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Cation-Vacancy Ordered Superstructure Enhanced Cycling Stability in Tungsten Bronze Anode

机译：Cation-Vacancy Ordered Superstructure Enhanced Cycling Stability in Tungsten Bronze Anode

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摘要

Niobium-based tungsten bronze oxides have recently emerged as attractive fast-charging anodes for lithium-ion batteries (LIBs), owing to their structural openings and adjustability. However, electrodes with tungsten bronze structures usually suffer from structural variability induced by Li~+ intercalation/ de-intercalation, leading to unsatisfactory cycling performance. To circumvent this limitation, a novel tetragonal tungsten bronze (TTB) structure, Ba_(3.4)Nb_(10)O_(28.4) (BNO), is developed as an anode material for LIBs with prominent cycling performance. An unprecedented cation-vacancy ordered superstructure with a periodic distribution of active and inactive sites is revealed inside the BNO. Through multiple characterizations and theoretical studies, it is demonstrated that this superstructure can improve the lithium-ion diffusion and disperse the structural strain induced by Li~+-intercalation to enable stable Li~+-storage. Benefiting from the superstructure-induced local structural stability, both the BNO bulk and Ba_(3.4)Nb_(10)O_(28.4)@C (BNO@C) microspheres can deliver >90% capacity retention after 250 cycles at 2 C and close to 90% capacity retention after 2000 cycles at 10 C. These results are of significant importance for establishing the structure–property relationship between the cation-vacancy ordered superstructure and Li~+-storage performance, facilitating the rational design of stable tungsten bronze anodes.

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