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An efficient approach for treating composition-dependent diffusion within organic particles

机译:一种治疗有机颗粒内组成依赖性扩散的有效方法

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Mounting evidence demonstrates that under certain conditions the rate of component partitioning between the gas and particle phase in atmospheric organic aerosol is limited by particle-phase diffusion. To date, however, particle-phase diffusion has not been incorporated into regional atmospheric models. An analytical rather than numerical solution to diffusion through organic particulate matter is desirable because of its comparatively small computational expense in regional models. Current analytical models assume diffusion to be independent of composition and therefore use a constant diffusion coefficient. To realistically model diffusion, however, it should be composition-dependent (e.g. due to the partitioning of components that plasticise, vitrify or solidify). This study assesses the modelling capability of an analytical solution to diffusion corrected to account for composition dependence against a numerical solution. Results show reasonable agreement when the gas-phase saturation ratio of a partitioning component is constant and particle-phase diffusion limits partitioning rate (???10?% discrepancy in estimated radius change). However, when the saturation ratio of the partitioning component varies, a generally applicable correction cannot be found, indicating that existing methodologies are incapable of deriving a general solution. Until such time as a general solution is found, caution should be given to sensitivity studies that assume constant diffusivity. The correction was implemented in the polydisperse, multi-process Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) and is used to illustrate how the evolution of number size distribution may be accelerated by condensation of a plasticising component onto viscous organic particles.
机译:安装证据表明,在某些条件下,大气有机气溶胶中的气体和颗粒相之间的组分分配速率受到粒子相扩散的限制。然而,迄今为止,颗粒相扩散尚未纳入区域大气模型中。由于其在区域模型中的计算费用相对小,可以通过有机颗粒物扩散的分析而不是数值溶液。目前的分析模型假设扩散与组合物无关,因此使用恒定的扩散系数。然而,为了实际模型扩散,它应该是依赖性的(例如,由于塑料,玻璃化或固化的组分分配)。该研究评估了分析解决方案对扩散的建模能力校正,以算用于对数值溶液的组成依赖性。结果表明,当分配组分的气相饱和度是恒定和粒子相扩散限制分区速率(估计半径变化中的差异10℃的差异)的合理协议。然而,当分区组分的饱和比变化时,找不到通常适用的校正,表明现有方法不能导出一般解决方案。直到发现一般解决方案的时间,应注意敏感性研究,该研究假设恒定的扩散性。该校正在多分离的多过程模型中实现,用于模拟气溶胶相互作用和化学(马赛克),并且用于说明如何通过将增塑成分的冷凝在粘性有机颗粒上的缩合来加速数量分布的演化。

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