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RESEARCH PAPER · Angewandte Chemie International Edition · 2023

New Oxyhalide Solid Electrolytes with High Lithium Ionic Conductivity >10 mS cm −1 for All‐Solid‐State Batteries

Yoshiaki Tanaka, Koki Ueno, Keita Mizuno, Kaori Takeuchi, Tetsuya Asano, Akihiro Sakai

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New Oxyhalide Solid Electrolytes with High Lithium Ionic Conductivity >10 mS cm −1 for All‐Solid‐State BatteriesOriginalLi ion diffusion behavior of Li 3 OCl solid-state electrolytes with different defect structures: insights from the deep potential model20Revealing the Pnma crystal structure and ion-transport mechanism of the Li3YCl6 solid electrolyte39Li3–xZrx(Ho/Lu)1–xCl6 Solid Electrolytes Enable Ultrahigh-Loading Solid-State Batteries with a Prelithiated Si Anode91A cost-effective, ionically conductive and compressible oxychloride solid-state electrolyte for stable all-solid-state lithium-based batteries271Developments in New Materials for Electrochemistry and Energy Storage Devices20Towards practically accessible high-voltage solid-state lithium batteries: From fundamental understanding to engineering design61Ultrathin Superhydrophobic Coatings for Air‐Stable Inorganic Solid Electrolytes: Toward Dry Room Application for All‐Solid‐State Batteries66A Roadmap for Solid‐State Batteries207A perspective on the building blocks of a solid-state battery: from solid electrolytes to quantum power harvesting and storage27Interfacial Challenges, processing strategies, and composite applications for high voltage all-solid-state lithium batteries based on halide and sulfide solid-state electrolytes68Universal F4‐Modified Strategy on Metal–Organic Framework to Chemical Stabilize PVDF‐HFP as Quasi‐Solid‐State Electrolyte207Amorphous Chloride Solid Electrolytes with High Li-Ion Conductivity for Stable Cycling of All-Solid-State High-Nickel Cathodes160Anion Engineering for Stabilizing Li Interstitial Sites in Halide Solid Electrolytes for All-Solid-State Li Batteries34Polyoxometalate Li3PW12O40 and Li3PMo12O40 Electrolytes for High‐energy All‐solid‐state Lithium Batteries2Polyoxometalate Li3PW12O40 and Li3PMo12O40 Electrolytes for High‐energy All‐solid‐state Lithium Batteries45An Insight into Halide Solid-State Electrolytes: Progress and Modification Strategies77Hierarchically coated halide layers: enhancing the performance at composite cathode interfaces in solid-state Li–metal batteries20In situ interfacial reactions in hydride–oxide composite electrolytes for stable all-solid-state Li–metal batteries1New advances in solid-state electrolytes: from halides to oxyhalides29Revealing unprecedented cathode interface behavior in all-solid-state batteries with oxychloride solid electrolytes44Safety concerns in solid-state lithium batteries: from materials to devices143Superionic Halide Solid Electrolyte Li1.7zr0.7ta0.3cl6 for Durable All-Solid-State Lithium Batteries0Systematically Evaluation of the Cathodic Performance of Crobr with Vacancies and Partial Substitutions on Surface for Metal Batteries0Unraveling the interfacial compatibility of ultrahigh nickel cathodes and chloride solid electrolyte for stable all-solid-state lithium batteries44Stable Binder Boosting Sulfide Solid Electrolyte Thin Membrane for All-Solid-State Lithium Batteries66Modification of solid electrolyte interface layer between PVDF-based electrolyte and lithium anode22Solid Interfaces for the Garnet Electrolytes91Cubic Iodide LixYI3+x Superionic Conductors through Defect Manipulation for All‐Solid‐State Li Batteries47Cubic Iodide LixYI3+x Superionic Conductors through Defect Manipulation for All‐Solid‐State Li Batteries3Research progress on chloride solid electrolytes for all-solid-state batteries49Amorphous Oxyhalide Matters for Achieving Lithium Superionic Conduction186Influence Mechanism of Interfacial Oxidation of Li3YCl6 Solid Electrolyte on Reduction Potential10Nanoscale Visualization of Lithium Plating/Stripping Tuned by On‐site Formed Solid Electrolyte Interphase in All‐Solid‐State Lithium‐Metal Batteries18Nanoscale Visualization of Lithium