Wireless potentiometry of thermochemical heterogeneous catalysis

IF 42.8 1区化学 Q1 CHEMISTRY, PHYSICAL

Nature Catalysis Pub Date : 2025-04-02 DOI:10.1038/s41929-025-01308-7

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

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Abstract

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.

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来源期刊

Nature Catalysis Chemical Engineering-Bioengineering

CiteScore

52.10

自引率

1.10%

发文量

140

期刊介绍： Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry. Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.