统-大气交换在有机气溶胶形成中的作用

半挥发性有机化合物 (SVOC) 的气体部分的沉积可能是重要的去除途径,并且由于 SVOC 的气体-颗粒分配,可能会强烈影响有机气溶胶的浓度。该过程的所有研究均基于经典的 Wesely 电阻方法,该方法使用亨利定律常数来计算与 SO 2沉积速率成比例的沉积速率。然而,如对持久性有机污染物 (POP) 建模的大量研究表明,即使是高度疏水的 SVOC 也可以被植被和土壤有效去除。此外,沉积的 SVOC 可能会重新挥发,并可能影响有机气溶胶浓度。

在 3D 空气质量模型 CHIMERE 2017 β中开发并实施了大气-土壤-植被模块,以表示生物圈不同区域中化合物的积累以及它们之间的交换。土壤隔间用多层方法(对应于不同土壤深度的层)表示,以模拟土壤内部化合物的多相扩散。空气、土壤和植被隔间之间的 SVOC 交换使用基于 R g(土壤隔间中的气相分配)和 K va植被-空气分配系数的双向方法进行模拟。基于化合物的物理性质及其分子结构估计参数。

在欧洲进行的模拟表明,对于气相分数高于 10% 的 SVOC,空气-植被-土壤交换可能是比颗粒干沉积更有效的去除途径。考虑到模拟中的空气-植被-土壤交换导致有机气溶胶浓度降低 15%,并且主要 SVOC(被视为疏水化合物)可以通过这些途径有效去除(与 Wesely 方法计算的结果相反)。浓度的降低主要是由于空气-植被交换。在夏季,使用 Wesely 方法可能会导致对沉积通量的轻微高估(导致浓度低估 1%)。

再挥发可能会限制沉积的 SVOC 的数量。根据假设,模拟表明冬季积累的 SVOC 在夏季重新排放(交换向排放的转化)在理论上是可能的,并且可能是有机气溶胶的次要来源。

更新日期:2021-08-16
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