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Precise Tailoring of Lithium-Ion Transport for Ultralong-Cycling Dendrite-Free All-Solid-State Lithium Metal Batteries

Journal Article · · Advanced Materials
 [1];  [2];  [1];  [3];  [4];  [5];  [1];  [6];  [7];  [8];  [8];  [8];  [1];  [2];  [1];  [9]
  1. Western University, London, ON (Canada)
  2. Newcastle University, Newcastle upon Tyne (United Kingdom)
  3. Eastern Institute of Technology, Ningbo (EIT) (China)
  4. Harwell Science and Innovation Campus, Didcot (United Kingdom). The Faraday Institution
  5. Chinese Academy of Sciences (CAS), Beijing (China). Institute of High Energy Physics (IHEP)
  6. Argonne National Laboratory (ANL), Argonne, IL (United States)
  7. University of Hong Kong, Kowloon (Hong Kong)
  8. University of Saskatchewan, Saskatoon, SK (Canada). Canadian Light Source, Inc.
  9. Western University, London, ON (Canada); Eastern Institute of Technology, Ningbo (EIT) (China)
+ Show Author Affiliations
All-solid-state lithium metal batteries can address crucial challenges regarding insufficient battery cycling life and energy density. The demonstration of long-cycling dendrite-free all-solid-state lithium metal batteries requires precise tailoring of lithium-ion transport of solid-state electrolytes (SSEs). Here, in this work, a proof of concept is reported for precise tailoring of lithium-ion transport of a halide SSE, Li3InCl6, including intragranular (within grains) but also intergranular (between grains) lithium-ion transport. Lithium-ion migration tailoring mechanism in crystals is developed by unexpected enhanced Li, In, and Cl vacancy populations and lower energy barrier for hopping. The lithium-ion transport tailoring mechanism between the grains is determined by the elimination of voids between grains and the formation of unexpected supersonic conducting grain boundaries, boosting the lithium dendrite suppression ability of SSE. Due to boosted lithium-ion conduction and dendrite-suppression ability, the all-solid-state lithium metal batteries coupled with Ni-rich LiNi0.83Co0.12Mn0.05O2 cathodes and lithium metal anodes demonstrate breakthroughs in electrochemical performance by achieving extremely long cycling life at a high current density of 0.5 C (2000 cycles, 93.7% capacity retention). This concept of precise tailoring of lithium-ion transport provides a cost, time, and energy efficient solution to conquer the remaining challenges in all-solid-state lithium-metal batteries for fast developing electric vehicle markets.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
Engineering and Physical Sciences Research Council (EPSRC); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2564828
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 13 Vol. 36; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (18)

Solid Halide Electrolytes with High Lithium-Ion Conductivity for Application in 4 V Class Bulk-Type All-Solid-State Batteries journal September 2018
Water‐Mediated Synthesis of a Superionic Halide Solid Electrolyte journal September 2019
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Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction journal December 2015
Molecular Dynamics Simulation of Li-Ion Conduction at Grain Boundaries in NASICON-Type LiZr2(PO4)3 Solid Electrolytes journal October 2021
Challenges for and Pathways toward Li-Metal-Based All-Solid-State Batteries journal March 2021
Atomic-Scale Influence of Grain Boundaries on Li-Ion Conduction in Solid Electrolytes for All-Solid-State Batteries journal December 2017
Origin of fast ion diffusion in super-ionic conductors journal June 2017
Design principles for solid-state lithium superionic conductors journal August 2015
High electronic conductivity as the origin of lithium dendrite formation within solid electrolytes journal January 2019
Pathways for practical high-energy long-cycling lithium metal batteries journal February 2019
Fundamentals of inorganic solid-state electrolytes for batteries journal August 2019
Visualizing plating-induced cracking in lithium-anode solid-electrolyte cells journal April 2021
Lithium superionic conductors with corner-sharing frameworks journal March 2022
Designing solid-state electrolytes for safe, energy-dense batteries journal February 2020
Air-stable Li 3 InCl 6 electrolyte with high voltage compatibility for all-solid-state batteries journal January 2019
High-throughput computational screening for solid-state Li-ion conductors journal January 2020
Atomic-scale origin of the large grain-boundary resistance in perovskite Li-ion-conducting solid electrolytes journal January 2014

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Related Subjects

25 ENERGY STORAGE
all-solid-state lithium metal batteries
dendrite suppression
intergranular
intragranular
lithium-ion transport