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CeO2 Modification Promotes the Oxidation Kinetics for Adipic Acid Electrosynthesis from KA Oil Oxidation at

Shuoshuo Guo1, Changhong Wang2, Huizhi Li1

  • 1Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.

Angewandte Chemie (International Ed. in English)
|January 12, 2025
PubMed
Summary

This study introduces NiCo2O4/CeO2 for efficient electrocatalytic oxidation of cyclohexanol to adipic acid (AA). The novel catalyst enhances reaction kinetics and Faradaic efficiency, offering a sustainable route for polymer feedstock production.

Keywords:
Adipic acidCeO2 modificationElectrocatalysisKA Oil oxidationKinetic analysis

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Adipic acid (AA) is a key polymer feedstock, traditionally produced via energy-intensive methods.
  • Electrocatalytic oxidation of cyclohexanol/cyclohexanone in water offers a sustainable alternative but suffers from slow kinetics and low Faradaic efficiency (FE).
  • A limited understanding of the reaction mechanism hinders the optimization of electrocatalytic processes for AA production.

Purpose of the Study:

  • To develop an efficient electrocatalyst for cyclohexanol oxidation to adipic acid.
  • To elucidate the reaction mechanism and understand the role of catalyst components in enhancing performance.
  • To demonstrate the practical application of the developed catalyst in a flow reactor for AA synthesis.

Main Methods:

  • Synthesis and characterization of NiCo2O4/CeO2 nanocomposite electrocatalyst.
  • Electrochemical measurements including cyclic voltammetry and chronoamperometry.
  • Mechanistic investigations using theoretical calculations and kinetic analysis.
  • Construction and operation of a two-electrode flow reactor for continuous AA production.

Main Results:

  • NiCo2O4/CeO2 catalyst achieved a high yield rate of 0.0992 mmol h⁻¹ cm⁻² and 87% FE for cyclohexanol electrooxidation to AA at a lower potential.
  • Mechanistic studies revealed a gradual oxidation pathway involving cyclohexanone intermediates.
  • Theoretical calculations indicated that electronic interactions between NiCo2O4 and CeO2 reduce activation energy for key steps and inhibit side reactions.
  • Kinetic analysis confirmed CeO2's role in promoting cyclohexanone adsorption and activation.
  • A flow reactor produced 72.1 mmol AA and 10.4 L H2 from KA oil, showcasing practical viability.

Conclusions:

  • NiCo2O4/CeO2 is a highly effective electrocatalyst for cyclohexanol oxidation to adipic acid.
  • The catalyst's performance is attributed to synergistic electronic interactions and enhanced surface kinetics.
  • The study provides crucial mechanistic insights for designing efficient electrocatalytic systems for adipic acid synthesis.
  • The demonstrated flow reactor system highlights the potential for industrial-scale sustainable production of adipic acid.