期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 136, 期 27, 页码 9773-9779出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja505022f
关键词
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资金
- Center for Catalytic Hydrocarbon Functionalization, an Energy Frontier Research Center (EFRC) - U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-SC0001298]
- U.S. DOE, Office of Basic Energy Sciences [DE-SC0001011]
- Department of Defense, Air Force Office of Scientific Research, National Defense Science and Engineering Graduate (NDSEG) Fellowship [FA9550-11-C-0028, 32 CFR 168a]
- Research Triangle Solar Fuels Institute
- U.S. Department of Education through a GAANN Fellowship [P200A120021]
Light-driven dehydrogenation of benzyl alcohol (BnOH) to benzaldehyde and hydrogen has been shown to occur in a dye-sensitized photoelectrosynthesis cell (DSPEC). In the DSPEC, the photoanode consists of mesoporous films of TiO2 nanoparticles or of core/shell nanoparticles with tin-doped In2O3 nanoparticle (nanoITO) cores and thin layers of TiO2 deposited by atomic layer deposition (nanoITO/TiO2). Metal oxide surfaces were coderivatized with both a ruthenium polypyridyl chromophore in excess and an oxidation catalyst. Chromophore excitation and electron injection were followed by cross-surface electron-transfer activation of the catalyst to -Ru-IV=O2+, which then oxidizes benzyl alcohol to benzaldehyde. The injected electrons are transferred to a Pt electrode for H-2 production. The nanoITO/TiO2 core/shell structure causes a decrease of up to 2 orders of magnitude in back electron-transfer rate compared to TiO2. At the optimized shell thickness, sustained absorbed photon to current efficiency of 3.7% was achieved for BnOH dehydrogenation, an enhancement of similar to 10 compared to TiO2.
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