Ab initio and variational transition state approach to beta-C3N4 formation: kinetics for the reaction of CH3NH2 with H.
The CH3NH2 molecule has been considered as either an important intermediate in methane and ammonia mixtures or a precursor in methylamine and hydrogen mixtures in the synthesis of carbon nitride thin films. The fast Hydrogen (H) abstraction from CH3NH2 is an important process involved in the formation of HCN or CNH in the chemical vapor deposition (CVD) of carbon nitride thin films. The energetic and kinetic characteristics of the H abstraction reaction from CH3NH2 by atomic H used in CVD of beta-C3N4 were studied using ab initio direct dynamics methods for the first time. Two primary processes were identified for this reaction: H abstraction from the CH3 group and H abstraction from the NH2 group. On the basis of ab initio data, the rate constants of each channel have been deduced by canonical variational transition state theory with small-curvature tunneling correction over a wide temperature range of 200 to approximately 3000 K. The theoretical results were compared with available experimental data.
Zhang
Qingzhu
Q
Center of Super-Diamond and Advanced Films and Department of Physics and Materials Science, City University of Hong Kong, Hong Kong SAR, China.
Zhang
R Q
RQ
Chan
K S
KS
Bello
I
I