Stable high-capacity and high-rate silicon-based lithium battery anodes upon two-dimensional covalent encapsulation

Silicon is a promising anode material for lithium-ion and post lithium-ion batteries but suffers from a large volume change upon lithiation and delithiation. The resulting instabilities of bulk and interfacial structures severely hamper performance and obstruct practical use. Stability improvements have been achieved, although at the expense of rate capability. Herein, a protocol is developed which we describe as two-dimensional covalent encapsulation. Two-dimensional, covalently bound silicon-carbon hybrids serve as proof-of-concept of a new material design. Their high reversibility, capacity and rate capability furnish a remarkable level of integrated performances when referred to weight, volume and area. Different from existing strategies, the two-dimensional covalent binding creates a robust and efficient contact between the silicon and electrically conductive media, enabling stable and fast electron, as well as ion, transport from and to silicon. As evidenced by interfacial morphology and chemical composition, this design profoundly changes the interface between silicon and the electrolyte, securing the as-created contact to persist upon cycling. Combined with a simple, facile and scalable manufacturing process, this study opens a new avenue to stabilize silicon without sacrificing other device parameters. The results hold great promise for both further rational improvement and mass production of advanced energy storage materials. Stabilizing silicon without sacrificing other device parameters is essential for practical use in lithium and post lithium battery anodes. Here, the authors show the skin-like two-dimensional covalent encapsulation furnishing a remarkable level of integrated lithium storage performances of silicon.