Catalyzing Desolvation at Cathode-Electrolyte Interface Enabling High-Performance Magnesium-Ion Batteries

Rongrui Deng; Guanjie Lu; Zhongting Wang; Shuangshuang Tan; Xueting Huang; Rong Li; Menghong Li; Ronghua Wang; Chaohe Xu; Guangsheng Huang; Jingfeng Wang; Xiaoyuan Zhou; Fusheng Pan

doi:10.1002/smll.202311587

Catalyzing Desolvation at Cathode-Electrolyte Interface Enabling High-Performance Magnesium-Ion Batteries

Small. 2024 Feb 22:e2311587. doi: 10.1002/smll.202311587. Online ahead of print.

Authors

Rongrui Deng^{1

2}, Guanjie Lu³, Zhongting Wang^{1

2}, Shuangshuang Tan^{1

2}, Xueting Huang^{1

2}, Rong Li^{1

2}, Menghong Li³, Ronghua Wang^{1

2}, Chaohe Xu^{1

3}, Guangsheng Huang^{1

2}, Jingfeng Wang^{1

2}, Xiaoyuan Zhou^{1

4}, Fusheng Pan^{1

2}

Affiliations

¹ National Engineering Research Center for Magnesium Alloys, Chongqing University, Chongqing, 400044, P. R. China.
² College of Materials Science and Engineering, Chongqing University, Chongqing, 400044, P. R. China.
³ College of Aerospace Engineering, Chongqing University, Chongqing, 400044, P. R. China.
⁴ College of Physics, Chongqing University, Chongqing, 400044, P. R. China.

PMID: 38385836
DOI: 10.1002/smll.202311587

Abstract

Magnesium ion batteries (MIBs) are expected to be the promising candidates in the post-lithium-ion era with high safety, low cost and almost dendrite-free nature. However, the sluggish diffusion kinetics and strong solvation capability of the strongly polarized Mg²⁺ are seriously limiting the specific capacity and lifespan of MIBs. In this work, catalytic desolvation is introduced into MIBs for the first time by modifying vanadium pentoxide (V₂ O₅ ) with molybdenum disulfide quantum dots (MQDs), and it is demonstrated via density function theory (DFT) calculations that MQDs can effectively lower the desolvation energy barrier of Mg²⁺ , and therefore catalyze the dissociation of Mg²⁺ -1,2-Dimethoxyethane (Mg²⁺ -DME) bonds and release free electrolyte cations, finally contributing to a fast diffusion kinetics within the cathode. Meanwhile, the local interlayer expansion can also increase the layer spacing of V₂ O₅ and speed up the magnesiation/demagnesiation kinetics. Benefiting from the structural configuration, MIBs exhibit superb reversible capacity (≈300 mAh g^-1 at 50 mA g^-1 ) and unparalleled cycling stability (15 000 cycles at 2 A g^-1 with a capacity of ≈70 mAh g^-1 ). This approach based on catalytic reactions to regulate the desolvation behavior of the whole interface provides a new idea and reference for the development of high-performance MIBs.

Keywords: catalytic desolvation; diffusion kinetics; magnesium ion battery; molybdenum disulfide; vanadium oxide.

Abstract

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