Journal
ACS CATALYSIS
Volume 5, Issue 9, Pages 5627-5635Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.5b01306
Keywords
photodeposition; carbon dioxide reduction; artificial photosynthesis; photocatalysis; copper oxide catalyst; heterobinuclear light absorber
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Funding
- Office of Science, Office of Basic Energy Sciences, Division of Chemical, Geological and Biosciences of the U.S. Department of Energy [DE-AC02-05CH11231]
- National Center for Electron Microscopy
- Lawrence Berkeley National Laboratory
- U.S. Department of Energy
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Hierarchical assembly of an oxo-bridged binuclear ZrOCoII light absorber unit coupled to a cuprous oxide nanocluster catalyst for CO2 reduction on mesoporous silica support is demonstrated. The proper positioning of the Cu oxide cluster was achieved by photodeposition of a [Cu(NCCH3)(4)](2+)precursor by visible light excitation of the ZrOCo charge transfer chromophore, followed by mild calcination at 350 C. Illumination of the CuxOy-ZrOCo unit so formed in the presence of a diethylamine electron donor resulted in the reduction of surface Cu centers to Cu-0 as demonstrated by the characteristic infrared band of adsorbed (CO)-C-13 probe molecules at 2056 cm(-1). For analogous CuxOy-TiOCoII units, the oxidation state makeup of the surface Cu centers was dominated by Cu-I, and the Cu-0, Cu-I, and Cu-II composition was found to depend on the wavelength of MMCT excitation. The observed strong dependence of the CO2 photoreduction yield on the oxidation state of the surface Cu centers directly proves that CO2 is reduced on the CuxOy surface, thus establishing that the ZrOCoII unit functions as light absorber, donating electrons to the CuxOy catalyst on whose surface CO2 is reduced.
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