Surface electronic structure reconstruction of binary metal spinel oxide by sulfur inducing for superior water electrolysis

APPLIED SURFACE SCIENCE(2024)

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摘要
The selection of electrocatalysts for the oxygen evolution reaction (OER) is crucial for hydrogen production from water electrolysis. Binary metal spinel oxide CuCo2O4 has emerged as a promising OER catalyst due to its unique multi-valence characteristics and cost-effectiveness, but its practical application has faced challenges stemming from limitations in its electronic structure and a scarcity of active sites. Herein, we have introduced sulfur (S) into CuCo2O4, leading to a significant increase in oxygen defects and a partially amorphous phase formation. The optimized S-CuCo2O4/CC electrocatalyst exhibits an overpotential of only 216 mV at 10 mA cm-2. The excellent performance originates from reconfiguring the electronic structure upon S introduction, leading to optimized intermediates' adsorption/desorption and an increase in active sites by forming a partially amorphous phase. Meanwhile, due to the abundance of active S sites and enhanced kinetics, the catalyst demonstrates outstanding performance in the hydrogen evolution reaction (HER). It exhibits a promising potential for overall water splitting (OWS) with a low voltage of 1.67 V at 10 mA cm-2. This study synergistically combines doping, vacancy, and amorphization strategies to thoroughly analyze their impact on catalytic performance, offering valuable insights for the design of efficient and stable non-noble metal catalysts.
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关键词
Surface electronic structure,Binary metal spinel oxide,Amorphous phase,Oxygen evolution reaction,DFT calculation
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