A Statistical Model for Predicting Thermal Chemical Reaction Rate: Application to Bimolecule Reactions
LI Wang-Yao1,2 , LIN Zheng-Zhe3,4 , XU Jian-Jun1,2 , NING Xi-Jing3,4**
1 Department of Physics, Fudan University, Shanghai 200433 2 State Key Laboratory of Surface Physics, Fudan University, Shanghai 200433 3 Institute of Modern Physics, Fudan University, Shanghai 200433 4 Key Laboratory of Applied Ion Beam Physics (Ministry of Education), Fudan University, Shanghai 200433
Abstract ：A model based on the statistics of individual atoms [Europhys. Lett. 94 (2011) 40002], which has been successfully applied to predict the rate constant of unimolecular reactions, was further extended to bimolecular reactions induced by collisions. Compared with the measured rate constants of the reactions S+SO2 →SO+SO and NH3 +Cl→NH2 +HCl, the model is proved to be significantly better than conventional transition state theory. In order to strictly test the model, we perform molecular dynamics simulation of C60 +C60 →C120 , and show that the rate constants are in excellent agreement with our model but far away from the transition state theory.
收稿日期: 2012-04-24
出版日期: 2012-07-31
:
05.20.Dd
(Kinetic theory)
34.50.Lf
(Chemical reactions)
71.15.Pd
(Molecular dynamics calculations (Car-Parrinello) and other numerical simulations)
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2012, Vol. 29 
