title: Water oxidation by a nickel-glycine catalyst.
abstract: The utilization of solar energy requires an efficient means for its storage as chemical energy. In bioinspired artificial photosynthesis, light energy can be used to drive water oxidation, but catalysts that produce molecular oxygen from water are needed to avoid excessive driving potentials. In this paper, we demonstrate the utility of a novel complex utilizing earth-abundant Ni in combination with glycine as an efficient catalyst with a modest overpotential of 0.475 ± 0.005 V at a current density of 1 mA/cm(2) at pH 11. Catalysis requires the presence of the amine moiety with the glycine most likely coordinating the Ni in a 4:1 molar ratio. The production of molecular oxygen at a high potential is verified by measurement of the change in oxygen concentration, yielding a Faradaic efficiency of 60 ± 5%. The catalytic species is most likely a heterogeneous Ni-hydroxide formed by electrochemical oxidation. This Ni species can achieve a current density of 4 mA/cm(2) that persists for at least 10 h. Based upon the observed pH dependence of the current amplitude and oxidation/reduction peaks, the catalytic mechanism is an electron-proton coupled process.
authors.affiliation: Department of Chemistry and Biochemistry, Arizona State University , Tempe, Arizona 85287-1604, United States.
authors.forename: Dong
authors.initials: D
authors.lastname: Wang
authors.forename: Giovanna
authors.initials: G
authors.lastname: Ghirlanda
authors.forename: James P
authors.initials: JP
authors.lastname: Allen
mesh_terms: D002384:Catalysis; D004563:Electrochemistry; D005998:Glycine / Q000737:chemistry*; D006863:Hydrogen-Ion Concentration; D008027:Light; D009532:Nickel / Q000737:chemistry*; D010084:Oxidation-Reduction; D055668:Photochemical Processes; D014867:Water / Q000737:chemistry*
chemical_list: D014867:Water; D009532:Nickel; D005998:Glycine