High-Entropy Single Atom Catalysts Anchored on Flexible Carbon Fibers for Enhanced Bifunctional Oxygen Catalysis Activity and Stability.
basic_science · Level V
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- Record sourced from PubMed, PMID 41618917.
- Also identified by DOI 10.1021/acsnano.5c18441.
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Abstract
High-entropy single atom (SA) catalysts (HESACs) represent a paradigm shift in electrocatalyst design, yet precise structural control and mechanistic understanding remain key challenges. Here, we report a porous carbon fiber-supported HESAC (ZnCoNiCuFe@PCF) that synergistically integrates five atomically dispersed M-N<sub>4</sub> sites (M = Zn, Co, Ni, Cu, Fe) and Co<sub>6</sub>/Fe<sub>5</sub> nanoclusters, creating unprecedented electronic interactions and maximizing high-entropy synergy. As a result, ZnCoNiCuFe@PCF exhibits outstanding bifunctional electrocatalytic activity for both oxygen reduction (oxygen reduction reaction (ORR)) and oxygen evolution reactions (OER), outperforming the benchmark Pt/C and RuO<sub>2</sub> catalysts. Density functional theory calculations reveal that the unique combination of high-entropy atom sites and nanoclusters facilitates charge redistribution and optimizes the adsorption of key intermediates (OH*, O*), thereby accelerating the rate-limiting steps of ORR/OER. When deployed as the cathode in a zinc-air battery (ZAB), the catalyst delivers a peak power density of 240.9 mW cm<sup>-2</sup> and exceptional cycling stability of over 2600 h (7800 cycles). This work provides fundamental insights into the rational design of HESACs by leveraging high-entropy and heterojunction effects, offering a robust platform for next-generation energy storage and conversion technologies.