Mesoporous Silica Reinforced Hybrid Polymer Artificial Layer for High-Energy and Long-Cycling Lithium Metal Batteries

Rechargeable lithium metal batteries are regarded as the “Holy Grail” of energy storage systems but suffer from poor cycling stability and severe safety concerns caused by notorious Li dendrite growth. Herein, we have achieved a record-breaking cycling life of high-voltage Li metal full cells simply by constructing a mesoporous silica reinforced hybrid polymer artificial layer on the Li surface. The inorganic mesoporous SiO2 filler plays a critical role in regulating Li+ ion migration and strengthening the mechanical rigidity, while the polymeric PVDF matrix endows the artificial SEI with structural integrity and stretchable flexibility, thereby significantly stabilizing the fluid Li anode–electrolyte interface. A remarkably extended cycling life could be achieved for modified Li anodes when coupled with various high-voltage cathodes (4.5 V class LiNi0.5Co0.2Mn0.3O2 and LiNi0.8Co0.1Mn0.1O2 and 5 V class LiNi0.5Mn1.5O4) under practical and even harsh operating conditions. Our work clears the obstacles on the way to a practical Li metal anode and provides guidance for the development of high-energy batteries.