# The following data include various measurements using electrochemical impedance spectroscopy (EIS), scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS) and time-of-flight secondary ion mass spectroscopy (ToF-SIMS). EIS and galvanostatic electrochemical measurements were conducted using a VMP300 potentiostat from Biologic. All SEM measurements were done using a high-Resolution field-emission instrument (GEMINI SEM 560) from Carl Zeiss Microscopy GmbH. For EDS measurements the same SEM was used, coupled with a X-Max Extreme Silicon drift detector from Oxford Instruments. For further informations, please see the "Methods" section of the manuscript. All data is structured according to the figures presented in the manuscript. ## The following overview summarizes the uploaded data and is intended to help the reader understand it more easily. Figure 1.zip: Electrochemical data of the electrodeposition of lithium at the steel|LPSCl interface using a constant current method. File type .txt. Figure 2.zip: XPS and ToF-SIMS data of the analyzed lithium species LiLP, LiHP and LiD in a cross-sectional geometry. In the case of the ToF-SIMS data both the depth-profile measurements as well as surface spectra are provided. File type .txt. Figure 3.zip: XPS and ToF-SIMS data of analyzed LPSCl pellet surfaces. Files ending with "_pristine" are referring to a pristine LPSCl pellet. Files ending with "_after_LiLP_contact" are analyzed after being contacted with a LiLP electrode used for lithium Stripping. File type .txt. Figure 4.zip: This file contains two subfolders, one each for experiments using LPSCl or LLZO as solid electrolyte. Both subfolders contain electrochemical data during stripping of the different lithium samples LiLP, LiHP and LiD. These experiments were performed by galvanostatic impedance spectroscopy. The impedance data are included. File type .txt. Figure 5.zip: Reference to the data structure. File type .txt. Figure 6.zip: Reference to the data structure. File type .txt. Supplementary Information Figure 1.zip: Optical images of a LPSCl pellet and a steel working electrode after electrodeposition of lithium at the LPSCl|steel interface. File type .tif. Supplementary Information Figure 2.zip: XPS spectra (Li 1s) acquired on a LiLP sample after different sputter times. File type .txt. Supplementary Information Figure 3.zip: XPS spectra (Na 1s) acquired on the different lithium samples LiLP, LiHP, LiD. File type .txt. Supplementary Information Figure 4.zip: EDS data of a LiLP electrode after being in contact with a LPSCl pellet for lithium stripping. In addition, an electron image of a prepared FIB crater is provided. File type .h5oina and .png. Supplementary Information Figure 5.zip: EDS data of a LiHP electrode after being in contact with a LPSCl pellet for lithium stripping. In addition, an electron image of a prepared FIB crater is provided. File type .h5oina and .png. Supplementary Information Figure 6.zip: Reference to the data structure. File type .txt. Supplementary Information Figure 7.zip: Optical images of a LLZO pellet Surface after LiLP electrode removal after a stripping experiment. In addition, XPS and ToF-SIMS data are provided of the different areas of the LLZO pellet surface (contact area and pristine area). File type .tif and .txt. Supplementary Information Figure 8.zip: EDS data of two LLZO surfaces after being in contact with either LiLP or LiHP for lithium stripping. File type .h5oina. Supplementary Information Figure 9.zip: Electrochemical data of the electrodeposition of lithium at the steel|LPSCl interface using a constant current method. File type .txt. Supplementary Information Figure 10.zip: This file contains three subfolders, one each for experiment using LiLP, LiHP or LiD as electrodes in contact with LPSCl during stripping. In each folder, the impedance data at different stages of the lithium stripping is provided. File type .txt. Supplementary Information Figure 11.zip: This file contains two subfolders, one each for experiment using LiLP or LiHP as electrodes in contact with LLZO during stripping. In each folder, the impedance data at different stages of the lithium stripping is provided. File type .txt. Supplementary Information Figure 12.zip: Electron images of the pore morphology of either LiLP or LiHP after lithium stripping on a LLZO pellet. File type .tif. Supplementary Information Figure 13.zip: EDS data of a LiLP surface after being in contact with LLZO as solid electrolyte for lithium stripping. File type .h5oina. Supplementary Information Figure 14.zip: Electron images of a crater prepared after the electrodeposition of lithium at the steel|LPSCl interface. File type .png. ### Information about the data file type for EDS data The acquired EDS data are stored in a Oxford Instruments NanoAnalysis HDF5 file format (.h5onia) and can be accessed through Oxford Instruments' AZtec software or compatible third-party software. For further insights into the file structure, we refer the reader to the following link: https://github.com/oinanoanalysis/h5oina