Issue 18, 2024

Tailoring the Wadsley–Roth crystallographic shear structures for high-power lithium-ion batteries

Abstract

Exploring a universal strategy to increase Li-ion storage capacity and ionic conductivity while maintaining a robust crystal framework is a significant challenge for advancing Wadsley–Roth shear phases as promising anodes for high-power lithium-ion batteries. Here we report a potent cation-engineering driven crystallographic shear structure tailoring strategy, demonstrated through a novel titanium niobium tungsten oxide (TNWO). This is a significant model containing inspiring domains with tetrahedron, tetrahedron-free and large-size blocks in the lattice. Theoretical calculations reveal that the TNWO model, featuring the partial absence of a [WO4] tetrahedron and intrinsic multiple cation features, not only exhibits enhanced electronic conductivity and alleviated Li+ adsorbed structural distortion, but also facilitates both horizontal inter-block type and vertical-tunnel type Li+ diffusions, accompanied by sufficient redox reactions. Accordingly, it offers 1.48 Li+ per metal atom along with a high Li+ diffusion coefficient of 10−12 cm−2 s−1 and remarkable structural stability, featuring a reversible spatial phase transition. Additionally, through modification of surface anisotropy, dimensional uniformity and electronic conductivity of individual TNWO particles, a composite anode demonstrates ultrahigh rate capability (103.7 mA h g−1 at 15 A g−1) and excellent cycling stability (capacity retention of 80% at 5 A g−1 over 4900 cycles). This work is believed to have opened a new avenue for tailoring shear structures and creating unprecedented phases to transcend the existing Wadsley–Roth niobium-based oxide system for next-generation high-power lithium-ion batteries.

Graphical abstract: Tailoring the Wadsley–Roth crystallographic shear structures for high-power lithium-ion batteries

Supplementary files

Article information

Article type
Paper
Submitted
26 May 2024
Accepted
01 Aug 2024
First published
06 Aug 2024
This article is Open Access
Creative Commons BY-NC license

Energy Environ. Sci., 2024,17, 6571-6581

Tailoring the Wadsley–Roth crystallographic shear structures for high-power lithium-ion batteries

P. Jing, M. Liu, H. Ho, Y. Ma, W. Hua, H. Li, N. Guo, Y. Ding, W. Zhang, H. Chen, B. Zhao, J. Wang and M. Liu, Energy Environ. Sci., 2024, 17, 6571 DOI: 10.1039/D4EE02293A

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