期刊
SCIENCE
卷 324, 期 5923, 页码 74-77出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1168600
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资金
- Israel Science Foundation
- American Chemical Society
- Deutsch-Israelische Partnerschaft
- Helen and Martin Kimmel Center for Molecular Design
- Humboldt Foundation, Feodor Lynen Postdoctoral Fellowship
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 degrees 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 degrees C, releases H-2 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 (H2O)-O-17 and (H2O)-O-18 show unequivocally that the process of oxygen-oxygen bond formation is intramolecular, establishing a previously elusive fundamental step toward dioxygen-generating homogeneous catalysis.
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