Organosilane Plasma Enhanced Interfacial Engineering to Boost Inorganic‐Rich Hybrid Solid Electrolyte Interface for Advanced Lithium Metal Batteries

Abstract The design and development of high‐performance artificial solid‐electrolyte interphase (SEI) are crucial for constructing advanced lithium metal anodes, as they critically stabilize the electrode‐electrolyte interface. Herein, a facile plasma‐enhanced interfacial engineering strategy to construct a robust inorganic‐rich hybrid SEI on Li metal anodes using octamethyltrisiloxane (OMTS) plasma is reported. This process forms a hybrid SEI layer comprising primarily an inner inorganic‐rich layer (e.g., Li 2 SiO 3 , Li 2 CO 3 , Li x Si) and an outer organic‐rich layer (lithium compounds). The formation mechanism is attributed to interfacial reactions between Li and OMTS plasma‐generated radicals. Theoretical calculations demonstrate that this designed inorganic‐rich hybrid SEI effectively regulates Li⁺ transport and promotes uniform Li deposition, thereby suppressing Li dendrite growth. Consequently, symmetric Li|| Li cells equipped with the modified anodes achieve stable cycling for 700 h at 1 mA cm −2 and 1 mAh cm −2 . Furthermore, when paired with an LFP cathode, the full cells exhibit significantly enhanced high‐rate capability and superior cycling stability, retaining 97.8% capacity after 800 cycles at 7.5C. This work provides a plasma interfacial engineering route for constructing advanced alkali metal anodes.