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

Abstract 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||LiNi_0.8Co_0.1Mn_0.1O₂ 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||LiNi_0.8Co_0.1Mn_0.1O₂ 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.