Publication date: 15th December 2014
The photoelectrochemical(PEC) process is an innovative approach in which energy collection (solar absorber) and water electrolysis (catalysis) are mated into a single device. The bulk of the research over the last 40+ years has been focused on metal oxides where the efficiency of PEC solar hydrogen generation is very low due to the combined challenges of poor solar absorption and poor electronic properties. More suitable semiconductors (SC) for high efficiency solar photoconversion such as the III-Vs suffer from material instability. Incorporation of proper electrocatalystsonto the illuminated SC surface is necessary to both stabilize the PEC interface and increase catalysis, thus enhancing the overall device performance. The branching ratio between catalysis and corrosion must be extremely high (>106) in order for the system to have the necessary lifetime, thus the catalysts must have a very high turnover frequency (TOF) and turnover number (TON). Such materials for SC surface modification are particularly beneficial if they are potentially low-cost and scalable, transparent and conductive while also highly catalytically active and stable. Work on hydrogen evolution catalysts has been a very active area of research where numerous molecular, nanomaterial, and bulk catalysts have been developed. Nonetheless noble metals, particularly platinum, are mostly commonly applied as they are the most active for the water redox reactions. Nobel metals are neither earth abundant nor low-cost, so identifying catalytic systems that can match the activity and stability of platinum but are based on earth abundant materials are clearly a high-priority area of research.We will report on the immobilization of a cobaltoxime hydrogen evolution catalyst on an ALD TiO2 modified p-GaInP2 surface and its catalytic activity under illumination in pH 13 aqueous solution. The GaInP2-TiO2-cobaltoxime photocathode exhibited remarkable stability during 24 hours of continuous operation at 0 V vs. RHE with the catalyst showing a TON of 303,000 and TOF of 12600 sec-1 during that time. A high IPCE, up to ~70% through visible range (<690nm), was observed from this structure clarifying the advantage of a visible-light transparent hydrogen evolution catalyst.
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