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Effects of a Proximal Base on Water Oxidation and Proton Reduction Catalyzed by Geometric Isomers of [Ru(tpy)(pynap)(OH₂)]²⁺ 

The importance of pendent bases in promoting proton-coupled electron-transfer (PCET) reactions with low activation barriers has been discussed for H⁺ reduction or H₂ oxidation in MeCN by many groups. PCET is also essential for the 4e– oxidation of water in order to mitigate charge buildup and to reduce overpotential. We investigated the redox and spectroscopic properties, and report the intriguing catalytic activity for the oxidation of H₂O and the reduction of protons with geometric isomers of Ru complexes with pendent bases. While 1(OH₂)²⁺ shows catalytic activity toward proton reduction, but not toward water oxidation, the geometric isomer, 2(OH₂)²⁺, exhibits the opposite behavior.

Last Modified: September 13, 2012

One of ten national laboratories overseen and primarily funded by the Office of Science of the U.S. Department of Energy (DOE), Brookhaven National Laboratory conducts research in the physical, biomedical, and environmental sciences, as well as in energy technologies and national security. Brookhaven Lab also builds and operates major scientific facilities available to university, industry and government researchers. Brookhaven is operated and managed for DOE's Office of Science by Brookhaven Science Associates, a limited-liability company founded by the Research Foundation for the State University of New York on behalf of Stony Brook University, the largest academic user of Laboratory facilities, and Battelle, a nonprofit, applied science and technology organization.

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