Dual-interface engineering via boron pre-anchoring and electronegative synergy for coupled ion transport and self-stabilizing interphases in lithium metal batteries

Abstract

Lithium metal anodes hold immense promise for next-generation high-energy-density batteries due to their outstanding theoretical capacity and low electrochemical potential. Despite these advantages, their practical implementation remains restricted by the unstable solid electrolyte interphase (SEI) and the uncontrollable lithium dendrite growth, which compromise cycling stability and safety. In this work, we propose a dual-interface engineering approach involving boron pre-anchoring in lithium anodes and coordination with electronegative components. This design establishes coupled mechanisms for ion transport optimization and self-stabilizing interphase formation through a hierarchical interface architecture. Theoretical simulations reveal that pre-embedded boron atoms lower the adsorption energy for lithium-ion diffusion while directing homogeneous metal deposition. Consequently, symmetric cells deliver stable Li plating/stripping behavior for over 2500 h at 0.5 mA cm^-2. Full cells paired with LiCoO₂ retain 92 % capacity after 200 cycles, while Li-B||NCM811 pouch cells (6.5Ah) exhibit a high energy density of 526 Wh kg⁻¹ and maintain 95 % capacity retention after 60 cycles. The interfacial design principles provide a blueprint for synchronizing ion transport kinetics and chemical stability in high-performance lithium metal batteries.