Due to the advantages of high safety and high energy density, solid-state lithium batteries (SSLBs) are promising competitors for next-generation batteries. Unfortunately, the growth of Li dendrites and irreversible capacity loss caused by the Li metal anode/solid electrolyte interfacial incompatibility remain challenges. Herein, an in situ formed artificial protective layer between the lithium metal anode and solid electrolyte Li 6 PS 5 Cl (LPSC) is introduced. A stable solid electrolyte interface (SEI) is in situ formed in the Li/Li 6 PS 5 Cl interface via the electrochemical reduction of the liquid electrolyte LiTFSI/tetraethylene glycol dimethyl ether (Li(G4)TFSI), which is beneficial for the improvement of the stability of interfacial chemistry and homogeneous lithium deposition behavior. The assembled Li/Li(G4)TFSI-assisted Li 6 PS 5 Cl/Li symmetric cells enable stable cycles for 850 and 400 h at a current density of 0.1 and 0.2 mA/cm 2 , respectively. Moreover, the LiNi 0.6 Co 0.1 Mn 0.3 O 2 (NCM613)/Li(G4)TFSI-assisted Li 6 PS 5 Cl/Li SSLBs can achieve prominent cycling stability at room temperature. This work provides a new insight into the interfacial modification to design SSLBs with high energy density.
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