H2 Production from Reactions Between Water and Metal Centers in Non-Traditional Oxidation States

Professors Caroline Chick Jarrold and Krishnan Raghavachari are applying experimental and computational approaches to learn about the production of H2 from decomposition of water on transition metal oxide clusters in which the metal centers are in non-traditional oxidation states. These clusters are used to model the local, electronically complex and structurally dynamic properties of defect sites on photocatalysts used in the decomposition of water. The chemistry of these clusters is probed using high-pressure reactivity studies, and product distributions are rationalized using the results of high-level computational studies. Subsequent validation of the computational results is achieved by spectroscopic interrogation of reactants and products. Results of this collaboration have pointed to the electronic and structural features of defect sites that are most active with respect to H2 production, as well as potential mechanisms for liberating trapped H2 on catalyst surfaces.

To learn more, see: “Fluxionality in the Chemical Reactions of Transition Metal Oxide Clusters: The Role of Metal, Spin-State and the Reactant Molecule”, K. Raghavachari et al., J. Phys. Chem. A, in press, and “Properties of Metal Oxide Clusters in non-Traditional Oxidation States” C. C. Jarrold et al., Chem. Phys. Lett. 2012, 525-6, 1.

Caroline Chick Jarrold

Department Chair
Class of 1948 Herman B Wells Endowed Professor

Inorganic, Materials, Physical