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Realizing Reversible Conversion-Alloying of Sb(V) in Polyantimonic Acid for Fast and Durable Lithium- and Potassium-Ion Storage

Journal Article


Abstract


  • Finding suitable electrode materials for alkali-metal-ion storage is vital to the next-generation energy-storage technologies. Polyantimonic acid (PAA, H2Sb2O6 · nH2O), having pentavalent antimony species and an interconnected tunnel-like pyrochlore crystal framework, is a promising high-capacity energy-storage material. Fabricating electrochemically reversible PAA electrode materials for alkali-metal-ion storage is a challenge and has never been reported due to the extremely poor intrinsic electronic conductivity of PAA associated with the highest oxidation state Sb(V). Combining nanostructure engineering with a conductive-network construction strategy, here is reported a facile one-pot synthesis protocol for crafting uniform internal-void-containing PAA nano-octahedra in a composite with nitrogen-doped reduced graphene oxide nanosheets (PAA⊂N-RGO), and for the first time, realizing the reversible storage of both Li+ and K+ ions in PAA⊂N-RGO. Such an architecture, as validated by theoretical calculations and ex/in situ experiments, not only fully takes advantage of the large-sized tunnel transport pathways (0.37 nm2) of PAA for fast solid-phase ionic diffusion but also leads to exponentially increased electrical conductivity (3.3 S cm−1 in PAA⊂N-RGO vs 4.8 × 10−10 S cm−1 in bare-PAA) and yields an inside-out buffer function for accommodating volume expansion. Compared to electrochemically irreversible bare-PAA, PAA⊂N-RGO manifests reversible conversion-alloying of Sb(V) toward fast and durable Li+- and K+-ion storage.

Authors


  •   Wang, Boya (external author)
  •   Deng, Zhiwen (external author)
  •   Xia, Yuting (external author)
  •   Hu, Jiaxuan (external author)
  •   Li, Hongju (external author)
  •   Wu, Hao (external author)
  •   Zhang, Qiaobao (external author)
  •   Zhang, Yun (external author)
  •   Liu, Hua K.
  •   Dou, Shi Xue

Publication Date


  • 2019

Citation


  • Wang, B., Deng, Z., Xia, Y., Hu, J., Li, H., Wu, H., Zhang, Q., Zhang, Y., Liu, H. & Dou, S. (2019). Realizing Reversible Conversion-Alloying of Sb(V) in Polyantimonic Acid for Fast and Durable Lithium- and Potassium-Ion Storage. Advanced Energy Materials, Online First 1903119-1-1903119-15.

Scopus Eid


  • 2-s2.0-85075180331

Ro Metadata Url


  • http://ro.uow.edu.au/aiimpapers/3935

Has Global Citation Frequency


Start Page


  • 1903119-1

End Page


  • 1903119-15

Volume


  • Online First

Place Of Publication


  • Germany

Abstract


  • Finding suitable electrode materials for alkali-metal-ion storage is vital to the next-generation energy-storage technologies. Polyantimonic acid (PAA, H2Sb2O6 · nH2O), having pentavalent antimony species and an interconnected tunnel-like pyrochlore crystal framework, is a promising high-capacity energy-storage material. Fabricating electrochemically reversible PAA electrode materials for alkali-metal-ion storage is a challenge and has never been reported due to the extremely poor intrinsic electronic conductivity of PAA associated with the highest oxidation state Sb(V). Combining nanostructure engineering with a conductive-network construction strategy, here is reported a facile one-pot synthesis protocol for crafting uniform internal-void-containing PAA nano-octahedra in a composite with nitrogen-doped reduced graphene oxide nanosheets (PAA⊂N-RGO), and for the first time, realizing the reversible storage of both Li+ and K+ ions in PAA⊂N-RGO. Such an architecture, as validated by theoretical calculations and ex/in situ experiments, not only fully takes advantage of the large-sized tunnel transport pathways (0.37 nm2) of PAA for fast solid-phase ionic diffusion but also leads to exponentially increased electrical conductivity (3.3 S cm−1 in PAA⊂N-RGO vs 4.8 × 10−10 S cm−1 in bare-PAA) and yields an inside-out buffer function for accommodating volume expansion. Compared to electrochemically irreversible bare-PAA, PAA⊂N-RGO manifests reversible conversion-alloying of Sb(V) toward fast and durable Li+- and K+-ion storage.

Authors


  •   Wang, Boya (external author)
  •   Deng, Zhiwen (external author)
  •   Xia, Yuting (external author)
  •   Hu, Jiaxuan (external author)
  •   Li, Hongju (external author)
  •   Wu, Hao (external author)
  •   Zhang, Qiaobao (external author)
  •   Zhang, Yun (external author)
  •   Liu, Hua K.
  •   Dou, Shi Xue

Publication Date


  • 2019

Citation


  • Wang, B., Deng, Z., Xia, Y., Hu, J., Li, H., Wu, H., Zhang, Q., Zhang, Y., Liu, H. & Dou, S. (2019). Realizing Reversible Conversion-Alloying of Sb(V) in Polyantimonic Acid for Fast and Durable Lithium- and Potassium-Ion Storage. Advanced Energy Materials, Online First 1903119-1-1903119-15.

Scopus Eid


  • 2-s2.0-85075180331

Ro Metadata Url


  • http://ro.uow.edu.au/aiimpapers/3935

Has Global Citation Frequency


Start Page


  • 1903119-1

End Page


  • 1903119-15

Volume


  • Online First

Place Of Publication


  • Germany