Plating/Stripping Tuned by On‐site Formed Solid Electrolyte Interphase in All‐Solid‐State Lithium‐Metal Batteries3Inorganic lithium-ion conductors for fast-charging lithium batteries: a review9Strategies of Enhancing Ionic Conductivity in Model Solid‐State Electrolyte Li15P4S16Cl38Surface Lattice Modulation Enables Stable Cycling of High‐Loading All‐solid‐state Batteries at High Voltages34Surface Lattice Modulation Enables Stable Cycling of High‐Loading All‐solid‐state Batteries at High Voltages6Materials and chemistry design for low-temperature all-solid-state batteries121NaTaCl6: Chloride as the End-Member of Sodium-Ion Conductors40Halide Superionic Conductors with Non‐Close‐Packed Anion Frameworks0Halide Superionic Conductors with Non‐Close‐Packed Anion Frameworks36Electronic structure modulation of iron sites with fluorine coordination enables ultra-effective H2O2 activation132Enhancing moisture and electrochemical stability of the Li5.7PS4.7Cl1.3 electrolyte by boron nitride coating for all-solid-state lithium metal batteries6Fluorinated Superionic Oxychloride Solid Electrolytes for High-Voltage All-Solid-State Lithium Batteries72Origin of Fast Li+-Ion Conductivity in the Compressible Oxyhalide LiNbOCl431Ternary Rotational Polyanion Coupling Enables Fast Li Ion Dynamics in Tetrafluoroborate Ion Doped Antiperovskite Li2OHCl Solid Electrolyte0Ternary Rotational Polyanion Coupling Enables Fast Li Ion Dynamics in Tetrafluoroborate Ion Doped Antiperovskite Li2OHCl Solid Electrolyte13Lithium Metal-Compatible Antifluorite Electrolytes for Solid-State Batteries39Exploring Layered Disorder in Lithium-Ion-Conducting Li3Y1–xInxCl621LaCl3-based sodium halide solid electrolytes with high ionic conductivity for all-solid-state batteries88General synthesis of ionic-electronic coupled two-dimensional materials34Lithium Batteries – Lithium Secondary Batteries – Lithium All-Solid State Battery | Overview0Constructing An Oxyhalide Interface for 4.8 V‐Tolerant High‐Nickel Cathodes in All‐Solid‐State Lithium‐Ion Batteries52Constructing An Oxyhalide Interface for 4.8 V‐Tolerant High‐Nickel Cathodes in All‐Solid‐State Lithium‐Ion Batteries8An Active Halide Catholyte Boosts the Extra Capacity for All‐Solid‐State Batteries42Critical Role of Framework Flexibility and Disorder in Driving High Ionic Conductivity in LiNbOCl 478In Situ Analysis of Interfacial Morphological and Chemical Evolution in All‐Solid‐State Lithium‐Metal Batteries43In Situ Analysis of Interfacial Morphological and Chemical Evolution in All‐Solid‐State Lithium‐Metal Batteries0High-Voltage Long-Cycling All-Solid-State Lithium Batteries with High-Valent-Element-Doped Halide Electrolytes60Wet Chemistry Route to Li3InCl6: Microstructural Control Render High Ionic Conductivity and Enhanced All‐Solid‐State Battery Performance48Sodium Metal Oxyhalides NaMOCl4 (M = Nb, Ta) with High Ionic Conductivities494 V Na Solid State Batteries Enabled by a Scalable Sodium Metal Oxyhalide Solid Electrolyte62Structure designing, interface engineering, and application prospects for sodium‐ion inorganic solid electrolytes46Long‐Life All‐Solid‐State Batteries Enabled by Cold‐Pressed Garnet Composite Electrolytes with Enhanced Li + Conduction13Long‐Life All‐Solid‐State Batteries Enabled by Cold‐Pressed Garnet Composite Electrolytes with Enhanced Li+ Conduction8High Performance All‐Solid‐State Lithium Batteries: Interface Regulation Mechanism15Progress and Challenges in Buffer Layers Between Cathode Materials and Sulfide Solid Electrolytes in All‐Solid‐State Batteries28Superionic halide solid electrolyte Li1.7Zr0.7Ta0.3Cl6 for durable all-solid-state lithium batteries40The importance of A-site cation chemistry in superionic halide solid electrolytes10Tuning the Properties of Halide Nanocomposite Solid Electrolytes with Diverse Oxides for All-Solid-State Batteries7Diffusion mechanisms of fast lithium-ion conductors171A New Class of Oxyhalide Solid Electrolytes NaNbCl6‐2xOx for Solid‐state Sodium Batteries1A New Class of Oxyhalide Solid Electrolytes NaNbCl6‐2xOx for Solid‐state Sodium Batteries46A family of dual-anion-based sodium superionic conductors for