Scholarlink

<p>Electrochemical conversion of petrochemical-derived hydrocarbons to high-value oxygenates can utilize renewable energy and reduce carbon emissions. However, this involves the challenging activation of inert C(s<i>p</i><sup>3</sup>)-H bonds at room temperature. Here, we introduce an electrocatalyst:mediator assembly in which CoO<sub>x</sub> clusters-decorated IrO<sub>2</sub> electrocatalyst activates NO<sub>3</sub><sup>-</sup> mediator to a highly reactive radical capable of abstracting a hydrogen atom from benzylic C-H. The interface between CoO<sub>x</sub> and IrO<sub>2</sub> promotes NO<sub>3</sub><sup>-</sup> activation by facilitating the desorption of NO<sub>3</sub><sup>●</sup> radical for subsequent reaction. Our strategy is demonstrated through the selective oxidation of toluene to benzaldehyde with high Faradaic efficiency of 86( ±1)% at 25 mA/cm<sup>2</sup>, a factor of &gt;3 times higher than the bare electrocatalyst. The electrocatalyst:mediator assembly is operated stably for 100 h, with minimal decline in performance. When translated into a flow system, a Faradaic efficiency of 60( ±4)% at 200 mA/cm<sup>2</sup> was achieved.</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

CoOx clusters-decorated IrO2 electrocatalyst activates NO3- mediator for benzylic C-H activation

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年4月10日

查看全文
  • Ziyu Mi,
  • Yuke Li,
  • Chao Wu,
  • Mingsheng Zhang,
  • Xun Cao,
  • Shibo Xi,
  • Jia Zhang,
  • Wan Ru Leow

摘要

Electrochemical conversion of petrochemical-derived hydrocarbons to high-value oxygenates can utilize renewable energy and reduce carbon emissions. However, this involves the challenging activation of inert C(sp3)-H bonds at room temperature. Here, we introduce an electrocatalyst:mediator assembly in which CoOx clusters-decorated IrO2 electrocatalyst activates NO3- mediator to a highly reactive radical capable of abstracting a hydrogen atom from benzylic C-H. The interface between CoOx and IrO2 promotes NO3- activation by facilitating the desorption of NO3● radical for subsequent reaction. Our strategy is demonstrated through the selective oxidation of toluene to benzaldehyde with high Faradaic efficiency of 86( ±1)% at 25 mA/cm2, a factor of >3 times higher than the bare electrocatalyst. The electrocatalyst:mediator assembly is operated stably for 100 h, with minimal decline in performance. When translated into a flow system, a Faradaic efficiency of 60( ±4)% at 200 mA/cm2 was achieved.