Spatiotemporally coupled sulfur chemistry for stable silicon-90+ anodes

Silicon-based materials stand as tantalizing battery anodes for markedly advancing performance indicators of today’s rechargeable lithium-ion batteries; however, their structural degradations, together with detestable side reactions residing in electrode-electrolyte interphases, greatly hinder the delivery of energy promises under practical conditions. Herein, we introduce the spatiotemporally coupled sulfur chemistry as an effective antidote to cope with the volume change and structural integrity of near-full silicon anodes, and concurrently modulate inherent properties of electrode-electrolyte interphases layers enlisting elasticity and ion diffusivity. The sulfur regulated approach is readily achieved by overlaying silicon with a homogenous layer of elemental sulfur, which is highly compatible with present production facilities for lithium-ion batteries industry. The prototype LiNi0.9Co0.05Mn0.05O2 | |Si90+ pouch cell at ampere-hour level (7.3 Ah) delivers great performances assessed simultaneously by energy density (1190 Wh L−1 for cell), specific energy (416 Wh kg−1 for cell), and cycle life (80% capacity retention after 1700 cycles). In light of the significantly improved battery performance and practical applicability, the sulfur regulated Si90+ anodes thus could be considered as a game-changer for offering reliable power source and rapidly turning emerging applications into reality. Silicon-based materials stand as tantalizing battery negative electrodes for rechargeable lithium-ion batteries. Herein, authors introduce the spatiotemporally coupled sulfur chemistry as an effective antidote to cope with the volume change and structural integrity of silicon-90 negative electrodes.