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RESEARCH PAPER · Chemical Reviews · 2017

Odyssey of Multivalent Cathode Materials: Open Questions and Future Challenges

Pieremanuele Canepa, Gopalakrishnan Sai Gautam, Daniel C. Hannah, Rahul Malik, Miao Liu, Kevin G. Gallagher, Kristin Aslaug Persson, Gerbrand Ceder

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Odyssey of Multivalent Cathode Materials: Open Questions and Future ChallengesOriginalOn the Reliability of Half-Cell Tests for Monovalent (Li + , Na + ) and Divalent (Mg 2+ , Ca 2+ ) Cation Based Batteries138Fervent Hype behind Magnesium Batteries: An Open Call to Synthetic Chemists—Electrolytes and Cathodes Needed270Chemistry-Inspired Adaptable Framework Structures368Lithium ion, lithium metal, and alternative rechargeable battery technologies: the odyssey for high energy density1116Production of Liquid Solar Fuels and Their Use in Fuel Cells240High-Voltage Aqueous Magnesium Ion Batteries378Two-Dimensional Vanadium Carbide (MXene) as a High-Capacity Cathode Material for Rechargeable Aluminum Batteries611Reducing Mg Anode Overpotential via Ion Conductive Surface Layer Formation by Iodine Additive153Revitalized interest in vanadium pentoxide as cathode material for lithium-ion batteries and beyond313High magnesium mobility in ternary spinel chalcogenides306Carbons from biomass precursors as anode materials for lithium ion batteries: New insights into carbonization and graphitization behavior and into their correlation to electrochemical performance219Plating and stripping calcium in an organic electrolyte429Towards high-performance dual-graphite batteries using highly concentrated organic electrolytes159A critical review of cathodes for rechargeable Mg batteries591A rechargeable aqueous Zn 2+ -battery with high power density and a long cycle-life311An adaptive and stable bio-electrolyte for rechargeable Zn-ion batteries237An electrochemically induced bilayered structure facilitates long-life zinc storage of vanadium dioxide250Aqueous vs. nonaqueous Zn-ion batteries: consequences of the desolvation penalty at the interface832Binder-free stainless steel@Mn 3 O 4 nanoflower composite: a high-activity aqueous zinc-ion battery cathode with high-capacity and long-cycle-life329Li + intercalated V 2 O 5 · n H 2 O with enlarged layer spacing and fast ion diffusion as an aqueous zinc-ion battery cathode998Novel layered iron vanadate cathode for high-capacity aqueous rechargeable zinc batteries195High Rate Magnesium–Sulfur Battery with Improved Cyclability Based on Metal–Organic Framework Derivative Carbon Host187Electrochemical Intercalation of Calcium and Magnesium in TiS2: Fundamental Studies Related to Multivalent Battery Applications146Pre-Lithiation Strategies for Rechargeable Energy Storage Technologies: Concepts, Promises and Challenges358Reversible Mg-Ion Insertion in a Metastable One-Dimensional Polymorph of V2O5185On the road toward calcium-based batteries164Magnesium storage performance and mechanism of CuS cathode233High-Capacity Mg–Organic Batteries Based on Nanostructured Rhodizonate Salts Activated by Mg–Li Dual-Salt Electrolyte152Existence of Solid Electrolyte Interphase in Mg Batteries: Mg/S Chemistry as an Example141Novel Potassium-Ion Hybrid Capacitor Based on an Anode of K 2 Ti 6 O 13 Microscaffolds248A Universal Organic Cathode for Ultrafast Lithium and Multivalent Metal Batteries222Organic Cathode for Aqueous Zn-Ion Batteries: Taming a Unique Phase Evolution toward Stable Electrochemical Cycling493Ammonium Vanadium Bronze (NH 4 V 4 O 10 ) as a High-Capacity Cathode Material for Nonaqueous Magnesium-Ion Batteries162Ultrafast Zn 2+ Intercalation and Deintercalation in Vanadium Dioxide677Vanadium-Based Cathode Materials for Rechargeable Multivalent Batteries: Challenges and