Understanding pillar chemistry in potassium-containing polyanion materials for long-lasting sodium-ion batteries

Wenyi Liu, Wenjun Cui, Chengjun Yi, Jiale Xia, Jinbing Shang, Weifei Hu, Zhuo Wang (), Xiahan Sang, Yuanyuan Li and Jinping Liu ()
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Wenyi Liu: Wuhan University of Technology
Wenjun Cui: Wuhan University of Technology
Chengjun Yi: Wuhan University of Technology
Jiale Xia: Wuhan University of Technology
Jinbing Shang: Wuhan University of Technology
Weifei Hu: Wuhan University of Technology
Zhuo Wang: Zhengzhou University
Xiahan Sang: Wuhan University of Technology
Yuanyuan Li: Huazhong University of Science and Technology
Jinping Liu: Wuhan University of Technology

Nature Communications, 2024, vol. 15, issue 1, 1-15

Abstract: Abstract K-containing polyanion compounds hold great potential as anodes for sodium-ion batteries considering their large ion transport channels and stable open frameworks; however, sodium storage behavior has rarely been studied, and the mechanism remains unclear. Here, using a noninterference KTiOPO4 thin-film model, the Na+ storage mechanism is comprehensively revealed by in situ/operando spectroscopy, aberration-corrected electron microscopy and density functional theory calculations. We find that incomplete K+/Na+ ion exchange occurs and eventually 0.15 K+ remains as a pillar to stabilize the tunnel structure. The pillar effect substantially maintains the volume change within 3.9%, much smaller than that of K+(Na+) insertion into KTiOPO4(NaTiOPO4) (9.5%; 5%), thus enabling 10,000 cycles. The powder electrode demonstrates comparable capacity and can work efficiently at commercial-level areal capacity of 2.47 mAh cm−2. The quasi-solid-state pouch cell with high safety under extreme abuse also manifests long-term cycling stability. This pillar chemistry will inspire alkali metal ion storage in hosts containing heterogeneous cations.

Date: 2024
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DOI: 10.1038/s41467-024-54317-8

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