Consecutive thermal H2 and light-induced O2 evolution from water promoted by a metal complex

Stephan W. Kohl, Lev Weiner, Leonid Schwartsburd, Leonid Konstantinovski, Linda J.W. Shimon, Yehoshoa Ben David, Mark A. Iron, David Milstein

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Abstract

Discovery of an efficient artificial catalyst for the sunlight-driven splitting of water into dioxygen and dihydrogen is a major goal of renewable energy research. We describe a solution-phase reaction scheme that leads to the stoichiometric liberation of dihydrogen and dioxygen in consecutive thermal- and light-driven steps mediated by mononuclear, well-defined ruthenium complexes. The initial reaction of water at 25°C with a dearomatized ruthenium (II) [Ru(II)] pincer complex yields a monomeric aromatic Ru(II) hydrido-hydroxo complex that, on further reaction with water at 100°C, releases H2 and forms a cis dihydroxo complex. Irradiation of this complex in the 320-to-420-nanometer range liberates oxygen and regenerates the starting hydrido-hydroxo Ru(II) complex, probably by elimination of hydrogen peroxide, which rapidly disproportionates. Isotopic labeling experiments with H 2 17O and H2 18O show unequivocally that the process of oxygen-oxygen bond formation is intramolecular, establishing a previously elusive fundamental step toward dioxygen-generating homogeneous catalysis.

Original languageEnglish
Pages (from-to)74-77
Number of pages4
JournalScience
Volume324
Issue number5923
DOIs
Publication statusPublished - Apr 3 2009

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Cite this

Kohl, S. W., Weiner, L., Schwartsburd, L., Konstantinovski, L., Shimon, L. J. W., David, Y. B., Iron, M. A., & Milstein, D. (2009). Consecutive thermal H2 and light-induced O2 evolution from water promoted by a metal complex. Science, 324(5923), 74-77. https://doi.org/10.1126/science.1168600