Citation: Haoyu Fang, Kai Yong, Boya Wang, Kaipeng Wu, Yun Zhang, Hao Wu. V-substituted pyrochlore-type polyantimonic acid for highly enhanced lithium-ion storage[J]. Chinese Chemical Letters, ;2023, 34(5): 107545. doi: 10.1016/j.cclet.2022.05.059 shu

V-substituted pyrochlore-type polyantimonic acid for highly enhanced lithium-ion storage

College of Materials Science and Engineering, Sichuan University, Chengdu 610064, China

wukaipeng@scu.edu.cn

hao.wu@scu.edu.cn

Received Date: 26 April 2022
Revised Date: 10 May 2022
Accepted Date: 18 May 2022
Available Online: 23 May 2022

Figures(6)

Pyrochlore-structured polyantimonic acid (PAA) is a potential high-capacity electrode material, but its innately poor electroconductivity (~10⁻¹⁰ S/cm) seriously impairs its electrochemical reversibility for lithium-ion storage. Herein, we report design and synthesis of a novel V-substituted PAA (PAA-V), where V⁵⁺ are introduced to partially replace Sb⁵⁺. Owing to identical valence and close ionic radius relative to Sb⁵⁺, the V⁵⁺ cation can constitute the covalent VO₆ octahedra framework without changing the pyrochlore crystal structure of PAA. As a result, the V⁵⁺-substitution is capable to modulate the electronic structure of PAA with significantly improved electrical conductivity (~10⁻⁶ S/cm for PAA-V) and meanwhile decreases the size of crystals with reduced diffusion length for Li⁺-ions. With varying the ratio of V⁵⁺-substitution, the PAA-V with optimized substitution molar ratio (18%) exhibits the best lithium-ion storage performance, delivering a long cycling life with high reversible capacity (731 mAh/g after 1200 cycles at 1 A/g) and outstanding rate capability (279 mAh/g at 15 A/g). More importantly, by pairing the PAA-V as anode and commercial LiFePO₄ as cathode, the full cell with a limited negative/positive capacity ratio of 1.2 exhibits decent cycling stability at 1 C after 150 cycles with 85.5% capacity retention.
- Lithium-ion batteries,
- Anode materials,
- Polyantimonic acid,
- Element substitution,
- Electrochemical reaction mechanism
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