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Enhancing Capacity and Rate Performance of Lamellar V2O5 Cathode Materials by Modulating Vanadium 3d Orbital Splitting

Xiu-Fen Ma1,*, Bai-Qing Zhao2,*, Qing Zhong1, Hongyu Liu1, Hong-Yi Li1,3,†, Xie Zhang4,‡, Jiang Diao1,3, Jili Yue1,3, Guangsheng Huang1,3 et al.

Jingfeng Wang1,3 and Fusheng Pan1,3,5

  • *These authors contributed equally to this work
  • †Contact author: hongyi.li@cqu.edu.cn
  • ‡Contact author: xie.zhang@nwpu.edu.cn
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PRX Energy 4, 033008 – Published 19 August, 2025

DOI: https://doi.org/10.1103/9wnj-xv2w

Abstract

Magnesium-ion batteries (MIBs) are promising next-generation energy storage devices. Vanadium oxides are promising cathode materials for MIBs due to their rich chemical valences and versatile structures. However, vanadium oxide cathodes face challenges such as low structural stability, slow Mg2+ diffusion kinetics, and low electrical conductivity. The work reported herein used hydrothermal synthesis to pre-intercalate H2O molecules and Mg2+ into V2O5 interlayers to stabilize the lamellar structure and modulate V 3d orbital splitting, leading to a Mg0.2V2O5⋅1.5H2O cathode (MVOH1). The V 3d orbital splitting facilitates electron hopping between V4+ and V5+ cations, leading to the enhanced conductivity of MVOH1; it also makes it easier for V atoms to acquire and lose electrons during discharging and charging, leading to high capacity and high rate capability of MVOH1. Consequently, the MVOH1 cathode exhibited a high specific capacity of 300 mA h g−1 at a current density of 0.05 A g−1 and retained a specific capacity of 85 mA h g−1 at 10 A g−1; the capacity and rate capability surpass those of previously reported V2O5 cathode materials. The aqueous MIB based on MVOH1 demonstrated an ultralong lifespan of 11 000 cycles, which is significantly longer than that of previously reported aqueous MIBs. This study highlights the synergistic effect of regulating interlayer spacing and V 3d orbital splitting on electrochemical performance, which is crucial for developing more efficient and more durable energy storage systems.

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Popular Summary

Magnesium-ion batteries are promising secondary batteries, but they suffer from relatively low cathode capacity and short lifespan due to sluggish Mg2+ migration kinetics. Current strategies focus on the enlargement of the Mg2+ migration pathway, overlooking opportunities unlocked by changes to the transition metal orbitals. Here the authors investigate the effect of vanadium 3d orbital splitting on the Mg2+ migration kinetics in a V2O5 cathode. They find that modulating the V 3d orbital splitting increases the electronic conductivity and electron-accepting capability of V2O5, leading to ultrahigh capacity and ultralong lifespan. Such cathode material design incorporating transition metal orbital splitting can be a strategy to boost battery performance.

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PRX Energy 4, 033008– Published 19 August, 2025
  • Received 14 January 2025
  • Revised 8 May 2025
  • Accepted 21 July 2025
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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