all-solid-state sodium-ion batteries148Li 2.9 Fe 0.9 Zr 0.1 Cl 6 as Redox-Active Catholyte for Solid-State Li-Ion Batteries13Novel Amorphous Nitride‐Halide Solid Electrolytes with Enhanced Performance for All‐Solid‐State Batteries4Novel Amorphous Nitride‐Halide Solid Electrolytes with Enhanced Performance for All‐Solid‐State Batteries43Synthesis, Structure, and Electrochemistry of Crystallized Layered Chlorides, LiMCl6 (M = Ta/Nb)23A Rapid Synthesis of Amorphous LiTaOCl 4 Solid Electrolytes Through a Two‐Step Reaction Pathway for High‐Rate and Long‐Cycling Lithium Batteries36Exploring the Potential of Halide Electrolytes for Next‐Generation All‐Solid‐State Lithium Batteries77Halide solid electrolytes in all-solid-state batteries: Ion transport kinetics, failure mechanisms and improvement strategies33Nanoarchitectonics for Biomedical Research: Post‐Nanotechnology Materials Approach for Bio‐Active Application6Metalloid Phosphorus Induces Tunable Defect Engineering in High Entropy Oxide Toward Advanced Lithium‐Ion Batteries33Research Progress on Solid-State Electrolytes in Solid-State Lithium Batteries: Classification, Ionic Conductive Mechanism, Interfacial Challenges53A Solid Electrolyte Based on Sodium‐Doped Li4‐xNaxTi5O12 with PVDF for Solid State Lithium Metal Battery2Commonalities and Characteristics Analysis of Fluorine and Iodine used in Lithium‐Based Batteries4Emerging Superionic Sulfide and Halide Glass–Ceramic Solid Electrolytes: Recent Progress and Future Perspectives26Deciphering and overcoming the high-voltage limitations of halide and sulfide-based all-solid-state lithium batteries23Fast ionic conduction achieved through the design and synthesis of ceramic heterointerfaces26Multi‐Electron Transfer Halide Cathode Materials Based on Intercalation‐Conversion Reaction Towards All‐Solid‐State Lithium Batteries20Multi‐Electron Transfer Halide Cathode Materials Based on Intercalation‐Conversion Reaction Towards All‐Solid‐State Lithium Batteries8Tailoring Ion Transport in Li3‐3yHo1+yCl6‐xBrx via Transition‐Metal Free Structural Planes and Charge Carrier Distribution10Advancing high-voltage halide-based solid-state batteries: Interfacial challenges, material innovations, and applications26Fast‐Charging Solid‐State Li Batteries: Materials, Strategies, and Prospects44Interfacial Challenges of Halide‐Based All‐Solid‐State Batteries62A Li-enriched amorphous Zr-based oxychloride solid electrolyte for high-rate and long-cycling all-solid-state ultrahigh-nickel cathodes2A low-cost, lithium-rich zirconium-based oxyhalide solid electrolyte featuring an efficient ion transport structure4Amorphous oxyhalide solid electrolytes with improved ionic conductivity and reductive stability for all-solid-state batteries12Computational Insights into Superionic Behavior of Amorphous Lithium Oxyhalide 1.6li2o-Tacl5 Solid Electrolyte0Halide-based solid electrolytes: opportunities and challenges in the synergistic development of all-solid-state Li/Na batteries22Insight into the prospects and limitations of mechanochemically-synthesised lithium tetrahalogallates, LiGaX 4 (X = Cl, Br, I), as Li-ion conductors2Insights into chemical substitution of metal halide solid-state electrolytes for all-solid-state lithium batteries11Insights into the chemical and electrochemical behavior of halide and sulfide electrolytes in all-solid-state batteries18Oxygen-tuned aluminum-based halide solid electrolytes enabling low-voltage anode compatibility in all-solid-state batteries31Solid-state electrolytes expediting interface-compatible dual-conductive cathodes for all-solid-state batteries15Synthesis and interfacial engineering of nitride–halide electrolytes in all-solid-state Li batteries7The chemistry of halide-based solid electrolytes: unlocking advances in solid-state Li-ion batteries20All-solid-state batteries designed for operation under extreme cold conditions50Advancements in the emerging rare-earth halide solid electrolytes for next-generation all-solid-state lithium batteries29Building a Better All-Solid-State Lithium-Ion Battery with Halide Solid-State Electrolyte62Structural and Li-Ion Conduction Properties of