Theoretical study of H2 dissociation on a ZrO2 cluster

摘要

We present a detailed study of the interaction between the ZrO_2 molecule and H2 within DFT and CCSD(T) approaches. H_2 activation is followed by cleavage of H-H bond giving OZrH-OH species with hydride and hydroxyl groups. Both direct transfer of H from Zr-H to Zr-OH and a two step process via a Zr(OH)_2 intermediate (in a triplet state) lead to water formation generating ZrO...H_2O. The hybrid B3LYP or PBE0 functionals with SDD pseudopotential/basis set on Zr and 6-311++G(2df,2p) basis sets for O, H represent the best compromise between accuracy and computational cost.