期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 21, 期 47, 页码 16948-16954出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201502863
关键词
hydroxide; photocatalysis; rhodium; ruthenium; solar fuel production
资金
- Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Sciences, U.S. Department of Energy [DE FG02-05ER15751]
Polyazine-bridged (RuRhRuII)-Rh-II-Ru-III complexes with two halide ligands, Cl- or Br-, bound to the catalytically active Rh center are efficient single-component photocatalysts for H2O reduction to H-2 fuel, with the coordination environment on Rh impacting photocatalysis. Herein reported is a new, halide-free (RuRhRuII)-Rh-II-Ru-III photocatalyst with OH- ligands bound to Rh, further enhancing the photocatalytic reactivity of the structural motif. H-2 production experiments using the photocatalyst bearing OH- ligands at Rh relative to the analogues bearing halides at Rh in solvents of varying polarity (DMF, CH3CN, and H2O) suggest that ion pairing with halides deactivates photocatalyst function, representing an exciting phenomenon to exploit in the development of catalysts for solar H-2 production schemes.
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