An LiFSI DME electrolyte (6 M) was prepared by adding LiFSI into anhydrous DME solvents. Before preparing the electrolyte, DME was dried with a molecular sieve (4 Å, Sigma-Aldrich) to reduce the water content to less than 5 ppm, which is measured with a Karl-Fisher titrator (Metrohm 899 Coulometer). All the cells were assembled in an Al-filled glove box with O2 and moisture content of <2 ppm. To assemble the Li|LPS|Li solid-state cell, 110 mg of LPS SSE was pressed into a pellet under 300 MPa in a polytetrafluoroethylene hollow cylinder with a diameter of 10 mm. Then, one drop of 6 M LiFSI DME was added on both sides of the LPS pellet, and two Li foils with the same diameter were attached on both sides. After that, the Li|LPS|Li was dried at 120°C under vacuum overnight. The dried Li|LPS|Li cell was then sandwiched between two SS rods, which functioned as current collectors. For reference, the Li|LPS|Li cell without LiFSI was also assembled with the same procedures. A huge volume change of the electrodes will trigger the contact issues, changing the local current densities during cycling. To avoid the contact issues in the Li|LPS|SS cell, a relatively small plating capacity of 0.1 mAh cm−2 was applied for all the SSE Li metal cells. To obtain the interfacial information on the LPS SSE, LPS was recovered from the Li|LPS|SS after cycling. The surface of the LPS facing the SS was analyzed. For the Li||LCO solid-state cells, the cathode of LiCoO2 was precoated with LiNbO2 through the sol-gel method followed by heat treatment (38). The loading of the cathode is about 1 mAh cm−2. The weight ratio of the LiNbO2-coated LiCoO2 and LPS was 70:30. The ionic conductivity of the LPS was measured by the EIS test of the Pt|LPS|Pt cell, which was tested on a Gamry workstation (Gamry 1000E, Gamry Instruments, USA). The galvanostatic cycling test was determined by an Arbin BT2000 workstation (Arbin Instruments, USA). All the electrochemical tests were performed at room temperature (25°C).

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