We integrated laser-made highly active nickel iron layered double hydroxide ([NiFe]-LDH) water oxidation nanocatalysts, which we developed in our group (J. Am. Chem. Soc. 2014, 136, 13118), with BiVO4 photoanodes and tested their photoelectrochemical performance under simulated sunlight illumination. We demonstrated decreased aggregation and increased photocurrent generation with nanocatalysts that contain dipositive metals ([NiFe]-LDH and cobalt oxide) as citrate surfactant selectively ligated the catalyst nanoparticles. We also optimized catalyst mass loading, which is a tradeoff between most efficient depletion of photogenerated holes that drive catalytic turnover and parasitic light absorption by the catalyst particles. Integrated [NiFe]-LDH–BiVO4 photoanodes enhanced photocurrent generation by a factor of 3.3 compared to bare BiVO4. Comparison of photoelectrochemical performance of integrated [NiFe]-LDH–BiVO4 photoanodes in sulfite-free aqueous electrolyte with photocurrent generation of neat BiVO4 photoanodes in aqueous electrolyte with sulfite added as sacrificial hole acceptor showed that two thirds of all photogenerated holes escaped loss processes in our optimized integrated photoanodes. Our systematic integration strategies provide a path towards functional artificial photosynthesis devices.

Photoelectrochemical performance of BiVO4 photoanodes integrated with [NiFe]-layered double hydroxide water oxidation nanocatalysts

255th National Meeting (2018)

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