Lithium‐Metal Anode Instability of the Superionic Halide Solid Electrolytes and the Implications for Solid‐State Batteries

Riegger, Luise M.; Schlem, Roman; Sann, Joachim; Zeier, Wolfgang G.; Janek, Jürgen

doi:10.1002/ange.202015238

Cited by 41 publications

(53 citation statements)

References 40 publications

(53 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Also, Li 6 PS 5 Cl and Li 3 InCl 6 were even combined as the cathode-electrolyte. 89 There are few studies on the stability of halide electrolytes against the lithium metal anode. Janek's group has investigated the stability of Li 3 InCl 6 and Li 3 YCl 6 against lithium metal anode.…”

Section: Halidesmentioning

confidence: 99%

Ionic conductivity and ion transport mechanisms of solid‐state lithium‐ion battery electrolytes: A review

Yang

2022

Energy Science & Engineering

209

View full text Add to dashboard Cite

This review article deals with the ionic conductivity of solid-state electrolytes for lithium batteries. It has discussed the mechanisms of ion conduction in ceramics, polymers, and ceramic-polymer composite electrolytes. In ceramic electrolytes, ion transport is accomplished with mobile point defects in a crystal. Li + ions migrate mainly via the vacancy mechanism, interstitial mechanism, or interstitial-substitutional exchange mechanism. In solid polymer electrolytes, Li + ions are transported mainly via the segment motion, ion hopping (Grotthuss mechanism), or vehicle mechanism (mass diffusion). This study has also introduced various electrolyte materials including perovskite oxides, garnet oxides, sodium superionic conductors, phosphates, sulfides, halides, cross-linked polymers, block-copolymers, metal-organic frameworks, covalent organic frameworks, as well as ceramic-polymer composites. In addition, it has highlighted some strategies to improve the ionic conductivity of solid-state electrolytes, such as doping, defect engineering, microstructure tuning, and interface modification.

show abstract

Section: Halidesmentioning

confidence: 99%

Ionic conductivity and ion transport mechanisms of solid‐state lithium‐ion battery electrolytes: A review

Yang

2022

Energy Science & Engineering

209

View full text Add to dashboard Cite

show abstract

“…However, such configuration was not suitable to test Li3InCl6 due to its known instability at the anode interface leading to the reduction of In 3+ . 34 Thus, a hetero-structure cell design was employed. It consists in the use of Li3InCl6 only in the cathode composite, C-Li6PS5Cl as separator and a composite made of C-Li6PS5Cl and Li0.5In as the anode.…”

Section: Cathode Composites and Battery Testingmentioning

confidence: 99%

In Search of the Best Solid Electrolyte-Layered Oxide Pairing for Assembling Practical All-Solid-State Batteries

Koç

Marchini

Rousse

et al. 2021

ACS Appl. Energy Mater.

View full text Add to dashboard Cite

All-solid-state batteries (ASSBs) are the subject of large enthusiasm as they could boost by 50% the energy density of today's Li-ion batteries provided that several fundamental/practical roadblocks can be solved.Focusing on the interface between the solid electrolyte and cathode active material (CAM), we herein studied the chemical/electrochemical compatibility of coated-layered oxide LiNi0.6Mn0.2Co0.2O2 with the three main inorganic electrolytes contenders, these being lithium thiophosphate (β-Li3PS4), argyrodite (Li6PS5Cl), and halide (Li3InCl6). Such electrolytes were prepared by either solvent-free or solution chemistry and paired with the CAM to form a composite which was further tested by assembling solid-state batteries using Li0.5In as negative electrode. Amongst the electrolytes prepared by dry routes, the best performing was found to be Li6PS5Cl followed by β-Li3PS4 and lastly Li3InCl6. In contrast, no general trend of benefit or detriment was observed when switching to solution route as it resulted in either performance improvement or deterioration depending on the electrolyte. Additionally, we show a strong dependence of the battery performance upon the presence of carbon additives. Lastly, we unraveled a pronounced chemical/electrochemical incompatibility of Li3InCl6 towards Li6PS5Cl and β-Li3PS4, hence questioning the design of hetero-structural cell architectures. Altogether, we hope these findings to provide guidance in the proper pairing of electrode-electrolytes components for designing highly performing solid-state batteries.

