A Diels-Alder-based rGO anchoring binder for robust conductive networks in SiOx anodes

Abstract

Silicon oxide (SiOx, 0 < x < 2) is a promising anode material for high-energy lithium-ion batteries; however, its practical application is limited by the instability of conductive networks caused by aggregation of hydrophobic conductive additives during cycling. Here, we present a binder-centered strategy that stabilizes conductive pathways by uniformly integrating reduced graphene oxide (rGO) within a poly(acrylic acid) (PAA)-based binder. Furfurylamine-functionalized PAA (FPAA) was covalently cross-linked with 6-amino-4-hydroxy-2-naphthalenesulfonic acid–functionalized rGO (AHNSrGO) via Diels–Alder chemistry, forming a homogeneously dispersed rGO network anchored in the binder matrix. The resulting rGO-integrated binder effectively redistributes hydrophobic Super P through π–π interactions while maintaining strong adhesion to hydrophilic SiOx particles via hydrogen bonding, thereby suppressing conductive-additive aggregation during long-term cycling. Consequently, SiOx electrodes employing this FPAA–AHNSrGO (FG) binder exhibit enhanced adhesion strength, accelerated electrochemical utilization of SiOx, reduced interfacial resistance, and significantly improved rate capability and cycling stability compared to conventional PAA-based electrodes. Notably, these advantages are more pronounced under high mass-loading and low conductive-additive conditions and are retained in full-cell configurations paired with NCM811 cathodes. This work demonstrates that binder-level rGO integration is an effective and scalable approach to preserving conductive-network integrity, enabling high-energy and long-life silicon-based lithium-ion batteries. © 2026 Elsevier B.V. All rights are reserved, including those for text and data mining, AI training, and similar technologies.