| Autor: |
Yu C; Department of Radiation Science and Technology, Delft University of Technology , Mekelweg 15, Delft 2629 JB, The Netherlands., Ganapathy S; Department of Radiation Science and Technology, Delft University of Technology , Mekelweg 15, Delft 2629 JB, The Netherlands., de Klerk NJ; Department of Radiation Science and Technology, Delft University of Technology , Mekelweg 15, Delft 2629 JB, The Netherlands., Roslon I; Department of Radiation Science and Technology, Delft University of Technology , Mekelweg 15, Delft 2629 JB, The Netherlands., van Eck ER; Institute for Molecules and Materials, Radboud University Nijmegen , Heyendaalseweg 135, Nijmegen 6525 AJ, The Netherlands., Kentgens AP; Institute for Molecules and Materials, Radboud University Nijmegen , Heyendaalseweg 135, Nijmegen 6525 AJ, The Netherlands., Wagemaker M; Department of Radiation Science and Technology, Delft University of Technology , Mekelweg 15, Delft 2629 JB, The Netherlands. |
| Abstrakt: |
One of the main challenges of all-solid-state Li-ion batteries is the restricted power density due to the poor Li-ion transport between the electrodes via the electrolyte. However, to establish what diffusional process is the bottleneck for Li-ion transport requires the ability to distinguish the various processes. The present work investigates the Li-ion diffusion in argyrodite Li6PS5Cl, a promising electrolyte based on its high Li-ion conductivity, using a combination of (7)Li NMR experiments and DFT based molecular dynamics simulations. This allows us to distinguish the local Li-ion mobility from the long-range Li-ion motional process, quantifying both and giving a coherent and consistent picture of the bulk diffusion in Li6PS5Cl. NMR exchange experiments are used to unambiguously characterize Li-ion transport over the solid electrolyte-electrode interface for the electrolyte-electrode combination Li6PS5Cl-Li2S, giving unprecedented and direct quantitative insight into the impact of the interface on Li-ion charge transport in all-solid-state batteries. The limited Li-ion transport over the Li6PS5Cl-Li2S interface, orders of magnitude smaller compared with that in the bulk Li6PS5Cl, appears to be the bottleneck for the performance of the Li6PS5Cl-Li2S battery, quantifying one of the major challenges toward improved performance of all-solid-state batteries. |
