title: Unravelling Li-Ion Transport from Picoseconds to Seconds: Bulk versus Interfaces in an Argyrodite Li6PS5Cl-Li2S All-Solid-State Li-Ion Battery.
abstract: 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.
authors: Department of Radiation Science and Technology, Delft University of Technology , Mekelweg 15, Delft 2629 JB, The Netherlands.
authors: Chuang
authors: C
authors: Yu
authors: Department of Radiation Science and Technology, Delft University of Technology , Mekelweg 15, Delft 2629 JB, The Netherlands.
authors: Swapna
authors: S
authors: Ganapathy
authors: Department of Radiation Science and Technology, Delft University of Technology , Mekelweg 15, Delft 2629 JB, The Netherlands.
authors: Niek J J
authors: NJ
authors: de Klerk
authors: Department of Radiation Science and Technology, Delft University of Technology , Mekelweg 15, Delft 2629 JB, The Netherlands.
authors: Irek
authors: I
authors: Roslon
authors: Institute for Molecules and Materials, Radboud University Nijmegen , Heyendaalseweg 135, Nijmegen 6525 AJ, The Netherlands.
authors: Ernst R H
authors: ER
authors: van Eck
authors: Institute for Molecules and Materials, Radboud University Nijmegen , Heyendaalseweg 135, Nijmegen 6525 AJ, The Netherlands.
authors: Arno P M
authors: AP
authors: Kentgens
authors: Department of Radiation Science and Technology, Delft University of Technology , Mekelweg 15, Delft 2629 JB, The Netherlands.
authors: Marnix
authors: M
authors: Wagemaker