Density functional theory study on NiTi+catalytic dehydrogenation of methylcyclohexane
Organic liquid hydrogen storage is a promising hydrogen storage method.Studying the catalytic mecha-nism of hydrogen storage-release at the atomic level is an important way to find efficient and low-cost cata-lysts.The reaction mechanism of stepwise dehydrogenation of methylcyclohexane(MCH)to toluene under the ca-talysis of transition metal dimer ion NiTi+was studied by density functional theory(DFT)method,and the ener-gy changes of reactants,intermediates and products were investigated.The wave function analysis method was used to observe the change of atomic charge during the reaction,and the properties such as the density of states(DOS)of the initial compound were analyzed.The results show that the reaction between NiTi+and methylcyclo-hexane is an exothermic reaction on the mixed potential energy surface.The three dehydrogenation molecular mechanisms are similar.The overall exothermic heat of the reaction is-12.19 kcal·mol-1.The intermediates methylcyclohexene and methylcyclohexadiene were obtained,which were consistent with the experimental re-sults.The rate-determining step of the whole reaction is IM10→TS10 during the third dehydrogenation reaction.
DehydrogenationDensity functional theoryDensity of statesReaction mechanismNiTi+Meth-ylcyclohexane
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