Journal
CHEMISTRY OF MATERIALS
Volume 20, Issue 21, Pages 6770-6778Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cm801807b
Keywords
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Funding
- Office of Basic Energy Sciences
- Division of Chemical Sciences, Geosciences, and Energy Biosciences
- Department of Energy [DE-FG02-07ER15911]
- Japan Society for the Promotion of Science (JSPS) Fellowship
- U.S. Department of Energy (DOE) [DE-FG02-07ER15911] Funding Source: U.S. Department of Energy (DOE)
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Potassium hexaniobate nanoscrolls (NS-K4Nb6O17) formed by exfoliation of lamellar K4Nb6O17 were studied as building blocks for visible-light-driven H-2 production (lambda > 420 nm) from water using tris(2,2'-bipyridyl)ruthenium(II) chloride (Ru(bpy)(3)(2+)) as a sensitizer and ethylenediaminetetraacetic acid (EDTA) as an electron donor. The surface of NS-K4Nb6O17 is negatively charged at pH 3-11, enabling cationic Ru(bpy)(3)(2+) molecules to be efficiently adsorbed onto the surface, allowing for rapid excited-state electron and subsequent H-2 evolution without any chemical bond linkage between the sensitizer and the oxide surface. The rate of visible light H-2 production in the nanoscroll-based system is 10 times higher than that of similarly sensitized K4Nb6O17. The difference can be primarily attributed to the strong adsorption of Ru(bpy)(3)(2+) in the case of the nanoscrolls. The maximum photocatalytic reactivity is found over a narrow range of pH and Pt-loading. This study highlights the utility of single-crystalline oxide nanosheets as components of photosystems for visible-light-driven H-2 production from water.
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