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Engineering Gradient D-d Orbital Occupancy to Boost Substrate Adsorption for Efficient Electrocatalytic Biomass

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Summary

This study enhances electrocatalysis for converting biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) using Mn-modified nickel catalysts. The optimized catalyst achieves high efficiency and stability for sustainable polymer production.

Keywords:
2,5‐Furandicarboxylic acid5‐HydroxymethylfurfuralElectronic orbital structureMEA electrolyzerUltra‐high current density

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Electrocatalysis offers a sustainable route for biomass upgrading.
  • 5-hydroxymethylfurfural (HMF) conversion to 2,5-furandicarboxylic acid (FDCA) is key for polymer production.
  • Tuning catalyst electronic structure is vital for efficient HMF electrooxidation.

Purpose of the Study:

  • To investigate the effect of Mn modification on Ni-based electrocatalysts for HMF electrooxidation.
  • To understand the relationship between electronic structure (electron gradient orbitals, spin state) and catalytic activity.
  • To achieve high current density and stable FDCA production.

Main Methods:

  • Synthesis of Mn-modified porous metallic skeleton Ni electrocatalysts.
  • Electrochemical characterization of catalysts for HMF electrooxidation.
  • Analysis of electronic structure and its correlation with catalytic performance.
  • Continuous flow electrolysis experiments for stability assessment.

Main Results:

  • Mn introduction weakens e-e repulsion via π-donation, tuning the electronic structure.
  • Achieved ultra-high current density of 1.2 A cm⁻² at 1.42 V vs RHE for HMF electrooxidation.
  • Demonstrated stable FDCA production with 88.3% yield after ~300 h in continuous flow electrolysis.

Conclusions:

  • The electron gradient orbitals-activity relationship provides guidance for designing efficient electrocatalysts.
  • Mn-modified Ni catalysts show significant potential for sustainable biomass upgrading.
  • This work advances the electrocatalytic conversion of HMF to FDCA for polymer applications.