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Cationic Defect Engineering for Promoting Oxidation of 5-Hydroxymethylfurfural While Passivating OER.

Haodong Zheng1, Xiaoxiang Wang1, Kaile Shi1

  • 1School of Chemical Engineering, Hebei University of Technology, Tianjin 300130, China.

ACS Applied Materials & Interfaces
|August 22, 2025
PubMed
Summary

This study enhances electrochemical oxidation of 5-hydroxymethylfurfural (HMFOR) by creating cationic defects in NiMnFe-layered double hydroxide (LDH) catalysts. This method boosts HMFOR oxidation efficiency while suppressing the competing oxygen evolution reaction (OER).

Keywords:
5-hydroxymethylfurfuralNiMnFe-LDHcationic defectcharge transferelectrocatalytic reactionintermediates adsorption

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Electrochemical organic oxidation offers green, energy-efficient industrial advantages.
  • The oxygen evolution reaction (OER) competes with organic oxidation, reducing efficiency.
  • Developing selective electrocatalysts is crucial for industrial applications.

Purpose of the Study:

  • To develop a method for promoting 5-hydroxymethylfurfural oxidation (HMFOR) while suppressing OER.
  • To investigate the role of cationic defects in enhancing HMFOR electrocatalysis.
  • To provide a strategy for high-performance electrocatalyst design.

Main Methods:

  • Etching NiMnFe-layered double hydroxide (LDH) with N,N-dimethylacetamide (DMF) to create cationic defects.
  • Utilizing in situ electrochemical impedance spectroscopy to analyze reaction kinetics.
  • Employing in situ infrared spectroscopy and theoretical calculations to study reaction pathways.

Main Results:

  • The etched NiMnFe-LDH (d-NiMnFe-LDH) showed a 50 mV potential decrease for HMFOR and a 30 mV increase for OER at 50 mA cm⁻².
  • d-NiMnFe-LDH exhibited faster kinetics for HMFOR but slower kinetics for OER compared to pristine NiMnFe-LDH.
  • Cationic defects were found to enhance intermediate adsorption and lower the reaction energy barrier for HMFOR.

Conclusions:

  • DMF etching effectively creates cationic defects in NiMnFe-LDH, promoting HMFOR and suppressing OER.
  • The observed changes in reaction kinetics and energy barriers confirm the beneficial role of cationic defects.
  • This approach offers a promising strategy for designing industrial electrocatalysts for efficient organic oxidation at high current densities.