Covalently Bonded Silicon/Carbon Nanocomposites as Cycle-Stable Anodes for Li-Ion Batteries

Carbon coating is a popular strategy to boost the cyclability of Si anodes for Li-ion batteries. However, most of the Si/C nanocomposite anodes fail to achieve stable cycling due to the easy separation and peeling off of the carbon layer from the Si surface during extended cycles. To overcome this problem, we develop a covalent modification strategy by chemically bonding a large conjugated polymer, poly-peri-naphthalene (PPN), on the surfaces of nano-Si particles through a mechanochemical method, followed by a carbonization reaction to convert the PPN polymer into carbon, thus forming a Si/C composite with a carbon coating layer tightly bonded on the Si surface. Due to the strong covalent bonding interaction of the Si surface with the PPN-derived carbon coating layer, the Si/C composite can keep its structural integrity and provide an effective surface protection during the fluctuating volume changes of the nano-Si cores. As a consequence, the thus-prepared Si/C composite anode demonstrates a reversible capacity of 1512.6 mA h g^–1, a stable cyclability over 500 cycles with a capacity retention of 74.2%, and a high cycling Coulombic efficiency of 99.5%, providing a novel insight for designing highly cyclable silicon anodes for new-generation Li-ion batteries.