Catalytic mechanism for single-site water oxidation process: A theoretical study
Water oxidation catalyzed by single-site ruthenium complexes has generated enormous interests related to solar fuels. Combining several theoretical tools, we studied the entire catalytic cycle of water oxidation for a single site catalyst starting with [RuII(OH2)(tpy)(bpm)]2+ (i.e, [RuII-OH2]2+) as a representative example of a new class of single site catalysts. The electronic spin states of ruthenium intermediates during the catalytic cycle are identified as well as the corresponding optimal geometries. Results about each individual step will be presented in this talk. Our theoretical studies with atomistic details shed light on the reaction mechanisms of several pivotal reaction steps during the entire catalytic cycle and should be helpful in the design new catalysts for solar fuels.