摘要
硫酸与硫酸铵二次无机气溶胶是大气气溶胶的重要组成部分,由于气溶胶的环境、气候以及健康效应,与其有关的研究越来越受到人们的重视。在量子化学的理论计算这一背景下,硫酸与硫酸铵气溶胶在分子层面的形成机理得以揭示。对于硫酸气溶胶,通过比较不同计算方法下所得几何构型与相对能量的差异,表明密度泛函理论以及二阶微扰理论更为适用;并且从基本反应出发,研究了额外加入其他物质起到的催化作用。对于硫酸铵气溶胶,通过研究硫酸与氨之间以及最典型的三元系统SO3/NH3/H2O之间形成硫酸铵气溶胶的过程,阐述其形成的历程与特点。
Secondary inorganic aerosols including sulfuric acid aerosols and ammonium sulfate are important components of atmospheric aerosols. Due to the environmental, climatic and health effects of aerosols, more and more attention has been paid to the related researches. The mechanism of secondary inorganic aerosols including sulfuric acid aerosols and ammonium sulfate aerosols is elucidated at the molecular level under the background of theoretical calculation of the quantum chemistry. For sulfuric acid aerosols, the results of comparing the differences of geometric configurations and relative energies under different calculation methods show that the DFT and MP2 methods are more applicable. Moreover, the catalytic effects of additional substances are studied on the basic reaction. For ammonium sulfate aerosols, the reactions between sulfuric acid with ammonia and in the most typical ternary system SO3/NH3/H2O are induced to explain the formation process and characteristics.
作者
何晴
杨柳
盛重义
吴凯
王康慧
张斌
HE Qing;YANG Liu;SHENG Zhongyi;WU Kai;WANG Kanghui;ZHANG Bin(School of Environment,Nanjing Normal University,Nanjing 210023,China;Suzhou Industrial Technology Research Institute,Zhejiang University,Suzhou 215163,China)
出处
《环境科学与技术》
CAS
CSCD
北大核心
2019年第8期118-124,共7页
Environmental Science & Technology
基金
国家自然科学基金面上项目(41877469,41771498)
江苏省高校自然科学研究面上项目(16KJD610001)
关键词
二次气溶胶
硫酸
氨
分子
量子化学
secondary aerosols
sulfuric acid
ammonia
molecules
quantum chemistry
