Print Email Facebook Twitter Facile Synthesis toward the Optimal Structure-Conductivity Characteristics of the Argyrodite Li6PS5Cl Solid-State Electrolyte Title Facile Synthesis toward the Optimal Structure-Conductivity Characteristics of the Argyrodite Li6PS5Cl Solid-State Electrolyte Author Yu, C. (TU Delft RST/Fundamental Aspects of Materials and Energy) Ganapathy, S. (TU Delft RST/Storage of Electrochemical Energy) Hageman, J.G. (TU Delft Applied Sciences) van Eijck, L. (TU Delft RST/Neutron and Positron Methods in Materials) Van Eck, Ernst R.H. (Radboud Universiteit Nijmegen) Zhang, Long (Yanshan University) Schwietert, T.K. (TU Delft Applied Sciences) Basak, S. (TU Delft RST/Storage of Electrochemical Energy) Kelder, E.M. (TU Delft RST/Storage of Electrochemical Energy) Wagemaker, M. (TU Delft RST/Storage of Electrochemical Energy) Faculty Applied Sciences Date 2018 Abstract The high Li-ion conductivity of the argyrodite Li6PS5Cl makes it a promising solid electrolyte candidate for all-solid-state Li-ion batteries. For future application, it is essential to identify facile synthesis procedures and to relate the synthesis conditions to the solid electrolyte material performance. Here, a simple optimized synthesis route is investigated that avoids intensive ball milling by direct annealing of the mixed precursors at 550 °C for 10 h, resulting in argyrodite Li6PS5Cl with a high Li-ion conductivity of up to 4.96 × 10-3 S cm-1 at 26.2 °C. Both the temperature-dependent alternating current impedance conductivities and solid-state NMR spin-lattice relaxation rates demonstrate that the Li6PS5Cl prepared under these conditions results in a higher conductivity and Li-ion mobility compared to materials prepared by the traditional mechanical milling route. The origin of the improved conductivity appears to be a combination of the optimal local Cl structure and its homogeneous distribution in the material. All-solid-state cells consisting of an 80Li2S-20LiI cathode, the optimized Li6PS5Cl electrolyte, and an In anode showed a relatively good electrochemical performance with an initial discharge capacity of 662.6 mAh g-1 when a current density of 0.13 mA cm-2 was used, corresponding to a C-rate of approximately C/20. On direct comparison with a solid-state battery using a solid electrolyte prepared by the mechanical milling route, the battery made with the new material exhibits a higher initial discharge capacity and Coulombic efficiency at a higher current density with better cycling stability. Nevertheless, the cycling stability is limited by the electrolyte stability, which is a major concern for these types of solid-state batteries. Subject argyroditeconductivitysolid-state batteriesstructuresulfide solid electrolyte To reference this document use: http://resolver.tudelft.nl/uuid:4aeb9971-b567-4ba8-a9da-3776e0f69433 DOI https://doi.org/10.1021/acsami.8b07476 ISSN 1944-8244 Source ACS applied materials & interfaces, 10, 33296-33306 Part of collection Institutional Repository Document type journal article Rights © 2018 C. Yu, S. Ganapathy, J.G. Hageman, L. van Eijck, Ernst R.H. Van Eck, Long Zhang, T.K. Schwietert, S. Basak, E.M. Kelder, M. Wagemaker Files PDF acsami.8b07476_1.pdf 7.03 MB Close viewer /islandora/object/uuid:4aeb9971-b567-4ba8-a9da-3776e0f69433/datastream/OBJ/view