Ti- and W-Substituted LiTa2PO84Challenges and advances in low-temperature solid-state batteries19Fluorinated coating stabilizing halide solid electrolytes for all-solid-state lithium metal batteries19Characterizing Electrode Materials and Interfaces in Solid-State Batteries233Hydrochloric acid-free synthesis of LiNbOCl4 superionic conductor for all-solid-state Li batteries14Current trends and recent strategies to overcome battery safety issues18Ductile Inorganic Solid Electrolytes for All-Solid-State Lithium Batteries164Exploring the soft cradle effect and ionic transport mechanisms in the LiMXCl4 superionic conductor family301 +1 > 2 Effect Induced by Space Charge in Solid Electrolytes5Chemical Composition-Driven Machine Learning Models for Predicting Ionic Conductivity in Lithium-Containing Oxides2A Low-Strain Lithium Cathode Material Li 2–2 x Fe 1+ x Cl 4 for Halide-Based All-Solid-State Batteries15A Pre‐Oxidation Strategy to Establish Stable Oxide Cathode/Halide Solid‐State Electrolyte Interfaces for High Energy all Solid‐State Batteries11Exploring the Anion Site Disorder Kinetics in Lithium Argyrodites11Graded Cathode Design for Enhanced Performance of Sulfide-Based Solid-State Batteries28Surface engineering for high voltage LiCoO2 in halide all-solid-state lithium-ion batteries6Activating Interfacial Ion Exchange in Composite Electrolytes to Realize High‐Rate and Long‐Cycling Solid‐State Lithium Batteries1Activating Interfacial Ion Exchange in Composite Electrolytes to Realize High‐Rate and Long‐Cycling Solid‐State Lithium Batteries28Unraveling the Highly Reversible Lithiation/Delithiation of Aluminum in Inorganic All-Solid-State Lithium Batteries7Superhalogen-Based Double Antiperovskite Li6NBr(BH4)2: Structural Stability and Li Ion Transport Characteristics0Research progress and perspectives on rechargeable batteries30An all-garnet-type solid-state lithium-ion battery3High-voltage and high-capacity oxide cathode materials in sulfide-based all–solid–state lithium batteries9Solid-State Electrolytes and Their Interfacial Properties: Implications for Solid-State Lithium Batteries63Halide Chemistry Boosts All‐Solid‐State Li‐S Batteries9Boosting the ionic conductivity of amorphous oxychloride solid electrolytes via different degrees of amorphization21Multi-Solid-Electrolyte Systems for All-Solid-State Batteries: Current Status and Future Prospects16Unprecedented Superionicity of Ultra-Low Barrier in A0.5CoO2 (A = Li, Zn)0Machine Learning Assisted Materials Classification to Boost Catalyst Design for Electrochemical Oxidation5The wide range of battery systems: From micro- to structural batteries, from biodegradable to high performance batteries30Crystalline Li-Ta-Oxychlorides with Lithium Superionic Conduction1Revealing the Underlying Role of Li 2 CO 3 in Enhancing Performance of Oxyhalide‐Based Solid‐State Batteries12Unraveling Ultrafast Li-Ion Dynamics in the Solid Electrolyte LiTi2(PS4)3 by NMR down to Cryogenic Temperatures9Vacancy Driven Fast Ion Conduction in Lithium Deficient Magnesium Chloride Spinel6Fast lithium-ion diffusion in pyrochlore-type oxyfluoride Li1.25La0.58Nb2O6F5Assessing the Impact of Li+ Concentration and Stacking Faults in the Aliovalent-Substituted Ionic Conductor Li3ScCl63Near-Saturated Coordinated Cations in Oxyhalide Superionic Conductors Boost High-Rate All-Solid-State Batteries45Enhancing Compatibility of Halide with Sulfide‐Electrolytes via High Oxygen Incorporation for Robust Solid‐State Batteries31Li and Vacancy Co‐Enriched Halide Electrolytes via Non‐Equimolar Substitution for Stable All‐Solid‐State Lithium Batteries16Accelerated data-driven materials science with the Materials Project296

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  31. Amorphous Oxyhalide Matters for Achieving Lithium Superionic Conduction

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  36. Strategies of Enhancing Ionic Conductivity in Model Solid‐State Electrolyte Li15P4S16Cl3

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  50. Exploring Layered Disorder in Lithium-Ion-Conducting Li3Y1–xInxCl6

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