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<p>Selective production of valuable glycerol chemicals, such as glycerate (which serves as an important chemical intermediate), poses a significant challenge due to the facile cleavage of C–C bonds and the presence of multiple reaction pathways. This challenge is more severe in the electro-oxidation of glycerol, which requires the development of desirable electrocatalysts. To facilitate the glycerol electro-oxidation reaction to glycerate, here we present an approach utilizing a high-entropy PtCuCoNiMn nanosurface. It exhibits exceptional activity (~200 mA cm<sup>−2</sup> at 0.75 V versus a reversible hydrogen electrode) and selectivity (75.2%). In situ vibrational measurements and theoretical calculations reveal that the exceptional glycerol electro-oxidation selectivity and activity can be attributed to the unique characteristics of the high-entropy surface, which effectively modifies the electronic structure of the exposed Pt sites. The catalyst is successfully applied in an electrolyser for long-term glycerol electro-oxidation reaction, demonstrating excellent performance (~200 mA cm<sup>−2</sup> at 1.2<i>V</i><sub>cell</sub>) over 210 h. The present study highlights that tailoring the catalytic sites at the catalyst–electrolyte interface by constructing a high-entropy surface is an effective strategy for electrochemical catalysis.</p>

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Nanoscale high-entropy surface engineering promotes selective glycerol electro-oxidation to glycerate at high current density

  • 期刊论文

  • 发表日期：

    2025年3月17日

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  • Shuibo Wang,
  • Yichao Lin,
  • Yanle Li,
  • Ziqi Tian,
  • Yu Wang,
  • Zhiyi Lu,
  • Baoxin Ni,
  • Kun Jiang,
  • Hongbo Yu,
  • Shiwei Wang,
  • Hongfeng Yin,
  • Liang Chen

摘要

Selective production of valuable glycerol chemicals, such as glycerate (which serves as an important chemical intermediate), poses a significant challenge due to the facile cleavage of C–C bonds and the presence of multiple reaction pathways. This challenge is more severe in the electro-oxidation of glycerol, which requires the development of desirable electrocatalysts. To facilitate the glycerol electro-oxidation reaction to glycerate, here we present an approach utilizing a high-entropy PtCuCoNiMn nanosurface. It exhibits exceptional activity (~200 mA cm−2 at 0.75 V versus a reversible hydrogen electrode) and selectivity (75.2%). In situ vibrational measurements and theoretical calculations reveal that the exceptional glycerol electro-oxidation selectivity and activity can be attributed to the unique characteristics of the high-entropy surface, which effectively modifies the electronic structure of the exposed Pt sites. The catalyst is successfully applied in an electrolyser for long-term glycerol electro-oxidation reaction, demonstrating excellent performance (~200 mA cm−2 at 1.2Vcell) over 210 h. The present study highlights that tailoring the catalytic sites at the catalyst–electrolyte interface by constructing a high-entropy surface is an effective strategy for electrochemical catalysis.