Visible Light Driven Benzyl Alcohol Dehydrogenation in a Dye-Sensitized Photoelectrosynthesis Cell

Journal Article · Fri Jun 27 04:00:00 EDT 2014 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/ja505022f· OSTI ID:1387123

Song, Wenjing ^[1]; Vannucci, Aaron K. ^[1]; Farnum, Byron H. ^[1]; Lapides, Alexander M. ^[1]; Brennaman, M. Kyle ^[1]; Kalanyan, Berç ^[2]; Alibabaei, Leila ^[1]; Concepcion, Javier J. ^[1]; Losego, Mark D. ^[2]; Parsons, Gregory N. ^[2]; Meyer, Thomas J. ^[1]

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1. Department of Chemistry, University of North Carolina at Chapel Hill, CB3290, Chapel Hill, North Carolina 27599, United States
2. Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, North Carolina 27695, United States

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 RuIV=O2+, which then oxidizes benzyl alcohol to benzaldehyde. The injected electrons are transferred to a Pt electrode for H2 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 ~10 compared to TiO2.

• Research Organization: Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
• DOE Contract Number: SC0001011
• OSTI ID: 1387123
• Journal Information: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 27 Vol. 136; ISSN 0002-7863
• Publisher: American Chemical Society (ACS)
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
catalysis (heterogeneous)
catalysis (homogeneous)
charge transport
electrodes - solar
hydrogen and fuel cells
materials and chemistry by design
photosynthesis (natural and artificial)
solar (fuels)
solar (photovoltaic)
synthesis (novel materials)
synthesis (self-assembly)