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- Title
Theoretical study on reaction mechanism of sulfuric acid and ammonia and hydration of (NH)SO.
- Authors
Liu, Wei-Wei; Wang, Xiao-Lin; Chen, Shi-Lu; Zhang, Yun-Hong; Li, Ze-Sheng
- Abstract
In order to understand the mechanism of nucleation of (NH)SO aerosol, the reaction between sulfuric acid and ammonia in the absence of water molecule is performed at M06/6-311++G(d,p) level. The results show that the (NH)SO and NHHSO units may exist instantaneously in gas phase without water molecule, which is a theoretical prediction that needs detection by further experiment. To further study the growth of the primary nuclei, the geometries, energies, and harmonic frequencies of (NH)SO · (HO) ( n = 0-9) are calculated both at M06/6-311++G(d,p) and B3LYP/6-311++G(d,p) levels. The tendency of the theoretical vibration frequencies is in accordance with the experimental results. The influence of the water molecule on the properties of (NH)SO is also analyzed. Our results indicate that M06 is more accurate than B3LYP for this kind of system. Moreover, the first principle molecular dynamics method is used to simulate the structural transformation for two representative isomers whose energies are close, to understand the relationship between solvent-shared ion pairs and contact ion pairs.
- Subjects
REACTION mechanisms (Chemistry); SULFURIC acid; AMMONIA; HYDRATION; SULFATES; NUCLEATION; AEROSOLS; WATER; SIMULATION methods &; models; PHASE transitions; MOLECULAR dynamics
- Publication
Theoretical Chemistry Accounts: Theory, Computation, & Modeling, 2012, Vol 131, Issue 2, p1
- ISSN
1432-881X
- Publication type
Article
- DOI
10.1007/s00214-012-1103-4