Regulation of Catalyst Immediate Environment Enables Acidic Electrochemical Benzyl Alcohol Oxidation to Benzaldehyde

G. Shiva Shanker, Arnab Ghatak, Shahar Binyamin, Rotem Balilty, Ran Shimoni, Itamar Liberman, Idan Hod

Research output: Contribution to journalArticlepeer-review

Abstract

Electrocatalytic alcohol oxidation in acid offers a promising alternative to the kinetically sluggish water oxidation reaction toward low-energy H2 generation. However, electrocatalysts driving active and selective acidic alcohol electrochemical transformation are still scarce. In this work, we demonstrate efficient alcohol-to-aldehyde conversion achieved by reticular chemistry-based modification of the catalyst’s immediate environment. Specifically, coating a Bi-based electrocatalyst with a thin layer of metal-organic framework (MOF) substantially improves its performance toward benzyl alcohol electro-oxidation to benzaldehyde in a 0.1 M H2SO4 electrolyte. Detailed analysis reveals that the MOF adlayer influences catalysis by increasing the reactivity of surface hydroxides as well as weakening the catalyst-benzaldehyde binding strength. In turn, low-potential (0.65 V) cathodic H2 evolution was obtained through coupling it with anodic benzyl alcohol electro-oxidation. Consequently, the presented approach could be implemented in a wide range of electrocatalytic oxidation reactions for energy-conversion application.

Original languageEnglish
Pages (from-to)5654-5661
Number of pages8
JournalACS Catalysis
Volume14
Issue number8
DOIs
StatePublished - 19 Apr 2024

Keywords

  • UiO-66
  • catalyst microenvironment
  • electrocatalysis
  • intermediate binding
  • metal−organic framework (MOF)

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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