A Spiderweb-Inspired Dual-Crosslinked Polymer Binder for Stable Silicon Anodes
- 1School of Chemistry, Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, GD HPPC Lab, Sun Yat-sen University, Guangzhou 510275, China
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.
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BibTeX
@article{zheng2026spiderwebinspired,
title = {{A Spiderweb-Inspired Dual-Crosslinked Polymer Binder for Stable Silicon Anodes}},
author = {Chao Zheng and Kaixiang Chen and Wenhong Ruan},
journal = {Batteries},
year = {2026},
month = oct,
doi = {10.3390/batteries12100426},
url = {https://www.mdpi.com/2313-0105/12/10/426},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - A Spiderweb-Inspired Dual-Crosslinked Polymer Binder for Stable Silicon Anodes
AU - Chao Zheng
AU - Kaixiang Chen
AU - Wenhong Ruan
PY - 2026
DA - 2026/10/15
JO - Batteries
DO - 10.3390/batteries12100426
UR - https://www.mdpi.com/2313-0105/12/10/426
AB - 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.
SN - 2313-0105
ER -