Resonance-Promoted Formic Acid Oxidation via Dynamic Electrocatalytic Modulation

Joshua Gopeesingh, M. Alexander Ardagh, Manish Shetty, Sean T. Burke, Paul J. Dauenhauer, Omar A. Abdelrahman

Research output: Contribution to journalArticlepeer-review

Abstract

It is a truth universally acknowledged that faster catalysts enable more efficient transformation of molecules to useful products and enhance the utilization of natural resources. However, the limit of static catalyst performance defined by the Sabatier principle has motivated a dynamic approach to catalyst design, whereby catalysts oscillate between varying energetic states. In this work, the concept of dynamic catalytic resonance was experimentally demonstrated via the electrocatalytic oxidation of formic acid over Pt. Oscillation of the electrodynamic potential between 0 and 0.8 V NHE via a square waveform at varying frequency (10-3 < f < 103 Hz) increased the turnover frequency to â20 s-1 at 100 Hz, over one order of magnitude (20×) faster than optimal potentiostatic conditions. We attribute the accelerated dynamic catalysis to nonfaradaic formic acid dehydration to surface-bound carbon monoxide at low potentials, followed by surface oxidation and desorption to carbon dioxide at high potentials.

Original languageEnglish (US)
Pages (from-to)9932-9942
Number of pages11
JournalACS Catalysis
Volume10
Issue number17
DOIs
StatePublished - Sep 4 2020

Bibliographical note

Funding Information:
O.A.A. and J.G. acknowledge financial support for this work from the National Science Foundation (Award No. CBET - 1932788). P.J.D., M.A.A., and M.S. acknowledge financial support of the Catalysis Center for Energy Innovation, a U.S. Department of Energy – Energy Frontier Research Center under Grant No. DE-SC0001004.

Publisher Copyright:
Copyright © 2020 American Chemical Society.

Keywords

  • catalytic resonance
  • dynamic catalysis
  • formic acid
  • oxidation
  • potentiodynamic

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