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<p>The direct electrochemical oxidation of methane to high-value products under mild conditions holds significant economic importance, but challenges, such as insufficient active sites, poor product selectivity, and sluggish reaction kinetics, often persist. Herein, NiCuCoMnAg high-entropy alloys (HEAs) were prepared via a freeze-thaw method as highly active and selective catalysts for the methane electrooxidation reaction (CH<sub>4</sub>OR). The NiCuCoMnAg HEAs achieved a Faradaic efficiency (FE) of 95.3% for ethanol (CH<sub>3</sub>CH<sub>2</sub>OH) production at 1.4&#xa0;V vs. reversible hydrogen electrode (RHE), outperforming NiCuCoAg medium-entropy alloys (MEAs) and NiCuAg low-entropy alloys (LEAs). Furthermore, in the nano-impact electrochemical system at 1.4&#xa0;V vs. RHE, the NiCuCoMnAg HEAs exhibited a significantly higher current of 0.821&#xa0;mA compared to NiCuCoAg MEAs and NiCuAg LEAs. This superior catalytic performance likely stems from the unsaturated metal sites, complex coordination environment, and high configurational entropy of the NiCuCoMnAg HEAs, which facilitate *CH<sub>3</sub> dehydrogenation and the adsorption of *CH<sub>2</sub>OH and *CH<sub>3</sub> intermediates, thereby promoting C–C coupling and ultimately enhancing CH<sub>3</sub>CH<sub>2</sub>OH production. Additionally, this work not only provides insights into the controllable synthesis of alloy materials with varying configurational entropy but also pioneers the application of HEAs in the electrocatalytic oxidation of methane to ethanol.</p> Graphical abstract <p></p>

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High-entropy alloys for enhanced electrocatalytic methane oxidation via nanoparticle-impact technique

  • 期刊论文

  • 发表日期：

    2025年9月16日

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  • Hao-Sen Xiong,
  • Ming-Xin Chen,
  • Shi-Yu Jiang,
  • Xiao-Hong Fu,
  • Shu-Yong Shang,
  • Qiang Zhang,
  • Zong-You Yin

摘要

The direct electrochemical oxidation of methane to high-value products under mild conditions holds significant economic importance, but challenges, such as insufficient active sites, poor product selectivity, and sluggish reaction kinetics, often persist. Herein, NiCuCoMnAg high-entropy alloys (HEAs) were prepared via a freeze-thaw method as highly active and selective catalysts for the methane electrooxidation reaction (CH4OR). The NiCuCoMnAg HEAs achieved a Faradaic efficiency (FE) of 95.3% for ethanol (CH3CH2OH) production at 1.4 V vs. reversible hydrogen electrode (RHE), outperforming NiCuCoAg medium-entropy alloys (MEAs) and NiCuAg low-entropy alloys (LEAs). Furthermore, in the nano-impact electrochemical system at 1.4 V vs. RHE, the NiCuCoMnAg HEAs exhibited a significantly higher current of 0.821 mA compared to NiCuCoAg MEAs and NiCuAg LEAs. This superior catalytic performance likely stems from the unsaturated metal sites, complex coordination environment, and high configurational entropy of the NiCuCoMnAg HEAs, which facilitate *CH3 dehydrogenation and the adsorption of *CH2OH and *CH3 intermediates, thereby promoting C–C coupling and ultimately enhancing CH3CH2OH production. Additionally, this work not only provides insights into the controllable synthesis of alloy materials with varying configurational entropy but also pioneers the application of HEAs in the electrocatalytic oxidation of methane to ethanol.

Graphical abstract