期刊
NATURE MATERIALS
卷 15, 期 4, 页码 456-+出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/NMAT4511
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资金
- US Department of Energy, Office of Science, Office of Basic Energy Sciences, Solar Photochemistry Program [DE-AC36-08GO28308]
- NSF [DGE 1144083]
Producing hydrogen through solar water splitting requires the coverage of large land areas. Abundant metal-based molecular catalysts offer scalability, but only if they match noble metal activities. We report on a highly active p-GaInP2 photocathode protected through a 35-nm TiO2 layer functionalized by a cobaloxime molecular catalyst (GaInP2-TiO2-cobaloxime). This photoelectrode mediates H-2 production with a current density of similar to 9mAcm(-2) at a potential of 0V versus RHE under 1-sun illumination at pH 13. The calculated turnover number for the catalyst during a 20-h period is 139,000, with an average turnover frequency of 1.9 s(-1). Bare GaInP2 shows a rapid current decay, whereas the GaInP2-TiO2-cobaloxime electrode shows <= 5% loss over 20 min, comparable to a GaInP2-TiO2-Pt catalyst particle-modified interface. The activity and corrosion resistance of the GaInP2-TiO2-cobaloxime photocathode in basic solution is made possible by an atomic layer-deposited TiO2 and an attached cobaloxime catalyst.
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