Carbon Nanotube‐Reinforced Dual Carbon Stress‐Buffering for Highly Stable Silicon Anode Material in Lithium‐Ion Battery

Abstract Silicon (Si) anode suffers from huge volume expansion which causes poor structural stability in terms of electrode material, solid electrolyte interface, and electrode, limiting its practical application in high‐energy‐density lithium‐ion batteries. Rationally designing architectures to optimize the stress distribution of Si/carbon (Si/C) composites has been proven to be effective in enhancing their structural stability and cycling stability, but this remains a big challenge. Here, metal‐organic frameworks (ZIF‐67)‐derived carbon nanotube‐reinforced carbon framework is employed as an outer protective layer to encapsulate the inner carbon‐coated Si nanoparticles (Si@C@CNTs), which features dual carbon stress‐buffering to enhance the structural stability of Si/C composite and prolong their cycling lifetime. Finite element simulation proves the structural advantage of dual carbon stress‐buffering through significantly relieving stress concentration when Si lithiation. The outer carbon framework also accelerates the charge transfer efficiency during charging/discharging by the improvement of lithium‐ion diffusion and electron transport. As a result, the Si@C@CNTs electrode exhibits excellent long‐term lifetime and good rate capability, showing a specific capacity of 680 mAh g −1 even at a high rate of 1 A g −1 after 1000 cycles. This work provides insight into the design of robust architectures for Si/C composites by stress optimization.