Unravelling Li-Ion Transport from Picoseconds to Seconds

Bulk versus Interfaces in an Argyrodite Li<sub>6</sub>PS<sub>5</sub>Cl-Li<sub>2</sub>S All-Solid-State Li-Ion Battery

Journal article (2016)

Authors

C. Yu RST/Fundamental Aspects of Materials and Energy - AS
S. Ganapathy RST/Fundamental Aspects of Materials and Energy - AS
N.J.J. de Klerk RST/Fundamental Aspects of Materials and Energy - AS
I.E. Roslon Student
Ernst R.H. van Eck Radboud Universiteit Nijmegen
Arno P.M. Kentgens Radboud Universiteit Nijmegen
M. Wagemaker RST/Fundamental Aspects of Materials and Energy - AS
Research Group
RST/Fundamental Aspects of Materials and Energy (AS) (TU Delft)
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Published Date

2016

Language

English

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Faculty

Applied Sciences

Department

RST/Radiation, Science and Technology

Research Group

RST/Fundamental Aspects of Materials and Energy

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 7Li 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.