Photocatalytic Water Oxidation with Nonsensitized IrO2 Nanocrystals under Visible and UV Light

被引:225
作者
Frame, F. Andrew [1 ]
Townsend, Troy K. [1 ]
Chamousis, Rachel L. [1 ]
Sabio, Erwin M. [1 ]
Dittrich, Th [2 ]
Browning, Nigel D. [3 ]
Osterloh, Frank E. [1 ]
机构
[1] Univ Calif Davis, Dept Chem, Davis, CA 95616 USA
[2] Helmholtz Zentrum Berlin Mat & Energie, D-14109 Berlin, Germany
[3] Univ Calif Davis, Dept Chem Engn & Mat Sci, Davis, CA 95616 USA
基金
美国国家科学基金会;
关键词
CATALYSTS; OXYGEN; IRRADIATION; REDUCTION; EVOLUTION; COLLOIDS; FILM;
D O I
10.1021/ja200144w
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Rutile IrO2 is known as being among the best electrocatalysts for water oxidation. Here we report on the unexpected photocatalytic water oxidation activity of 1.98 nm +/- 0.11 nm succinic acid-stabilized IrO2 nanocrystals. From aqueous persulfate and silver nitrate solution the nonsensitized particles evolve oxygen with initial rates up to 0.96 mu mol min(-1) and with a quantum efficiency of at least 0.19% (measured at 530 nm). The catalytic process is driven by visible excitations from the Ir-d(t(2g)) to the Ir-d(e(g)) band (1.5-2.75 eV) and by ultraviolet excitations from the O-p band to the Ir-d(e(g)) (>3.0 eV) band. The formation of the photogenerated charge carriers can be directly observed with surface photovoltage spectroscopy. The results shed new light on the role of IrO2 in dye- and semiconductor-sensitized water splitting systems.
引用
收藏
页码:7264 / 7267
页数:4
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