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<p>The development of low-cost platinum-free electrocatalysts for the oxygen reduction reaction (ORR) is essential for the sustainable energy technologies. In this work, spinel-type LiMn<sub>2</sub>O<sub>4</sub> was chemically modified via proton exchange to systematically investigate the effects of protonation on crystal structure, electronic configuration, and ORR performance. Experimental results reveal that proton exchange not only regulates the lattice parameters and Mn oxidation states, but also enhances surface hydrophilicity and oxygen adsorption capacity, leading to a significant improvement in ORR activity with at a half-wave potential of 0.81 V for pure Mn-based oxide. Physical characterizations and theoretical calculations reveal that protonation optimizes the surface electronic structure by mitigating the over-stabilization of oxygen intermediates on LiMn<sub>2</sub>O<sub>4</sub>, thus facilitating the rate-determining step *OH adsorption and improving reaction kinetics. This work establishes proton exchange as a versatile strategy for the construction of Mn-based oxide electrocatalysts containing alkali metals, offering valuable insights for the rational design of nonprecious metal catalysts in energy conversion applications.</p>

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Enhanced oxygen reduction reaction performance of spinel lithium manganese oxide via proton exchange

  • 期刊论文

  • 发表日期：

    2026年1月10日

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  • Jiayi Li,
  • Shengxi Zhao,
  • Zhiwei Hu,
  • Xuepeng Zhong,
  • Nicolas Alonso-Vante,
  • Jiwei Ma

摘要

The development of low-cost platinum-free electrocatalysts for the oxygen reduction reaction (ORR) is essential for the sustainable energy technologies. In this work, spinel-type LiMn2O4 was chemically modified via proton exchange to systematically investigate the effects of protonation on crystal structure, electronic configuration, and ORR performance. Experimental results reveal that proton exchange not only regulates the lattice parameters and Mn oxidation states, but also enhances surface hydrophilicity and oxygen adsorption capacity, leading to a significant improvement in ORR activity with at a half-wave potential of 0.81 V for pure Mn-based oxide. Physical characterizations and theoretical calculations reveal that protonation optimizes the surface electronic structure by mitigating the over-stabilization of oxygen intermediates on LiMn2O4, thus facilitating the rate-determining step *OH adsorption and improving reaction kinetics. This work establishes proton exchange as a versatile strategy for the construction of Mn-based oxide electrocatalysts containing alkali metals, offering valuable insights for the rational design of nonprecious metal catalysts in energy conversion applications.