TY - JOUR
T1 - Facile Synthesis toward the Optimal Structure-Conductivity Characteristics of the Argyrodite Li6PS5Cl Solid-State Electrolyte
AU - Yu, Chuang
AU - Ganapathy, Swapna
AU - Hageman, Jart
AU - Van Eijck, Lambert
AU - Van Eck, Ernst R.H.
AU - Zhang, Long
AU - Schwietert, Tammo
AU - Basak, Shibabrata
AU - Kelder, Erik M.
AU - Wagemaker, Marnix
PY - 2018
Y1 - 2018
N2 - 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.
AB - 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.
KW - argyrodite
KW - conductivity
KW - solid-state batteries
KW - structure
KW - sulfide solid electrolyte
UR - http://www.scopus.com/inward/record.url?scp=85053837223&partnerID=8YFLogxK
UR - http://resolver.tudelft.nl/uuid:4aeb9971-b567-4ba8-a9da-3776e0f69433
U2 - 10.1021/acsami.8b07476
DO - 10.1021/acsami.8b07476
M3 - Article
AN - SCOPUS:85053837223
SN - 1944-8244
VL - 10
SP - 33296
EP - 33306
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
ER -