期刊
CHEMISTRY OF MATERIALS
卷 31, 期 1, 页码 90-100出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.8b03092
关键词
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资金
- NSF RENEW program [CBET-1336844, CBET-1805084 NSF ECCS-1542152]
We synthesized by atomic layer deposition (ALD) TiO2-IrOxF alloys that enable high photovoltages and catalyze water oxidation on silicon metal-insulator-semiconductor (MIS) photoanodes. The ratio of TiO2 to IrOx was precisely controlled by varying the number of ALD cycles for each precursor. Silicon with a 2 nm surface SiO2 layer was coated with TiO2-IrOx alloys ranging in composition from 18 to 35% iridium relative to the sum of titanium and iridium concentrations. IrOx catalyzed oxygen evolution and imparted a high work function to the TiO2-IrOx alloys, enabling photovoltages during water oxidation that exceeded 600 mV. TiO2 imparted stability and inhibited corrosion of the underlying silicon light absorber. After annealing in forming gas (5% H-2/95% N-2), TiO2-IrOx alloys were stable for 12 h of continuous water oxidation in 1 M H2SO4. Key properties of the MIS junction affecting electrochemical operation were also extracted by electrochemical impedance spectroscopy. This work demonstrates that alloying by ALD is a promising approach for designing corrosion resistant Schottky contacts with optimized electronic and materials properties for catalyzed, solar driven water oxidation.
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