Scholarlink

<p>Electrooxidation of pollutants at potentials near or below the thermodynamic hydrogen evolution potential offers transformative opportunities for energy-efficient pollutant valorization and diverse energy devices. However, existing catalysts suffer from rapid deactivation due to the inevitable overoxidation. Herein, we present an amorphous phosphorus-doped CoFe₂O₄ catalyst that achieves industrial-level current densities (1 A cm⁻²) at ultralow potentials (0.06, 0.65, and −0.17 V vs. reversible hydrogen electrode) for hydrazine, sulfion, and borohydride electrooxidation, respectively, along with 400-hour stability at 300 mA cm⁻² in a hydrazine-assisted electrolyzer. Mechanistic studies reveal electron transfer from Co-P ligands to Co-O ligands, which enhances the involvement of Co-O ligands in low-potential electrooxidation while protecting Co-P ligands from overoxidation. Furthermore, more positive charges on Co centers lower the activation barrier for such pollutant electrooxidation. This work opens a paradigm for designing robust electrocatalysts by decoupling catalytic activity from oxidative deactivation.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Surface amorphization enables robust catalyst for industrial-level low-potential electrooxidation reactions

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年7月28日

查看全文
  • Jian Chen,
  • Xin Wang,
  • Chang Sun,
  • Zheng Li,
  • Yangen Zhou,
  • Zhenhua Li,
  • Yumin Qian,
  • Mengran Wang,
  • Simin Li,
  • Yanqing Lai,
  • Shuangyin Wang

摘要

Electrooxidation of pollutants at potentials near or below the thermodynamic hydrogen evolution potential offers transformative opportunities for energy-efficient pollutant valorization and diverse energy devices. However, existing catalysts suffer from rapid deactivation due to the inevitable overoxidation. Herein, we present an amorphous phosphorus-doped CoFe₂O₄ catalyst that achieves industrial-level current densities (1 A cm⁻²) at ultralow potentials (0.06, 0.65, and −0.17 V vs. reversible hydrogen electrode) for hydrazine, sulfion, and borohydride electrooxidation, respectively, along with 400-hour stability at 300 mA cm⁻² in a hydrazine-assisted electrolyzer. Mechanistic studies reveal electron transfer from Co-P ligands to Co-O ligands, which enhances the involvement of Co-O ligands in low-potential electrooxidation while protecting Co-P ligands from overoxidation. Furthermore, more positive charges on Co centers lower the activation barrier for such pollutant electrooxidation. This work opens a paradigm for designing robust electrocatalysts by decoupling catalytic activity from oxidative deactivation.