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<p>The electrochemical CO<sub>2</sub> reduction to produce valuable chemicals is a viable approach for mitigating carbon emissions. In this study, a high-entropy oxides (HEOs)-based electrocatalyst comprising the oxide of transition metals (M = Co, Fe, Zn, Ni, and Cu; termed CFZNC) anchored on activated-carbon powder (ACP) is synthesized by the polymerization of phenol and formaldehyde in situ dispersed with the respective metal salts, followed by ball milling and thermal treatment (carbonization and steam activation) of the synthesized polymeric beads. The electrochemical characterization tests of the prepared CFZNC-HEO/ACP electrocatalyst confirm a high current density of 10&#xa0;mA.cm<sup>−2</sup> at a low applied potential of − 0.37&#xa0;V vs. RHE. The electrochemical CO<sub>2</sub> reduction tests reveal a formate (HCOO<sup>−</sup>) Faradaic efficiency of 98 ± 4.9% and a cathodic energy efficiency of 86 ± 4.3% at − 0.4&#xa0;V, thus highlighting an efficient energy utilization of the material and selectivity toward formate production. Notably, the comparative tests reveal CFZNC-HEO/ACP outperforming its high-entropy alloy (HEA) counterpart, viz. CFZNC-HEA/ACP-based electrocatalyst, thus obviating the need for the high-temperature hydrogen-reduction step required to transform metal oxides to metal alloy. The enhanced performance is attributed to the synergistic effect of the multiple metal oxides in the high-entropy formation and the highly porous and conductive carbon substrate. These findings demonstrate the promise of high-entropy metal-oxide-based electrocatalyst in advancing efficient and sustainable CO<sub>2</sub> reduction technologies.</p> Graphical Abstract <p></p>

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Electrochemical CO2-Reduction to Formate over Activated-Carbon-Supported Transition Metals (M = Cu, Fe, Zn, Ni, Co)-Based High-Entropy Oxide

  • 期刊论文

  • 发表日期：

    2025年10月18日

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  • Naveen Kumar Verma,
  • Basker Sundararaju,
  • Nishith Verma

摘要

The electrochemical CO2 reduction to produce valuable chemicals is a viable approach for mitigating carbon emissions. In this study, a high-entropy oxides (HEOs)-based electrocatalyst comprising the oxide of transition metals (M = Co, Fe, Zn, Ni, and Cu; termed CFZNC) anchored on activated-carbon powder (ACP) is synthesized by the polymerization of phenol and formaldehyde in situ dispersed with the respective metal salts, followed by ball milling and thermal treatment (carbonization and steam activation) of the synthesized polymeric beads. The electrochemical characterization tests of the prepared CFZNC-HEO/ACP electrocatalyst confirm a high current density of 10 mA.cm−2 at a low applied potential of − 0.37 V vs. RHE. The electrochemical CO2 reduction tests reveal a formate (HCOO−) Faradaic efficiency of 98 ± 4.9% and a cathodic energy efficiency of 86 ± 4.3% at − 0.4 V, thus highlighting an efficient energy utilization of the material and selectivity toward formate production. Notably, the comparative tests reveal CFZNC-HEO/ACP outperforming its high-entropy alloy (HEA) counterpart, viz. CFZNC-HEA/ACP-based electrocatalyst, thus obviating the need for the high-temperature hydrogen-reduction step required to transform metal oxides to metal alloy. The enhanced performance is attributed to the synergistic effect of the multiple metal oxides in the high-entropy formation and the highly porous and conductive carbon substrate. These findings demonstrate the promise of high-entropy metal-oxide-based electrocatalyst in advancing efficient and sustainable CO2 reduction technologies.

Graphical Abstract