Stabilizing silicon-sulfur cells via binder-free xerogel-silicon anode and interfacial network engineering

Silicon (Si) is an attractive anode for next-generation batteries owing to its high theoretical capacity, yet extreme volume expansion and unstable interfaces hinder practical implementation. Here we report a binder-free silicon architecture in which nanoparticles are encapsulated within a three-dimensional conductive poly (N-phenyl glycine) (PNPG) xerogel network that simultaneously provides mechanical resilience and electronic pathways. First-principles calculations reveal strong dissociative chemisorption of PNPG on Si (111) and Li 15 Si 4 surfaces, with adsorption energies up to −4.14 eV, far exceeding those of conventional PVDF binders and enabling robust interfacial anchoring. When integrated with a non-flammable gel polymer electrolyte, the Si–PNPG anode delivers 1464.2 mAh g −1 after 246 cycles at 600 mA g −1 . A prelithiated Si-PNPG | | S-PAN full cell achieves an energy density of 618 Wh kg −1 at room temperature and stable operation across a broad temperature range. This combined experimental-theoretical study establishes xerogel- mediated interfacial engineering as a scalable route toward safe, high-energy silicon-sulfur batteries.