A three-dimensional mesh β-CD-CMC adhesive was designed based on the structure of fishing nets. This cross-linked binder has the ability to disperse the stress at the anchor point and moderate the significant volume changes of the Si anode.

The strategy of material modification for improving the stability of silicon electrodes is laborious and costly, while the conventional binders cannot withstand the repeated massive volume variability of silicon-based materials. Hence, there is a demand to settle the silicon-based materials' problems with green and straightforward solutions. This paper presents a high-performance silicon anode with a binder obtained by in situ thermal cross-linking of citric acid (CA) and βcyclodextrin (β-CD) during the electrode preparation process. The Si electrode with a binder synthesized by the one-pot method shows excellent cycling performance. It maintains a specific capacity of 1696 mAh•g −1 after 200 cycles at a high current of 0.5 C. Furthermore, the carbonylation of β-CD to carbonyl-β-CD (c-β-CD) introduced better water solubility, and the c-β-CD can generate multidimensional connections with CA and Si, which significantly enhances the specific capacity to 1941 mAh•g −1 at 0.5 C. The results demonstrate that the prepared integrated electrode facilitates the formation of a stable and controllable solid electrolyte interface layer of Si and accommodates Si's repeated giant volume variations.