show abstract

“…[23][24][25][26][27][28][29] Additionally, halide materials are promising candidates as cathode electrolytes due to their oxidation stability. 18,26,30 Schlem et al, showed that the conductivity of Li3ErCl6, Li3YCl6, and Li3YBr6 is strongly dependent on a cation site-disorder that is affected by the synthesis conditions, enabling tailoring of the energy landscape for lithium ion diffusion. 29,31 Moreover, studies showed that the heat treatment conditions strongly influence the ionic conductivity.…”

Section: Introductionmentioning

confidence: 99%

Exploring Aliovalent Substitutions in the Lithium Halide Superionic Conductor Li_3–xIn_1–xZr_xCl₆ (0 ≤ x ≤ 0.5)

et al. 2021

Self Cite

View full text Add to dashboard Cite

In recent years, ternary halides Li3MX6 (M = Y, Er, In; X = Cl, Br, I) have garnered attention as solid electrolytes due to their wide electrochemical stability window and favorable roomtemperature conductivities. In this material class, the influences of iso-or aliovalent substitutions are so far rarely studied in-depth, despite this being a common tool for correlating structure and transport properties. In this work, we investigate the impact of Zr substitution on the structure and ionic conductivity of Li3InCl6 (Li3-xIn1-xZrxCl6 with 0 ≤ x ≤ 0.5) using a combination of neutron diffraction, nuclear magnetic resonance and impedance spectroscopy.Analysis of high-resolution diffraction data shows the presence of an additional tetrahedrally coordinated lithium position together with cation site-disorder, both of which have not been reported previously for Li3InCl6. This Li + position and cation disorder lead to the formation of a three-dimensional lithium ion diffusion channel, instead of the expected two-dimensional diffusion. Upon Zr 4+ substitution, the structure exhibits non-uniform volume changes along with an increasing number of vacancies, all of which lead to an increasing ionic conductivity in this series of solid solutions.

show abstract

Lithium‐Metal Anode Instability of the Superionic Halide Solid Electrolytes and the Implications for Solid‐State Batteries

Cited by 41 publications

References 40 publications

Ionic conductivity and ion transport mechanisms of solid‐state lithium‐ion battery electrolytes: A review

Ionic conductivity and ion transport mechanisms of solid‐state lithium‐ion battery electrolytes: A review

In Search of the Best Solid Electrolyte-Layered Oxide Pairing for Assembling Practical All-Solid-State Batteries

Exploring Aliovalent Substitutions in the Lithium Halide Superionic Conductor Li_3–xIn_1–xZr_xCl₆ (0 ≤ x ≤ 0.5)

Contact Info

Product

Resources

About

Lithium‐Metal Anode Instability of the Superionic Halide Solid Electrolytes and the Implications for Solid‐State Batteries

Cited by 41 publications

References 40 publications

Ionic conductivity and ion transport mechanisms of solid‐state lithium‐ion battery electrolytes: A review

Ionic conductivity and ion transport mechanisms of solid‐state lithium‐ion battery electrolytes: A review

In Search of the Best Solid Electrolyte-Layered Oxide Pairing for Assembling Practical All-Solid-State Batteries

Exploring Aliovalent Substitutions in the Lithium Halide Superionic Conductor Li3–xIn1–xZrxCl6 (0 ≤ x ≤ 0.5)

Contact Info

Product

Resources

About

Exploring Aliovalent Substitutions in the Lithium Halide Superionic Conductor Li_3–xIn_1–xZr_xCl₆ (0 ≤ x ≤ 0.5)