中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
首页 机构 成果 学者
  
  1. CAS IR Grid
  2. 地球环境研究所
  3. 中国科学院地球环境研究所
  4. 粉尘与环境研究室
Catalytic effect of (H2O)(n) (n=1-3) clusters on the HO2 + SO2 HOSO + O-3(2) reaction under tropospheric conditions

文献类型：期刊论文

作者Wang, Rui1; Yao, Qiuyue3; Wen, Mingjie1; Tian, Shaobo1; Wang, Yan1; Wang, Zhiyin1; Yu, Xiaohu1; Shao, Xianzhao1; Chen, Long2,4
刊名RSC ADVANCES
出版日期2019-05-29
卷号9期号:28页码:16195-16207
ISSN号2046-2069
DOI10.1039/c9ra00169g
通讯作者Wang, Rui(wangrui830413@163.com)
英文摘要The HO2 + SO2 HOSO + O-3(2) reaction, both without a catalyst and with (H2O)(n) (n = 1-3) as a catalyst, has been investigated using CCSD(T)/CBS//M06-2X/aug-cc-pVTZ methods, and canonical variational transition state theory with small curvature tunneling (CVT/SCT). The calculated results show that H2O exerts the strongest catalytic role in the hydrogen atom transfer processes of HO2 + SO2 HOSO + O-3(2) as compared with (H2O)(2) and (H2O)(3). In the atmosphere at 0 km altitude within the temperature range of 280.0-320.0 K, the reaction with H2O is dominant, compared with the reaction without a catalyst, with an effective rate constant 2-3 orders of magnitude larger. In addition, at 0 km, it is worth mentioning that the relevance of the HO2 + SO2 HOSO + O-3(2) reaction with H2O depends heavily on its ability to compete with the primary loss mechanism of HO2 radicals (such as the HO2 + HO2 and HO2 + NO3 reactions) and SO2 (such as the SO2 + HO reaction). The calculated results show that the HO2 + SO2 HOSO + O-3(2) reaction with H2O cannot be neglected in the primary loss mechanism of the HO2 radical and SO2. The calculated results also show that for the formation of HOSO and O-3(2), the contribution of H2O decreases from 99.98% to 27.27% with an increase in altitude from 0 km to 15 km, due to the lower relative concentration of water. With the altitude increase, the HO2 + SO2 HOSO + O-3(2) reaction with H2O cannot compete with the primary loss mechanism of HO2 radicals. The present results provide new insight into (H2O)(n) (n = 1-3) catalysts, showing that they not only affect energy barriers, but also have an influence on loss mechanisms. The present findings should have broad implications in computational chemistry and atmospheric chemistry.
WOS关键词SINGLE WATER MOLECULE ; HYDROGEN ABSTRACTION REACTION ; GAS-PHASE REACTIONS ; SELF-REACTION ; ATMOSPHERIC REACTION ; FORMIC-ACID ; SULFINIC ACID ; RADICALS ; OH ; KINETICS
资助项目National Natural Science Foundation of China[21603132] ; National Natural Science Foundation of China[41805107] ; Project of Education Department in Shaanxi[18JK0147] ; Funds of Research Programs of Shaanxi University of Technology[SLGQD13(2)-3] ; Funds of Research Programs of Shaanxi University of Technology[SLGQD13(2)-4]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000472461300056
出版者ROYAL SOC CHEMISTRY
资助机构National Natural Science Foundation of China ; Project of Education Department in Shaanxi ; Funds of Research Programs of Shaanxi University of Technology
源URL[http://ir.ieecas.cn/handle/361006/13790]  
专题地球环境研究所_粉尘与环境研究室
通讯作者Wang, Rui
作者单位1.Shaanxi Univ Technol, Sch Chem & Environm Sci, Shaanxi Key Lab Catalysis, Hanzhong, Shaanxi, Peoples R China
2.Chinese Acad Sci, State Key Lab Loess & Quaternary Geol, Inst Earth Environm, Xian, Shaanxi, Peoples R China
3.Henan Normal Univ, Sch Chem & Chem Engn, Henan Key Lab Boron Chem & Adv Energy Mat, Xinxiang 453007, Henan, Peoples R China
4.Chinese Acad Sci, Inst Earth Environm, Key Lab Aerosol Chem & Phys, Xian, Shaanxi, Peoples R China
推荐引用方式
GB/T 7714		 Wang, Rui,Yao, Qiuyue,Wen, Mingjie,et al. Catalytic effect of (H2O)(n) (n=1-3) clusters on the HO2 + SO2 HOSO + O-3(2) reaction under tropospheric conditions[J]. RSC ADVANCES,2019,9(28):16195-16207.
APA Wang, Rui.,Yao, Qiuyue.,Wen, Mingjie.,Tian, Shaobo.,Wang, Yan.,...&Chen, Long.(2019).Catalytic effect of (H2O)(n) (n=1-3) clusters on the HO2 + SO2 HOSO + O-3(2) reaction under tropospheric conditions.RSC ADVANCES,9(28),16195-16207.
MLA Wang, Rui,et al."Catalytic effect of (H2O)(n) (n=1-3) clusters on the HO2 + SO2 HOSO + O-3(2) reaction under tropospheric conditions".RSC ADVANCES 9.28(2019):16195-16207.

入库方式： OAI收割

来源：地球环境研究所

浏览0
下载0
收藏0
其他版本

除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。