为研究亚硝酸(HONO)在γ-Al_2O_3(110)表面非均相氧化SO_2的机理,基于密度泛函理论(density functional theory,DFT)的第一性原理计算了SO_2和HONO在γ-Al_2O_3(110)表面的吸附机制和氧化机制。结果表明,SO_2以分子的形式吸附在完整或缺陷的γ-Al_2O_3(110)表面,而HONO仅在完整表面上以分子的形式存在。表面氧缺陷的存在不仅会增强SO_2和HONO的吸附强度,而且能诱导HONO在含氧缺陷表面的分解(HONO→NO+·OH)。通过局域态密度(partial density of states,PDOS)和Mulliken电荷布局分析表明,HONO的分解遵循Haber-Weiss机制。当SO_2和HONO共同吸附在氧缺陷表面时,HONO分解产生·OH,氧化SO_2形成HOSO_2团簇分子。该研究不仅有助于理解HONO在矿物氧化物表面氧化SO_2的作用,而且为解释大气硫酸盐气溶胶的形成提供了理论依据。 相似文献
The impacts of different moisture profiles on the structure and vertical motion of squall lines were investigated by conducting a set of numerical simulations. The base state was determined by an observational sounding, with high precipitable water representing moist environmental conditions in the East Asian monsoon region. To reveal the impact of moisture at different levels, the moisture content at the middle and low levels were changed in the numerical simulations. The numerical results showed that more convective cells developed and covered a larger area in the high moisture experiments, which was characteristic of the convection during the Meiyu season in China. In addition, high moisture content at low levels favored the development of updrafts and triggered convection of greater intensity. This was demonstrated by the thermodynamic parameters, including Convective Available Potential Energy (CAPE), Lifted Index (LI), Lift Condensation Level (LCL), and Level of Free Convection (LFC). Dry air at middle levels led to strong downdrafts in the environment and updrafts in clouds. This could be because dry air at middle levels favors the release of latent heat, thereby promoting updrafts in clouds and downdrafts in the environment. Therefore, high relative humidity (RH) at low levels and low RH at middle levels favors updrafts in the cloud cores. Additionally, moist air at low levels and dry air at middle levels promotes the development of convective cells and the intensification of cold pool. The squall line can be organized by the outflow boundary induced by cold pool. The balance of cold pool and environmental wind shear is favorable for the maintenance and strengthening of squall lines. 相似文献