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Influence of seed aerosol surface area and oxidation rate on vapor walldeposition and SOA mass yields: a case study with α-pineneozonolysis

机译:种子气溶胶表面积和氧化率对蒸汽壁料和SOA质量产量的影响:一种α-泛喹唑溶分的案例研究

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Laboratory chambers, invaluable in atmospheric chemistry and aerosol formation studies, are subject to particle and vapor wall deposition, processes that need to be accounted for in order to accurately determine secondary organic aerosol (SOA) mass yields. Although particle wall deposition is reasonably well understood and usually accounted for, vapor wall deposition is less so. The effects of vapor wall deposition on SOA mass yields in chamber experiments can be constrained experimentally by increasing the seed aerosol surface area to promote the preferential condensation of SOA-forming vapors onto seed aerosol. Here, we study the influence of seed aerosol surface area and oxidation rate on SOA formation in α-pinene ozonolysis. The observations are analyzed using a coupled vapor–particle dynamics model to interpret the roles of gas–particle partitioning (quasi-equilibrium vs. kinetically limited SOA growth) and α-pinene oxidation rate in influencing vapor wall deposition. We find that the SOA growth rate and mass yields are independent of seed surface area within the range of seed surface area concentrations used in this study. This behavior arises when the condensation of SOA-forming vapors is dominated by quasi-equilibrium growth. Faster α-pinene oxidation rates and higher SOA mass yields are observed at increasing O3 concentrations for the same initial α-pinene concentration. When the α-pinene oxidation rate increases relative to vapor wall deposition, rapidly produced SOA-forming oxidation products condense more readily onto seed aerosol particles, resulting in higher SOA mass yields. Our results indicate that the extent to which vapor wall deposition affects SOA mass yields depends on the particular volatility organic compound system and can be mitigated through the use of excess oxidant concentrations.
机译:实验室室,在大气化学和气溶胶形成研究中无价值,受到颗粒和蒸气壁沉积的影响,需要考虑的方法,以便准确地确定二次有机气溶胶(SOA)质量产量。尽管粒子壁沉积合理地理解并且通常占,但蒸汽壁沉积较小。蒸汽壁沉积对腔室实验中的SOA质量产量的影响可以通过增加种子气溶胶表面积来实验地限制,以促进SOA形成蒸汽在种子气溶胶上的优先缩合。在此,我们研究种子气溶胶表面积和氧化率对α-叉烯臭氧溶解的SOA形成的影响。使用耦合的蒸汽粒子动力学模型分析观察结果,以解释气体颗粒分配的作用(准平衡与动力学上有限的SOA生长)和α-针烯氧化率在影响蒸汽壁沉积时。我们发现SOA生长速率和质量产量与本研究中使用的种子表面区域浓度范围内的种子表面积无关。当形成成型蒸气的冷凝以准平衡生长支配时,产生这种行为。在增加初始α-叉烯浓度的情况下,观察到更快的α-焦烯氧化速率和更高的SOA质量产量。当α-PineNe氧化速率相对于蒸汽壁沉积增加时,快速生产的SOA形成氧化产物浓缩在种子气溶胶颗粒上,导致较高的SOA质量产量。我们的结果表明,蒸汽壁沉积影响SOA质量产量的程度取决于特定的挥发性有机化合物体系,可以通过使用过量的氧化剂浓度来减轻。

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