Binder-enabled cross-scale stabilization of high-areal-capacity micro-sized silicon anodes for high-voltage lithium-ion batteries

Abstract

Sustainable micro-sized silicon (μSi) has emerged as a promising high-capacity alternative to traditional carbon-based anodes in lithium-ion batteries. However, addressing severe cracking in both electrodes and particles attributed to large volumetric change during cycling remains a challenge. Here we developed a cost-effective water-based cross-scale stabilization (CSS) binder to preserve the electrode integrity and stabilize the solid electrolyte interphase of μSi anodes. Forming a soft-rigid, electrically conductive, high-elasticity network and directing the growth of highly robust LiF-rich interphases, the CSS binder enables stable cycling of μSi anodes at impressive areal capacities of up to 5.9 mAh cm^–2 and a high volumetric capacity of 2458 mAh cm^–3, which represents a pioneering report on high-capacity μSi anodes. Furthermore, at commercial-level areal capacities, 4.2-V μSi||LiNi_0.8Mn_0.1Co_0.1O₂ pouch cells (N/P = 1.15) achieve 81% capacity retention in 100 cycles. This work introduces innovative strategies for enhancing reversible lithium storage in high-capacity alloy-type anodes and advancing the development of high-energy-density batteries.