Plasma Coupled Electrolyte Additive Strategy for Construction of High‐Performance Solid Electrolyte Interphase on Li Metal Anodes

Abstract High‐performance lithium metal anodes are crucial for the development of advanced Li metal batteries. Herein, this work reports a novel plasma coupled electrolyte additive strategy to prepare high‐quality composite solid electrolyte interphase (SEI) on Li metal to achieve enhanced performance and stability. With the guidance of calculations, this work selects diethyl dibromomalonate (DB) as an additive to optimize the solvation structure of electrolytes to modify the SEI. Meanwhile, this work groundbreakingly develops DB plasma technology coupled with DB electrolyte additive to construct a combinatorial SEI: inner plasma‐induced SEI layer composed of LiBr and Li 2 CO 3 plus additive‐reduced SEI containing LiBr/Li 2 CO 3 /organic lithium compounds as an outer compatible layer. The optimized hybrid SEI has strong affinity toward Li + and good mechanical properties, thereby inducing horizontal dispersion and uniform deposition of Li + and keep structure stable. Accordingly, the symmetrical cells exhibit enhanced cycling stability for 1200 h at an overpotential of 23.8 mV with average coulombic efficiency (99.51%). Additionally, the full cells with LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode deliver a capacity retention of 81.7% after 300 cycles at 0.5 C, and the pouch cell achieves a volumetric specific energy of ≈664 Wh L ‒1 . This work provides new enlightenment on plasma technology for fabrication of advanced metal anodes for energy storage.