An All‐Integrated Anode via Interlinked Chemical Bonding between Double‐Shelled–Yolk‐Structured Silicon and Binder for Lithium‐Ion Batteries

Abstract The concept of an all‐integrated design with multifunctionalization is widely employed in optoelectronic devices, sensors, resonator systems, and microfluidic devices, resulting in benefits for many ongoing research projects. Here, maintaining structural/electrode stability against large volume change by means of an all‐integrated design is realized for silicon anodes. An all‐integrated silicon anode is achieved via multicomponent interlinking among carbon@void@silica@silicon (CVSS) nanospheres and cross‐linked carboxymethyl cellulose and citric acid polymer binder (c‐CMC‐CA). Due to the additional protection from the silica layer, CVSS is superior to the carbon@void@silicon (CVS) electrode in terms of long‐term cyclability. The as‐prepared all‐integrated CVSS electrode exhibits high mechanical strength, which can be ascribed to the high adhesivity and ductility of c‐CMC‐CA binder and the strong binding energy between CVSS and c‐CMC‐CA, as calculated based on density functional theory (DFT). This electrode exhibits a high reversible capacity of 1640 mA h g −1 after 100 cycles at a current density of 1 A g −1 , high rate performance, and long‐term cycling stability with 84.6% capacity retention after 1000 cycles at 5 A g −1 .