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<p>The electrooxidation of biomass-derived glycerol provides a sustainable pathway for co-producing hydrogen and value-added chemicals, yet its efficiency is critically hindered by the competitive adsorption of reactants and the parasitic oxygen evolution (OER) at high potentials. Here, we propose an active-site decoupling strategy via fluorine doping in spinel CuCo<sub>2</sub>O<sub>4</sub> (CuCo<sub>2</sub>O<sub>4</sub>-F) to simultaneously enhance glycerol electrooxidation and suppress OER. The introduced fluorine atoms reconfigure the electronic structure and induce spatial segregation of active sites, thereby OH<sup>−</sup> preferentially adsorbs on Co centers while glycerol binds to Cu sites. This cooperative adsorption accelerates glycerol oxidation kinetics and switches the OER pathway from a facile lattice oxygen mechanism (LOM) to a sluggish adsorbate evolution mechanism (AEM), thus effectively mitigating parasitic OER. The optimized CuCo<sub>2</sub>O<sub>4</sub>-F electrocatalyst achieves a record-high Faradaic efficiency (&gt;90%) toward formate at 1.6 V <i>vs.</i> RHE and maintains &gt;90% efficiency at 200 mA cm<sup>−2</sup> for over 200 h. When integrated into a membrane electrode assembly (MEA), the system demonstrates exceptional durability and a projected economic benefit of $633 t<sup>−1</sup> of glycerol processed. This work establishes active-site decoupling as a general design principle for developing high-performance, energy-efficient electrocatalysts beyond glycerol oxidation.</p>

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Active site decoupling via fluorine doping in spinel CuCo2O4 for concurrent selective glycerol electrooxidation and OER suppression

  • 期刊论文

  • 发表日期：

    2026年3月30日

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  • Yajie Wang,
  • Mingkun Jiang,
  • Yuwei Li,
  • Fangwen Ye,
  • Yanan Li,
  • Xianbao Duan,
  • Dan Wu,
  • Jing-Li Luo

摘要

The electrooxidation of biomass-derived glycerol provides a sustainable pathway for co-producing hydrogen and value-added chemicals, yet its efficiency is critically hindered by the competitive adsorption of reactants and the parasitic oxygen evolution (OER) at high potentials. Here, we propose an active-site decoupling strategy via fluorine doping in spinel CuCo2O4 (CuCo2O4-F) to simultaneously enhance glycerol electrooxidation and suppress OER. The introduced fluorine atoms reconfigure the electronic structure and induce spatial segregation of active sites, thereby OH− preferentially adsorbs on Co centers while glycerol binds to Cu sites. This cooperative adsorption accelerates glycerol oxidation kinetics and switches the OER pathway from a facile lattice oxygen mechanism (LOM) to a sluggish adsorbate evolution mechanism (AEM), thus effectively mitigating parasitic OER. The optimized CuCo2O4-F electrocatalyst achieves a record-high Faradaic efficiency (>90%) toward formate at 1.6 V vs. RHE and maintains >90% efficiency at 200 mA cm−2 for over 200 h. When integrated into a membrane electrode assembly (MEA), the system demonstrates exceptional durability and a projected economic benefit of $633 t−1 of glycerol processed. This work establishes active-site decoupling as a general design principle for developing high-performance, energy-efficient electrocatalysts beyond glycerol oxidation.