Understanding the origin of photoelectrode performance enhancement by probing surface kinetics

Chemical Science
James E ThorneDunwei Wang

Abstract

Photoelectrochemical (PEC) water splitting holds the potential to meet the challenges associated with the intermittent nature of sunlight. Catalysts have often been shown to improve the performance of PEC water splitting, but their working mechanisms are not well understood. Using intensity modulated photocurrent spectroscopy (IMPS), we determined the rate constants of water oxidation and recombination at the surface of three different hematite-based photoanodes. It was found that the best performing electrodes, in terms of photocurrent onset potential, exhibited the slowest water oxidation rate constants, which was a surprise. The performance of these photoelectrodes was enabled by the slow surface recombination. When amorphous NiFeO x , a water oxidation catalyst, was present, the rate of surface hole transfer actually slowed down; what was slowed more was the recombination rate at the hematite surface, resulting in better water oxidation performance. As such, NiFeO x primarily serves as a passivation layer rather than a catalytic layer. Together a better understanding of the role of catalytic overlayers for water oxidation has been achieved.

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Citations

Jan 23, 2019·Chemical Society Reviews·Yumin HeDunwei Wang
Oct 9, 2019·The Journal of Chemical Physics·Yumin HeDunwei Wang
Mar 21, 2020·Advanced Science·Sitaramanjaneya Mouli ThalluriLifeng Liu
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May 23, 2017·Physical Chemistry Chemical Physics : PCCP·Chun DuBin Shan
Nov 1, 2017·Physical Chemistry Chemical Physics : PCCP·James E ThorneDunwei Wang
Jun 6, 2017·Chemical Science·Carolin ZachäusRoel van de Krol
Mar 27, 2020·Physical Chemistry Chemical Physics : PCCP·Zhongyuan ZhouXiaofeng Li
Aug 11, 2020·Advanced Functional Materials·Attila KormányosCsaba Janáky
Jul 20, 2017·Physical Chemistry Chemical Physics : PCCP·Dino KlotzAvner Rothschild
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May 25, 2018·ACS Applied Materials & Interfaces·Wei LiDunwei Wang
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Aug 14, 2020·The Journal of Physical Chemistry Letters·Camilo A MesaJames R Durrant
Mar 28, 2020·ACS Applied Materials & Interfaces·Yangqin GaoLei Ge

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Methods Mentioned

BETA
X-ray

Software Mentioned

IMVS
IMPS

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