Unraveling the Mechanisms of Electrocatalytic Oxygenation and Dehydrogenation of Organic Molecules to Value-Added Chemicals Over a Ni–Fe Oxide Catalyst

Biswajit Mondal, Neeta Karjule, Chanderpratap Singh, Ran Shimoni, Michael Volokh, Idan Hod, Menny Shalom

Research output: Contribution to journalArticlepeer-review

Abstract

Electrocatalytic oxidative upgrading of organic molecules is a promising alternative process to water oxidation for clean hydrogen production. Yet, its underlying mechanism is still not fully understood, and suitable low-cost electrocatalysts with good product selectivity and activity are still sought after. Here, an active NiFeOx-based catalyst is reported on as a general platform for the electro-oxidative upgrading of organic molecules through oxygenation and dehydrogenation, with hydrogen coproduction. Detailed mechanistic studies unveil that C–H bond oxidation (with a bond dissociation energy BDEC–H of ≈88–96 kcal mol−1) is involved in the rate-limiting step, which differs significantly from the oxygen evolution reaction mechanism. These findings show that the oxidation efficacy is linearly correlated with the BDEC–H of the molecule. Thus, the catalyst can be used as a general platform for large-scale electro-oxidation of various substrates through oxygenation and dehydrogenation at high current density (25 mA cm−2), with a good Faradaic yield. The platform's generality is further demonstrated by the selective oxidation of 5-(hydroxymethyl)furfural into 2,5-furandicarboxylic acid with good efficiency.

Original languageEnglish
Article number2101858
JournalAdvanced Energy Materials
Volume11
Issue number37
DOIs
StatePublished - 1 Oct 2021

Keywords

  • electrocatalysis
  • hybrid water electrolysis
  • hydrogen production
  • reaction mechanism
  • substrate oxidation

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