Modulating the Oxygen Evolution Reaction of Single-Crystal Cobalt Carbonate Hydroxide via Surface Fe Doping and Facet Dependence

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Abstract
The oxygen evolution reaction (OER) is a critical half-reaction in water splitting and metal-air cells. The sensitivity of the OER to the composition and structure of the electrocatalyst presents a significant challenge in elucidating the structure-property relationship. In this study, highly stable single-crystal cobalt carbonate hydroxide [Co2(OH)2CO3, CoCH] was used as a model to investigate the correlations among structure, composition, and reactivity. Single-crystal CoCH nanowires (denoted as CoCH NWs) and Fe-doped CoCH nanowires (denoted as Fe-CoCH NWs) with an exposed (210) facet and Fe-doped CoCH nanosheets (denoted as Fe-CoCH NSs) with an exposed (2-13) facet were synthesized using electrochemical and one-step hydrothermal strategies, respectively. Their OER activity decreased in the following order: Fe-CoCH NWs > Fe-CoCH NSs > CoCH NWs. Theoretical investigation suggested that the doped Fe sites serve as active sites, and the crystal-facet dependence can finely adjust the 3d configuration of Fe sites, resulting in the optimal adsorption strengths and energy barriers for potential-determining steps on the (210) facet of CoCH. This renders the as-prepared Fe-CoCH NWs as some of the most promising Co-based OER catalysts.
Funding Information
  • Shenzen Municipal Technical Project (JSGG20200925145800001)
  • Science and Technology Foundation of Shenzhen City (CJGJZD20210408092801005, GJHZ20220913142812025, SGDX20211123151002003)
  • Department of Education of Guangdong Province (2022ZDZX3018)
  • National Natural Science Foundation of China (11921006)
  • Natural Science Foundation of Guangdong Province (2022A1515010076)
  • Shenzhen University (2023QNT007)

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