Effects of Halogen and Sulfur Mixing on Lithium-Ion Conductivity in Li7-x-y(PS4)(S2-x-yClxBry) Argyrodite and the Mechanism for Enhanced Lithium Conduction

Article Engineering, Environmental

Chlorine-rich lithium argyrodite enabling solid-state batteries with capabilities of high voltage, high rate, low-temperature and ultralong cyclability

Linfeng Peng et al.

Summary: This study successfully improved the rate capability and cyclability of solid-state batteries by synthesizing a high-conductivity chloride Li5.5PS4.5Cl1.5 electrolyte and unraveling the role of carbon in the cathode mixture.

CHEMICAL ENGINEERING JOURNAL (2022)

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Article Chemistry, Physical

Synthesis, air stability and electrochemical investigation of lithium superionic bromine substituted argyrodite (Li6-xPS5-xCl1.0Brx) for all-solid-state lithium batteries

Yuvaraj Subramanian et al.

Summary: This study focuses on enhancing the ionic conductivity of lithium argyrodites by excess halogen substitution, resulting in a solid electrolyte with higher ionic conductivity and cycling stability. The optimized electrolyte shows improved capacity and capacity retention in solid battery systems, making it a promising candidate for lithium solid-state batteries. Moreover, the influence of excess halogen substitution on electrochemical kinetics is demonstrated through various techniques, showing the potential for further improvements in solid electrolyte performance.

JOURNAL OF POWER SOURCES (2022)

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Article Chemistry, Multidisciplinary

Opening Diffusion Pathways through Site Disorder: The Interplay of Local Structure and Ion Dynamics in the Solid Electrolyte Li6+xP1-xGexS5I as Probed by Neutron Diffraction and NMR

Katharina Hogrefe et al.

Summary: Solid electrolytes are crucial for future energy storage systems, and Li-bearing argyrodites are considered to be leading materials for Li+ ion conductivity. In this study, the effect of cation substitution on Li+ ion dynamics was investigated, revealing the microscopic origins of improved ion transport efficiency.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Multidisciplinary

Opening Diffusion Pathways through Site Disorder: The Interplay of Local Structure and Ion Dynamics in the Solid Electrolyte Li6+xP1-xGexS5I as Probed by Neutron Diffraction and NMR

Katharina Hogrefe et al.

Summary: This study focused on the impact of cation substitution on Li+ ion dynamics using Li6+xP1-xGexS5I as a model system, revealing that replacing P5+ with Ge4+ not only causes anion site disorder but also allows Li+ ions to occupy initially empty sites between Li rich cages. NMR results showed new Li+ exchange processes in Ge-rich samples with low activation barriers, facilitating rapid ion exchange processes between Li cages.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Physical

Influence of Aliovalent Cation Substitution and Mechanical Compression on Li-Ion Conductivity and Diffusivity in Argyrodite Solid Electrolytes

Parvin Adeli et al.

Summary: The study introduces dual-modified superionic conductors in the Li-argyrodite family prepared by a rapid synthesis method, showing improved Li+ diffusion and conductivity through aliovalent doping. The materials exhibit exceptional room temperature conductivity and diffusivity. Mechanical modification's impact on grain boundary diffusion in sulfide electrolytes was probed using PFG-NMR, highlighting the efficacy of particle-scale materials engineering modifications.

CHEMISTRY OF MATERIALS (2021)

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Article Chemistry, Physical

Engineering the Site-Disorder and Lithium Distribution in the Lithium Superionic Argyrodite Li6PS5Br

Ajay Gautam et al.

Summary: The study shows that controlling site-disorder in Li6PS5Br by adjusting synthesis conditions can enhance lithium ion diffusion pathways and increase ionic conductivity. Experimental results and ab initio molecular dynamics simulations corroborate each other, highlighting the importance of this modulation method for design and optimization of argyrodites.

ADVANCED ENERGY MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Superionic Si-Substituted Lithium Argyrodite Sulfide Electrolyte Li6+xSb1-xSixS5I for All-Solid-State Batteries

Yongheum Lee et al.

Summary: The study investigated the high ionic conductivities of Li6+xSb1-xSixS5I using first-principles calculations and experiments, demonstrating favorable characteristics like high ionic conductivity, low activation energy, and good stability. The high Si content in the superionic conductor Li6.75Sb0.25Si0.75S5I shows substantial promise for practical use in all-solid-state Li batteries.

ACS SUSTAINABLE CHEMISTRY & ENGINEERING (2021)

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Article Chemistry, Physical

Tunable Lithium-Ion Transport in Mixed-Halide Argyrodites Li6-xPS5-xClBrx: An Unusual Compositional Space

Sawankumar Patel et al.

