Advanced Tri-Layer Carbon Matrices with π–π Stacking Interaction for Binder-Free Lithium-Ion Storage

Enabling materials with distinct features toward achieving high-performance energy storage devices is of huge importance but highly challenging. Commercial carbon cloth (CC), because of its appealing chemical and mechanical properties, has been proven to be an excellent conductive substrate for active electrode materials. However, its performance is notably poor when directly used as an electrode in energy storage, due to its low theoretical capacity and surface area. Herein, we successfully endow the CC with enhanced storage capacity via formation of a π–π stacking interaction by integrating electrochemically activated CC (denoted CC/ACC) with biomass-derived carbon (BMDC) (denoted π-CC/ECC@BMDC). The π-CC/ECC@BMDC electrode displays excellent storage performance with a high capacity of 2.53 mAh cm–2 under 0.2 mA cm–2 when used as anode material for lithium ion batteries (LIBs). Due to the induction energy, the negatively charged molecules of the CC/ACC functional groups interact with the BMDC during carbonization, creating the π–π stacking interaction. Based on first-principles calculations, the structural design of the tri-layer carbon enables the movement of electrons around the π–π stacking interaction, which significantly facilitates rapid transportation of electrons, creates three-dimensional (3D) ion tunnels for fast transportation of ions, and improves the electrode’s mechanical and electronic properties.