4.8 Article

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

期刊

ADVANCED ENERGY MATERIALS
卷 12, 期 36, 页码 -

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202201967

关键词

anodes; cycling performance; Li; (+) storage; superstructure; tungsten bronze

资金

  1. National Natural Science Foundation of China [51725101, 11727807, 51672050, 61790581, 22088101]
  2. Ministry of Science and Technology of China (973 Project) [2018YFA0209102, 2021YFA1200600]
  3. Infrastructure and Facility Construction Project of Zhejiang Laboratory

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A novel tetragonal tungsten bronze structure with an unprecedented cation-vacancy ordered superstructure is developed, which improves the cycling performance of lithium-ion batteries by enhancing lithium-ion diffusion and reducing structural strain induced by lithium-ion intercalation.
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, Ba3.4Nb10O28.4 (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 Ba3.4Nb10O28.4@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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