Summary: This study introduces a new compositional space of argyrodite superionic conductors, Li6-xPS5-xClBrx [0 <= x <= 0.8], with high ionic conductivity and low lithium migration barrier. Bromination treatment can maintain the parent Li6PS5Cl structure within a certain range, leading to enhanced Li+ ion dynamics and a liquid-like Li sublattice. Halogen-rich compositions induce hypercoordination and coordination entropy, enhancing Li+ ion transport in the material.

CHEMISTRY OF MATERIALS (2021)

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Article Chemistry, Physical

Mechanistic Origin of Superionic Lithium Diffusion in Anion-Disordered Li6PS5X Argyrodites

Benjamin J. Morgan

Summary: The key to rapid ion transport lies in the substitutional anion disorder, which affects the lithium ion diffusion pathways and ultimately impacts the overall ionic conductivity. In materials where the anions are disordered, a three-dimensional diffusion network is established, allowing for long-ranged lithium diffusion through a concerted string-like mechanism. Conversely, in materials where the anions are ordered, lithium ions exhibit pseudo-ordering, hindering long-ranged diffusion and leading to localized lithium motion around sulfur positions.

CHEMISTRY OF MATERIALS (2021)

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Article Materials Science, Multidisciplinary

Methodology for enhancing the ionic conductivity of superionic halogen-rich argyrodites for all-solid-state lithium batteries

Shintaro Kitajima et al.

Summary: The study discovered halogen-rich argyrodites with high ionic conductivities and determined the optimal heat treatment protocol. Analysis of different heating speeds showed that slow heating promotes high ionic conductivity. Experimental results of all-solid-state batteries indicated that materials treated with slow heating outperformed those treated with fast heating.

MATERIALS TODAY COMMUNICATIONS (2021)

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Article Chemistry, Physical

On the Lithium Distribution in Halide Superionic Argyrodites by Halide Incorporation in Li7-xPS6-xClx

Ajay Gautam et al.

Summary: The study investigates the effects of different halide compositions on the ionic conductivity in superionic lithium argyrodites, revealing that replacement of S2- by Cl- increases Li+ conductivity by connecting clustered Li+ cages. This demonstrates the importance of anionic charge distribution changes on the structural-transport correlations within the Li+ ion substructure.

ACS APPLIED ENERGY MATERIALS (2021)

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Article Chemistry, Physical

Fast Ion Conduction and Its Origin in Li6-xPS5-xBr1+x

Pengbo Wang et al.

CHEMISTRY OF MATERIALS (2020)

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Article Chemistry, Physical

Superionic conductivity in lithium argyrodite solid-state electrolyte by controlled Cl-doping

Chuang Yu et al.

NANO ENERGY (2020)

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Article Chemistry, Multidisciplinary

Superionic Halogen-Rich Li-Argyrodites Using In Situ Nanocrystal Nucleation and Rapid Crystal Growth

Wo Dum Jung et al.

NANO LETTERS (2020)

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Article Chemistry, Physical

Structure and Diffusion Pathways in Li6PS5Cl Argyrodite from Neutron Diffraction, Pair-Distribution Function Analysis, and NMR

Ruth Schlenker et al.

CHEMISTRY OF MATERIALS (2020)

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Article Chemistry, Physical

Enabling ultrafast ionic conductivity in Br-based lithium argyrodite electrolytes for solid-state batteries with different anodes

Chuang Yu et al.

ENERGY STORAGE MATERIALS (2020)

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Article Chemistry, Physical

Enhanced ion conduction by enforcing structural disorder in Li-deficient argyrodites Li6-xPS5-xCl1-x

Xuyong Peng et al.

ENERGY STORAGE MATERIALS (2020)

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Article Chemistry, Physical

A lithium argyrodite Li6PS5Cl0.5Br0.5 electrolyte with improved bulk and interfacial conductivity

Heng Wang et al.

JOURNAL OF POWER SOURCES (2019)

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Article Chemistry, Multidisciplinary

Boosting Solid-State Diffusivity and Conductivity in Lithium Superionic Argyrodites by Halide Substitution

Parvin Adeli et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2019)

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Article Chemistry, Physical

Rapid Crystallization and Kinetic Freezing of Site-Disorder in the Lithium Superionic Argyrodite Li6PS5Br

Ajay Gautam et al.

CHEMISTRY OF MATERIALS (2019)

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Article Chemistry, Physical

Lithium Conductivity and Meyer-Neldel Rule in Li3PO4-Li3VO4-Li4GeO4 Lithium Superionic Conductors

Sokseiha Muy et al.

