Surface amorphization enables robust catalyst for industrial-level low-potential electrooxidation reactions

Jian Chen, Xin Wang, Chang Sun, Zheng Li, Yangen Zhou (), Zhenhua Li, Yumin Qian (), Mengran Wang, Simin Li, Yanqing Lai () and Shuangyin Wang ()
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Jian Chen: Central South University
Xin Wang: Zhejiang Wanli University
Chang Sun: Beijing Institute of Technology
Zheng Li: Hunan University of Science and Technology
Yangen Zhou: Central South University
Zhenhua Li: Central South University
Yumin Qian: Beijing Institute of Technology
Mengran Wang: Central South University
Simin Li: Central South University
Yanqing Lai: Central South University
Shuangyin Wang: Zhejiang Wanli University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Electrooxidation of pollutants at potentials near or below the thermodynamic hydrogen evolution potential offers transformative opportunities for energy-efficient pollutant valorization and diverse energy devices. However, existing catalysts suffer from rapid deactivation due to the inevitable overoxidation. Herein, we present an amorphous phosphorus-doped CoFe₂O₄ catalyst that achieves industrial-level current densities (1 A cm⁻²) at ultralow potentials (0.06, 0.65, and −0.17 V vs. reversible hydrogen electrode) for hydrazine, sulfion, and borohydride electrooxidation, respectively, along with 400-hour stability at 300 mA cm⁻² in a hydrazine-assisted electrolyzer. Mechanistic studies reveal electron transfer from Co-P ligands to Co-O ligands, which enhances the involvement of Co-O ligands in low-potential electrooxidation while protecting Co-P ligands from overoxidation. Furthermore, more positive charges on Co centers lower the activation barrier for such pollutant electrooxidation. This work opens a paradigm for designing robust electrocatalysts by decoupling catalytic activity from oxidative deactivation.

Date: 2025
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DOI: 10.1038/s41467-025-62293-w

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