A Spiderweb-Inspired Dual-Crosslinked Polymer Binder for Stable Silicon Anodes
Year: 2026
Type: article
Abstract: Silicon (Si) anodes suffer from severe structural degradation caused by large volume variation during lithiation/delithiation, requiring binders that can simultaneously provide mechanical support and deformation adaptability. Inspired by the functional specialization of spider webs, a dual-crosslinked polymer binder (DA1-B-PA) is developed by integrating differentiated load-bearing and energy-dissipating junctions into a hierarchical network. In this design, acrylic acid segments provide strong interfacial adhesion, flexible poly(ethylene glycol) methacrylate (APEG) chains accommodate deformation and facilitate Li-ion transport, Diels–Alder linkages construct stable load-bearing frameworks, and reversible boronate ester bonds enable local structural adjustment and energy dissipation. This molecularly engineered architecture effectively balances mechanical robustness and structural flexibility. Compared with conventional poly(acrylic acid) (PAA) and non-crosslinked DA1 binders, DA1-B-PA exhibits enhanced mechanical strength, hysteretic energy dissipation, and improved electrode integrity. Consequently, Si electrodes with DA1-B-PA deliver reversible capacities of approximately 1900, 1750, and 1300 mAh g−1 after 260, 550, and 850 cycles at 0.2, 0.5, and 1 C, respectively. Moreover, the Si||LiNi0.8Co0.1Mn0.1O2 (NCM811) full cell retains 73.15% of its capacity after 311 cycles. This work demonstrates that biomimetic functional differentiation provides a rational strategy for designing durable binders for high-volume-change electrode materials.
Source: Batteries
Authors: Chao Zheng, Kaixiang Chen, Wenhong Ruan
Institution: Sun Yat-sen University
Language: English
Subfield: Electrical and Electronic Engineering
Field: Engineering
Domain: Physical Sciences
Open Access status: gold
Estimated APC paid: $3,258
Awards: G4442975084, G7474729890
OpenAlex ID: W7221996107