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<p>The electrochemical potential of a catalyst defines the free-energy landscape of catalysis in liquid media and is readily measured for catalysts supported on conductive materials or wired to external circuits. However, the potential is difficult to quantify for thermochemical catalysts supported on electrical insulators, thereby impeding a unifying understanding of the role of electrochemical polarization during thermochemical catalysis. Here we develop a methodology to quantify the electrochemical potential of metal catalysts supported on insulators by introducing low concentrations of redox-active molecules that establish wireless electrical connections between the catalyst and a sensing electrode. Using this approach in tandem with simultaneous rate measurements, we demonstrate distinct rate-potential scalings for oxidative dehydrogenation of formic acid on SiO<sub>2</sub>-supported and Al<sub>2</sub>O<sub>3</sub>-supported versus TiO<sub>2</sub>-supported Pt and find deactivation modes specific to SiO<sub>2</sub>-supported Pt. These developments enable the comprehensive investigation of the role of electrochemical polarization in thermochemical catalysis and complement the existing toolkit for mechanistic investigation in catalysis.</p><p></p>

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Wireless potentiometry of thermochemical heterogeneous catalysis

  • 期刊论文

  • 发表日期：

    2025年4月2日

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  • Neil K. Razdan,
  • Karl S. Westendorff,
  • Yogesh Surendranath

摘要

The electrochemical potential of a catalyst defines the free-energy landscape of catalysis in liquid media and is readily measured for catalysts supported on conductive materials or wired to external circuits. However, the potential is difficult to quantify for thermochemical catalysts supported on electrical insulators, thereby impeding a unifying understanding of the role of electrochemical polarization during thermochemical catalysis. Here we develop a methodology to quantify the electrochemical potential of metal catalysts supported on insulators by introducing low concentrations of redox-active molecules that establish wireless electrical connections between the catalyst and a sensing electrode. Using this approach in tandem with simultaneous rate measurements, we demonstrate distinct rate-potential scalings for oxidative dehydrogenation of formic acid on SiO2-supported and Al2O3-supported versus TiO2-supported Pt and find deactivation modes specific to SiO2-supported Pt. These developments enable the comprehensive investigation of the role of electrochemical polarization in thermochemical catalysis and complement the existing toolkit for mechanistic investigation in catalysis.