Molecularly Tailored Lithium-Arene Complex Enables Chemical Prelithiation of High ­Capacity Lithium­Ion Battery Anodes

Abstract

Prelithiation is of great interest to Li&#8208

ion battery manufacturers as a strategy for compensating for the loss of active Li during initial cycling of a battery, which would otherwise degrade its available energy density. Solution&#8208

based chemical prelithiation using a reductive chemical promises unparalleled reaction homogeneity and simplicity. However, the chemicals applied so far cannot dope active Li in Si&#8208

based high&#8208

capacity anodes but merely form solid&#8211

electrolyte interphases, leading to only partial mitigation of the cycle irreversibility. Herein, we show that a molecularly engineered Li&#8211

arene complex with a sufficiently low redox potential drives active Li accommodation in Si&#8208

based anodes to provide an ideal Li content in a full cell. Fine control over the prelithiation degree and spatial uniformity of active Li throughout the electrodes are achieved by managing time and temperature during immersion, promising both fidelity and low cost of the process for large&#8208

scale integration.