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<p>Thermochemical redox catalysis is critical to a wide array of key chemical transformations and can proceed via the coupling of two electrochemical half-reactions. This electrochemical mechanism is exemplified by the platinum-catalysed aerobic oxidation of formic acid, wherein the oxygen reduction reaction is coupled to the formic acid oxidation reaction. Here using scanning electrochemical cell microscopy, we show there are grain-dependent variations in catalytic rates for the oxygen reduction and formic acid oxidation reactions at a platinum catalyst. Quantitative spatially resolved images of catalytic rates imply inter-grain cooperativity during ensemble thermochemical catalysis via lateral current flows that galvanically couple disparate active sites. Moreover, by comparing current–potential profiles of the half-reactions in isolation and in the presence of both reactants, we reveal additional site-specific chemical interactions that modify the two constituent half-reactions. These studies establish a methodology that exposes how electrochemical half-reactions couple and interact across surface structures to enable redox transformations.</p><p></p>

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Electrochemical imaging of thermochemical catalysis

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年3月5日

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  • Xiangdong Xu,
  • William C. Howland,
  • Daniel Martín-Yerga,
  • Cole S. Cadaram,
  • Deiaa M. Harraz,
  • Geoff D. West,
  • Patrick R. Unwin,
  • Yogesh Surendranath

摘要

Thermochemical redox catalysis is critical to a wide array of key chemical transformations and can proceed via the coupling of two electrochemical half-reactions. This electrochemical mechanism is exemplified by the platinum-catalysed aerobic oxidation of formic acid, wherein the oxygen reduction reaction is coupled to the formic acid oxidation reaction. Here using scanning electrochemical cell microscopy, we show there are grain-dependent variations in catalytic rates for the oxygen reduction and formic acid oxidation reactions at a platinum catalyst. Quantitative spatially resolved images of catalytic rates imply inter-grain cooperativity during ensemble thermochemical catalysis via lateral current flows that galvanically couple disparate active sites. Moreover, by comparing current–potential profiles of the half-reactions in isolation and in the presence of both reactants, we reveal additional site-specific chemical interactions that modify the two constituent half-reactions. These studies establish a methodology that exposes how electrochemical half-reactions couple and interact across surface structures to enable redox transformations.