Sulfur Vacancies and 1T Phase-Rich MoS₂ Nanosheets as an Artificial Solid Electrolyte Interphase for 400 Wh kg^-1 Lithium Metal Batteries

Constructing large-area artificial solid electrolyte interphase (SEI) to suppress Li dendrites growth and electrolyte consumption is essential for high-energy-density Li metal batteries (LMBs). Herein, chemically exfoliated ultrathin MoS2 nanosheets (EMoS2) as an artificial SEI are scalable transfer-printed on Li-anode (EMoS2@Li). The EMoS2 with a large amount of sulfur vacancies and 1T phase-rich acts as a lithiophilic interfacial ion-transport skin to reduce the Li nucleation overpotential and regulate Li(+ )flux. With favorable Young's modulus and homogeneous continuous layered structure, the proposed EMoS2@Li effectively suppresses the growth of Li dendrites and repeat breaking/reforming of the SEI. As a result, the assembled EMoS2@Li||LiFePO4 and EMoS2@Li||LiNi0.8Co0.1Mn0.1O2 batteries demonstrate high-capacity retention of 93.5% and 92% after 1000 cycles and 300 cycles, respectively, at ultrahigh cathode loading of 20 mg cm(-2). Ultrasonic transmission technology confirms the admirable ability of EMoS2@Li to inhibit Li dendrites in practical pouch batteries. Remarkably, the Ah-class EMoS2@Li||LiNi0.8Co0.1Mn0.1O2 pouch battery exhibits an energy density of 403 Wh kg(-1 )over 100 cycles with the low negative/positive capacity ratio of 1.8 and electrolyte/capacity ratio of 2.1 g Ah(-1). The strategy of constructing an artificial SEI by sulfur vacancies-rich and 1T phase-rich ultrathin MoS2 nanosheets provides new guidance to realize high-energy-density LMBs with long cycling stability.