Issue 16, 2024

A large-capacity, superhigh-rate integrated lithium metal anode with top-down composition gradient enabled by polyantimonic acid

Abstract

Interface engineering is an effective approach to solving the difficult Li-dendrite issues in lithium–metal batteries, and yet a robust large-capacity Li anode (≥20 mA h cm−2) working at an ultrahigh rate density (≥20 mA cm−2) is still rarely achieved. Herein, an integrated Li–metal-based anode with a top-down composition gradient (Li2O–LiOH–Li3Sb/Li) is constructed through a thermal-induced reaction of molten Li with polyantimonic acid (PAA). Unexpectedly, the lattice-water-containing PAA is found in favor of a mild but homogeneous lithiation reaction, whilst accompanied by a spontaneous phase separation between the resulting Li2O, LiOH, and Li3Sb components due to their significant interfacial energy discrepancy. The consequent Li2O-enriched top layer affording a high Young's modulus (>10 GPa) and electron-shielding ability can effectually suppress the Li-dendrite growth, while the underlying LiOH–Li3Sb interphase as ionic-channels homogenize Li+-flux distribution, in turn enabling dendrite-free Li deposition in a lithiophilic Li3Sb/Li bottom layer. With this free-standing integrated electrode, large-areal-capacity symmetrical cells (25 mA h cm−2) can maintain over 1280 h Li plating/stripping cycles at an ultrahigh-current-density of 50 mA cm−2, and the full-cells paired with high-capacity LiCoO2 (3.5 mA h cm−2) exhibit improved cycling stability under a practical low N/P ratio (1.33). Importantly, this robust integrated anode also showcases decent compatibility with gel-polymer/Li7La3Zr2O12 solid-state electrolytes, signifying the application potential in safe Li–metal batteries.

Graphical abstract: A large-capacity, superhigh-rate integrated lithium metal anode with top-down composition gradient enabled by polyantimonic acid

Supplementary files

Article information

Article type
Paper
Submitted
08 Dec 2023
Accepted
30 Apr 2024
First published
01 May 2024

Energy Environ. Sci., 2024,17, 5819-5832

A large-capacity, superhigh-rate integrated lithium metal anode with top-down composition gradient enabled by polyantimonic acid

Y. Zhang, Y. Guo, K. Yong, Q. Wang, M. Yao, Y. Zhang and H. Wu, Energy Environ. Sci., 2024, 17, 5819 DOI: 10.1039/D3EE04243J

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