CHEMISTRY OF MATERIALS (2018)

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Article Electrochemistry

Lithium dissolution/deposition behavior with Li3PS4-LiI electrolyte for all-solid-state batteries operating at high temperatures

Motoshi Suyama et al.

ELECTROCHIMICA ACTA (2018)

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Article Chemistry, Multidisciplinary

Comparing the Descriptors for Investigating the Influence of Lattice Dynamics on Ionic Transport Using the Superionic Conductor Na3PS4-xSex

Thorben Krauskopf et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2018)

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Article Chemistry, Multidisciplinary

Inducing High Ionic Conductivity in the Lithium Superionic Argyrodites Li6+x P(1-x)Ge(x)S(5)l for All -Solid-State Batteries

Marvin A. Kraft et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2018)

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Article Chemistry, Multidisciplinary

Influence of Lattice Polarizability on the Ionic Conductivity in the Lithium Superionic Argyrodites Li6PS5X (X = Cl, Br, I)

Marvin A. Kraft et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2017)

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Review Green & Sustainable Science & Technology

A review of lithium-ion battery state of charge estimation and management system in electric vehicle applications: Challenges and recommendations

M. A. Hannan et al.

RENEWABLE & SUSTAINABLE ENERGY REVIEWS (2017)

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Article Chemistry, Physical

Diffusion Mechanism of Li Argyrodite Solid Electrolytes for Li-Ion Batteries and Prediction of Optimized Halogen Doping: The Effect of Li Vacancies, Halogens, and Halogen Disorder

Niek J. J. de Klerk et al.

CHEMISTRY OF MATERIALS (2016)

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Editorial Material Energy & Fuels

A solid future for battery development

Juergen Janek et al.

NATURE ENERGY (2016)

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Article Energy & Fuels

High-power all-solid-state batteries using sulfide superionic conductors

Yuki Kato et al.

NATURE ENERGY (2016)

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Article Materials Science, Ceramics

Development of an electrochemical impedance analysis program based on the expanded measurement model

Kiyoshi Kobayashi et al.

JOURNAL OF THE CERAMIC SOCIETY OF JAPAN (2016)

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Article Chemistry, Multidisciplinary

Hydride in BaTiO2.5H0.5: A Labile Ligand in Solid State Chemistry

Naoya Masuda et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2015)

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Article Chemistry, Physical

Highly Mobile Ions: Low-Temperature NMR Directly Probes Extremely Fast Li+ Hopping in Argyrodite-Type Li6PS5Br

Viktor Epp et al.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2013)

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Article Physics, Condensed Matter

The proton conducting electrolyte BaTi0.5In0.5O2.75: determination of the deuteron site and its local environment

Stefan T. Norberg et al.

JOURNAL OF PHYSICS-CONDENSED MATTER (2013)

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Article Chemistry, Physical

Electrochemical properties of all-solid-state lithium secondary batteries using Li-argyrodite Li6PS5Cl as solid electrolyte

Sylvain Boulineau et al.

SOLID STATE IONICS (2013)

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Article Chemistry, Physical

Formation and conductivity studies of lithium argyrodite solid electrolytes using in-situ neutron diffraction

R. Prasada Rao et al.

SOLID STATE IONICS (2013)

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Article Chemistry, Multidisciplinary

VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data

Koichi Momma et al.

JOURNAL OF APPLIED CRYSTALLOGRAPHY (2011)

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Article Chemistry, Physical

High rate capabilities of all-solid-state lithium secondary batteries using Li4Ti5O12-coated LiNi0.8Co0.15Al0.05O2 and a sulfide-based solid electrolyte

Yoshikatsu Seino et al.

JOURNAL OF POWER SOURCES (2011)

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Review Chemistry, Multidisciplinary

Review of solutions to global warming, air pollution, and energy security

Mark Z. Jacobson

ENERGY & ENVIRONMENTAL SCIENCE (2009)

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Article Chemistry, Inorganic & Nuclear

Neutron powder diffraction and difference maximum entropy method analysis of protium- and deuterium-dissolved BaSn0.5In0.5O2.75+α

Takanori Nagasaki et al.

JOURNAL OF SOLID STATE CHEMISTRY (2009)

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Location of deuteron sites in the proton conducting perovskite BaZr0.50In0.50O3-y

Istaq Ahmed et al.

JOURNAL OF ALLOYS AND COMPOUNDS (2008)

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Crystal structure and diffusion path in the fast lithium-ion conductor La0.62Li0.16TiO3

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2005)

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Effects of Halogen and Sulfur Mixing on Lithium-Ion Conductivity in Li7-x-y(PS4)(S2-x-yClxBry) Argyrodite and the Mechanism for Enhanced Lithium Conduction

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