Achieve Stable Lithium Metal Anode by Sulfurized-Polyacrylonitrile Modified Separator for High-Performance Lithium Batteries

Abstract

To develop a high-energy-density lithium battery, there still are several severe challenges for Li metal anode: low Coulombic efficiency caused by its high chemical reactivity, Li dendrite formation, and "dead" Li accumulation during repeated plating/stripping processes. Especially, lithium dendrite growth imposes inferior cycling stability and serious safety issues. Herein, we propose a facile but effective strategy to suppress lithium dendrite growth through an artificial inorganic-polymer protective layer derived from sulfurized polyacrylonitrile on a polyethylene separator. Benefiting from the lithiated sulfurized polyacrylonitrile and poly(acrylic acid), the flexible and ion-conductive protective layer could regulate Li⁺ flux and facilitate dendrite-free lithium deposition. Consequently, lithium metal with the meritorious protective layer can achieve a long-term cycling with negligible overpotential rise in Li-Li symmetric cells, even at a high areal capacity of 5 mAh cm^-2. Remarkably, such a protective layer enables stable cycling performance of Li-S cell with a high areal capacity (∼9 mAh cm^-2). This work provides a valuable exploration strategy for potential industrial applications of high-performance lithium metal batteries.