CCSD(T) and DFT have been used to study H2 and O2 production from the reaction of H2O with (MO2)n (M=Ti, Zr, Hf, n=1 - 3) nanoclusters on the ground state singlet and first excited state triplet potential energy surfaces. After Lewis acid-base addition of H2O to the cluster, a hydrogen is transferred to an M-O oxygen. H2 production occurs via the formation of an intermediate with an M-H bond followed by H-H recombination and H2 desorption. O2 is produced by breaking M-O bonds in an atomic oxygen saturated metal oxide composed of M-O-O-(M) bond. The water splitting reaction to generate H2 and O2 takes place predominantly on the excited triplet potential energy surface. The rate-determining steps are the formation of the metal hydride, a formal two-electron reduction starting from an OH group. This work is supported by the U.S. DOE Office of Science (BES).

Computational study of H2 and O2 production from water splitting by MO2 nanoclusters (M = Ti, Zr, Hf)

245th National Meeting (2013)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.