<p>Initial-anode-free lithium metal batteries offer the potential for high energy density and simplified manufacturing, positioning as a transformative platform for sustainable energy storage. However, their implementation is hindered by the low reversibility of lithium plating/stripping. Herein, we propose a dynamic integrated interface engineering strategy that incorporates an Ag-based multifunctional initiator into the electrolyte. This additive consists of Ag<sup>+</sup> paired with anions capable of generating Lewis acids, enabling electrode-electrolyte interfacial coupling through in situ polymerization, while simultaneously enhancing the lithiophilicity of current collectors via Ag<sup>+</sup>-driven in situ deposition. The controlled release of the additive regulates the solvation structure, leading to the solid electrolyte interphase with an inverted organic-rich inner/inorganic-rich outer architecture, which represents a deliberate departure from conventional models. The anion anchoring effect reinforces the self-healing capability of the interphase, ensuring the construction of fast Li-ion transport pathways and a durable protective barrier, realizing highly stable operation of initially&#xa0;anode-free quasi-solid-state batteries. Specifically, the Cu | |LiFePO<sub>4</sub> cell exhibits 90% capacity retention after 200 cycles at 0.1 C, and a 2 Ah-level pouch cell delivers a specific energy of 467 Wh kg<sup>−1</sup> based on total cell weight. This work provides an effective unified approach to address multiple interfacial challenges in initially&#xa0;anode-free lithium batteries.</p>

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Highly stable quasi-solid-state initially anode-free lithium metal batteries enabled by dynamic integrated interface engineering

  • Yunyi Chen,
  • Xitang Qian,
  • Yuxiang Lyu,
  • Yican Qiu,
  • Siyu Zhou,
  • Xinyi Lan,
  • Siqi Lu,
  • Minhua Shao

摘要

Initial-anode-free lithium metal batteries offer the potential for high energy density and simplified manufacturing, positioning as a transformative platform for sustainable energy storage. However, their implementation is hindered by the low reversibility of lithium plating/stripping. Herein, we propose a dynamic integrated interface engineering strategy that incorporates an Ag-based multifunctional initiator into the electrolyte. This additive consists of Ag+ paired with anions capable of generating Lewis acids, enabling electrode-electrolyte interfacial coupling through in situ polymerization, while simultaneously enhancing the lithiophilicity of current collectors via Ag+-driven in situ deposition. The controlled release of the additive regulates the solvation structure, leading to the solid electrolyte interphase with an inverted organic-rich inner/inorganic-rich outer architecture, which represents a deliberate departure from conventional models. The anion anchoring effect reinforces the self-healing capability of the interphase, ensuring the construction of fast Li-ion transport pathways and a durable protective barrier, realizing highly stable operation of initially anode-free quasi-solid-state batteries. Specifically, the Cu | |LiFePO4 cell exhibits 90% capacity retention after 200 cycles at 0.1 C, and a 2 Ah-level pouch cell delivers a specific energy of 467 Wh kg−1 based on total cell weight. This work provides an effective unified approach to address multiple interfacial challenges in initially anode-free lithium batteries.