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<p>The development of anode-free lithium metal batteries has enabled a key strategy for achieving high-energy-density lithium metal batteries with energy densities exceeding 500 Wh kg<sup>−1</sup>. However, anode-free batteries face critical challenges, including non-uniform lithium deposition, unstable solid-electrolyte interphase layer, and low lithium utilization efficiency. In this work, high-entropy sulfide (HES, WMoNbZrVS<sub><i>x</i></sub>) interface is designed for anode-free configurations through an <i>in situ</i> high-temperature sulfurization process. This long-range disordered layered HES surface with abundant chemically active sites facilitates both non-selective adsorption and multiple ion diffusion pathways. <i>In situ</i> analyses also confirmed the favorable interfacial stability and fast Li plating/stripping kinetics, promoting uniform lithium nucleation/growth with a dense and homogeneous lithium deposition layer. The HES interface engineering design demonstrated stable cycling performance up to 7000 h at high current densities of 60 mA cm<sup>−2</sup>/1 mAh cm<sup>−2</sup>. Moreover, the anode-free full cell exhibited a high initial Coulombic efficiency of 91.83% with a low capacity decay rate of 0.053% per cycle at 0.5 C rate within 700 cycles. This innovative HES structure demonstrates promising potential for anode-free Li metal batteries.</p>

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Nanostructured high-entropy sulfide interface engineering for accelerated Li+ kinetics in anode-free lithium metal batteries

  • 期刊论文

  • 发表日期：

    2026年1月4日

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  • Rujing Liu,
  • Ji Xue,
  • Wenlong Liu,
  • Fei Liang,
  • Jian Sun,
  • Songyu Jia,
  • Yi Gu,
  • Haizhou Zhao,
  • Yancheng Yang,
  • Qiang Zou,
  • Yao Yao,
  • Rui Tian,
  • Sizhe Wang

摘要

The development of anode-free lithium metal batteries has enabled a key strategy for achieving high-energy-density lithium metal batteries with energy densities exceeding 500 Wh kg−1. However, anode-free batteries face critical challenges, including non-uniform lithium deposition, unstable solid-electrolyte interphase layer, and low lithium utilization efficiency. In this work, high-entropy sulfide (HES, WMoNbZrVSx) interface is designed for anode-free configurations through an in situ high-temperature sulfurization process. This long-range disordered layered HES surface with abundant chemically active sites facilitates both non-selective adsorption and multiple ion diffusion pathways. In situ analyses also confirmed the favorable interfacial stability and fast Li plating/stripping kinetics, promoting uniform lithium nucleation/growth with a dense and homogeneous lithium deposition layer. The HES interface engineering design demonstrated stable cycling performance up to 7000 h at high current densities of 60 mA cm−2/1 mAh cm−2. Moreover, the anode-free full cell exhibited a high initial Coulombic efficiency of 91.83% with a low capacity decay rate of 0.053% per cycle at 0.5 C rate within 700 cycles. This innovative HES structure demonstrates promising potential for anode-free Li metal batteries.