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<p>Regulating the nucleation and growth of Li metal is crucial for achieving stable high-energy-density Li metal batteries (LMBs) without dendritic Li growth, severe volume expansion, and “dead Li” accumulation. Herein, we present a modulation layer composed of porous SnP<sub>0.94</sub>/CoP <i>p-n</i> heterojunction particles (SCP), synthesized applying the Kirkendall effect. The unique heterointerfaces in the SCP induce a fully ionized depletion region and built-in electric field. This provides strong Li affinity, additional adsorption sites, and facilitated electron transfer, thereby guiding dendrite-free Li nucleation/growth with a low Li deposition overpotential. Moreover, the strategic design of the SCP, accounting for its reaction with Li, yields electronically conductive Co, lithiophilic Li–Sn alloy, and ionic conductive Li<sub>3</sub>P during progressive cycles. The mixed electronic and ionic conductor (MEIC) ensure the long-term stability of the SCP modulation layer. With this layer, the SCP@Li symmetric cell maintains a low overpotential for 750 cycles even at a high current density of 5 mA cm<sup>−2</sup>. Additionally, the LiFePO<sub>4</sub>//SCP@Li full cell achieves an imperceptible capacity decay of 0.03% per cycle for 800 cycles at 0.5 C. This study provides insight into MEIC heterostructures for high-performance LMBs.</p>

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Designing Metal Phosphide Solid-Electrolyte Interphase for Stable Lithium Metal Batteries Through Electrified Interface Optimization and Synergistic Conversion

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年6月27日

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  • Jung Been Park,
  • Changhoon Choi,
  • Min Sang Kim,
  • Hyeongbeom Kang,
  • Eunji Kwon,
  • Seungho Yu,
  • Dong-Wan Kim

摘要

Regulating the nucleation and growth of Li metal is crucial for achieving stable high-energy-density Li metal batteries (LMBs) without dendritic Li growth, severe volume expansion, and “dead Li” accumulation. Herein, we present a modulation layer composed of porous SnP0.94/CoP p-n heterojunction particles (SCP), synthesized applying the Kirkendall effect. The unique heterointerfaces in the SCP induce a fully ionized depletion region and built-in electric field. This provides strong Li affinity, additional adsorption sites, and facilitated electron transfer, thereby guiding dendrite-free Li nucleation/growth with a low Li deposition overpotential. Moreover, the strategic design of the SCP, accounting for its reaction with Li, yields electronically conductive Co, lithiophilic Li–Sn alloy, and ionic conductive Li3P during progressive cycles. The mixed electronic and ionic conductor (MEIC) ensure the long-term stability of the SCP modulation layer. With this layer, the SCP@Li symmetric cell maintains a low overpotential for 750 cycles even at a high current density of 5 mA cm−2. Additionally, the LiFePO4//SCP@Li full cell achieves an imperceptible capacity decay of 0.03% per cycle for 800 cycles at 0.5 C. This study provides insight into MEIC heterostructures for high-performance LMBs.