BH4﹣在Ru(111)面水解制氢反应的密度泛函理论研究

he reaction mechanism of hydrogen generation from hydrolysis of BH4﹣ on Ru(111) was studied using density functional theory(DFT). All calculations use the generalized gradient approximation with the perdew-Burke-Ernzerhof exchange correlation functional. The geometries of all species in the reaction system (reactants, transition states and products) were optimized. Adsorption energies of possible species and the reaction barriers of possible elementary reactions involved in the mechanism were obtained in this work. The calculation results show that there are five adsorption sites for BH4﹣ on Ru(111), and the adsorption energy is the lowest on the top site. Meanwhile, reaction barrier of B－H bond rupture in BH4﹣ is lower than that of O－H in H2O, as a result, O－H bond rupture on Ru(111) is the control step of the reaction.