Two-Dimensional Silicon/Carbon from Commercial Alloy and CO2 for Lithium Storage and Flexible Ti3C2Tx MXene-Based Lithium–Metal Batteries

Silicon has been considered as the most promising anode candidate for next-generation lithium-ion batteries. However, the fast capacity decay caused by huge volume expansion and low electronic conductivity limit the electrochemical performance. Herein, atomic distributed, air-stable, layer-by-layer-assembled Si/C (L-Si/C) is designed and in situ constructed from commercial micron-sized layered CaSi2 alloy with the greenhouse gas CO2. The inner structure of Si as well as the content and graphitization of C can be regulated by simply adjusting the reaction conditions. The rationally designed layered structure can enhance electronic conductivity and mitigate volume change without disrupting the carbon layer or destroying the solid electrolyte interface. Moreover, the single-layer Si and C can enhance lithium-ion transport in active materials. With these advantages, L-Si/C anode delivers an 82.85% capacity retention even after 3200 cycles and superior rate performance. The battery-capacitance dual-model mechanism is certified via quantitative kinetics measurement. Besides, the self-standing architecture is designed via assembling L-Si/C and MXene. Lithiophilic L-Si/C can guide homogeneous Li deposition with alleviated volume change. With the MXene/L-Si/C host for lithium-metal batteries, an ultralong life span up to 500 h in a carbonate-based electrolyte is achieved. A full cell with a high-energy 5 V LiNi0.5Mn1.5O4 cathode is constructed to verify the practicality of L-Si/C and MXene/L-Si/C. The rational design of a special layer structure may propose a strategy for other materials and energy storage systems.