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Identification and manipulation of dynamic active site deficiency-induced competing reactions in electrocatalytic oxidation processes

  • Lin, R
  • Kang, L
  • Zhao, T
  • Feng, J
  • Celorrio, V
  • Zhang, G
  • Cibin, G
  • Kucernak, A
  • Brett, DJL
  • Corà, F
  • Parkin, IP
  • He, G
Publication Date
Mar 21, 2022
UPCommons. Portal del coneixement obert de la UPC
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Electrocatalytic organic compound oxidation reactions (OCORs) have been intensively studied for energy and environmentally benign applications. However, relatively little effort has been devoted to developing a fundamental understanding of OCORs, including the detailed competition with side reactions and activity limitations, thus inhibiting the rational design of high-performance electrocatalysts. Herein, by taking the NiWO4-catalysed urea oxidation reaction (UOR) in aqueous media as an example, the competition between the OCOR and the oxygen evolution reaction (OER) within a wide potential range is examined. It is shown that the root of the competition can be ascribed to insufficient surface concentration of dynamic Ni3+, an active site shared by both the UOR and OER. A similar phenomenon is observed in other OCOR electrocatalysts and systems. To address the issue, a “controllable reconstruction of pseudo-crystalline bimetal oxides” design strategy is proposed to maximise the dynamic Ni3+ population and manipulate the competition between the UOR and the OER. The optimised electrocatalyst delivers best-in-class performance and an ∼10-fold increase in current density at 1.6 V versus the reversible hydrogen electrode for alkaline urea electrolysis compared to those of the pristine materials.

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