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<p>As a promising cathode material for Li/MnO<sub>2</sub> primary batteries, β‑MnO<sub>2</sub> suffers from sluggish ion diffusion kinetics and limited high‑rate capability. Vanadium doping is herein proposed to tune its crystal structure and electrochemical performance. Hollow porous V-doped β‑MnO<sub>2</sub> microspheres rich in oxygen vacancies were synthesized via a hydrothermal route combined with two-step calcination. Structural characterizations reveal that 2% V doping maintains the intrinsic crystal phase of β-MnO<sub>2</sub> while simultaneously triggering lattice expansion, enlarging the specific surface area and generating abundant oxygen vacancies. Four-probe electrical measurements and GITT confirm the enhanced electronic conductivity and Li⁺ ionic transport in V-modified β-MnO<sub>2</sub>, respectively. Electrochemical measurements demonstrate that the 2%V-MnO<sub>2</sub> cathode exhibits discharge capacities of 249.1 mAh g<sup>− 1</sup> at 0.1&#xa0;C and 223.3 mAh g<sup>− 1</sup> at 1&#xa0;C, corresponding to a capacity retention of 89.6%. Such electrochemical performance surpasses that of pristine MnO<sub>2</sub> and 4%V-MnO<sub>2</sub> samples. High-temperature aging storage experiments verify that moderate V doping significantly suppresses self-discharge and improves the long-term shelf stability of the battery. DFT calculations elucidate that V doping lowers oxygen vacancy formation energy and narrows band gap of β-MnO<sub>2</sub>. This study demonstrates that moderate V doping combined with the hollow porous structure can synergistically accelerate electron transport and ion diffusion kinetics of β-MnO<sub>2</sub>, providing a feasible pathway for developing high-power cathode materials for Li/MnO<sub>2</sub> primary batteries.</p>

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Oxygen vacancy-enriched V-doped β-MnO2 as cathode for lithium primary batteries

  • 期刊论文

  • 发表日期：

    2026年7月27日

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  • Tao Chen,
  • Zhiyong Yu,
  • Guanghui Bi,
  • Hanxing Liu

摘要

As a promising cathode material for Li/MnO2 primary batteries, β‑MnO2 suffers from sluggish ion diffusion kinetics and limited high‑rate capability. Vanadium doping is herein proposed to tune its crystal structure and electrochemical performance. Hollow porous V-doped β‑MnO2 microspheres rich in oxygen vacancies were synthesized via a hydrothermal route combined with two-step calcination. Structural characterizations reveal that 2% V doping maintains the intrinsic crystal phase of β-MnO2 while simultaneously triggering lattice expansion, enlarging the specific surface area and generating abundant oxygen vacancies. Four-probe electrical measurements and GITT confirm the enhanced electronic conductivity and Li⁺ ionic transport in V-modified β-MnO2, respectively. Electrochemical measurements demonstrate that the 2%V-MnO2 cathode exhibits discharge capacities of 249.1 mAh g− 1 at 0.1 C and 223.3 mAh g− 1 at 1 C, corresponding to a capacity retention of 89.6%. Such electrochemical performance surpasses that of pristine MnO2 and 4%V-MnO2 samples. High-temperature aging storage experiments verify that moderate V doping significantly suppresses self-discharge and improves the long-term shelf stability of the battery. DFT calculations elucidate that V doping lowers oxygen vacancy formation energy and narrows band gap of β-MnO2. This study demonstrates that moderate V doping combined with the hollow porous structure can synergistically accelerate electron transport and ion diffusion kinetics of β-MnO2, providing a feasible pathway for developing high-power cathode materials for Li/MnO2 primary batteries.