Opportunities219Emerging Nonaqueous Aluminum‐Ion Batteries: Challenges, Status, and Perspectives504Interlayer‐Spacing‐Regulated VOPO4 Nanosheets with Fast Kinetics for High‐Capacity and Durable Rechargeable Magnesium Batteries235Rechargeable Magnesium Batteries using Conversion‐Type Cathodes: A Perspective and Minireview178Calcium‐Ion Batteries: Current State‐of‐the‐Art and Future Perspectives431Potassium vanadates with stable structure and fast ion diffusion channel as cathode for rechargeable aqueous zinc-ion batteries540Polyaniline-intercalated manganese dioxide nanolayers as a high-performance cathode material for an aqueous zinc-ion battery1466Toward Highly Reversible Magnesium–Sulfur Batteries with Efficient and Practical Mg[B(hfip)4]2 Electrolyte339How Water Accelerates Bivalent Ion Diffusion at the Electrolyte/Electrode Interface157High-rate and durable aqueous zinc ion battery using dendritic V10O24·12H2O cathode material with large interlamellar spacing165Recent Advances in Aqueous Zinc-Ion Batteries2258Water-Activated VOPO4 for Magnesium Ion Batteries165Evaluating transition metal oxides within DFT-SCAN and SCAN + U frameworks for solar thermochemical applications173Self-Healing Lamellar Structure Boosts Highly Stable Zinc-Storage Property of Bilayered Vanadium Oxides208Progress in Rechargeable Aqueous Zinc‐ and Aluminum‐Ion Battery Electrodes: Challenges and Outlook208Rechargeable aluminium organic batteries402Before Li Ion Batteries2189Directing Mg-Storage Chemistry in Organic Polymers toward High-Energy Mg Batteries200Formation of Magnesium Dendrites during Electrodeposition333A review on recent developments and challenges of cathode materials for rechargeable aqueous Zn-ion batteries550Advances in sodium secondary batteries utilizing ionic liquid electrolytes216Expanded hydrated vanadate for high-performance aqueous zinc-ion batteries803Rechargeable aqueous hybrid ion batteries: developments and prospects168Ultrastable and High-Performance Zn/VO 2 Battery Based on a Reversible Single-Phase Reaction302Flexible Zn‐Ion Batteries: Recent Progresses and Challenges566Microwave-Assisted Synthesis of CuS Hierarchical Nanosheets as the Cathode Material for High-Capacity Rechargeable Magnesium Batteries144Mg Cathode Materials and Electrolytes for Rechargeable Mg Batteries: A Review146Paving the Path toward Reliable Cathode Materials for Aluminum‐Ion Batteries332A Stable, Non‐Corrosive Perfluorinated Pinacolatoborate Mg Electrolyte for Rechargeable Mg Batteries184Vanadium Oxide Pillared by Interlayer Mg2+ Ions and Water as Ultralong-Life Cathodes for Magnesium-Ion Batteries298A Metal-Organic Framework Host for Highly Reversible Dendrite-free Zinc Metal Anodes937Multivalent rechargeable batteries410Tuning Anionic Chemistry To Improve Kinetics of Mg Intercalation139Recent progress and perspectives on aqueous Zn-based rechargeable batteries with mild aqueous electrolytes712Machine Learning the Voltage of Electrode Materials in Metal-Ion Batteries199The Aluminum-Ion Battery: A Sustainable and Seminal Concept?254High-performance flexible quasi-solid-state zinc-ion batteries with layer-expanded vanadium oxide cathode and zinc/stainless steel mesh composite anode264Bilayered Mg 0.25 V 2 O 5 ·H 2 O as a Stable Cathode for Rechargeable Ca-Ion Batteries200Diethyl ether as self-healing electrolyte additive enabled long-life rechargeable aqueous zinc ion batteries632Electrode Materials for Rechargeable Zinc-Ion and Zinc-Air Batteries: Current Status and Future Perspectives172Progress in development of electrolytes for magnesium batteries247Pseudo‐Zn–Air and Zn‐Ion Intercalation Dual Mechanisms to Realize High‐Areal Capacitance and Long‐Life Energy Storage in Aqueous Zn Battery153Halide‐Based Materials and Chemistry for Rechargeable Batteries238Simultaneous Cationic and Anionic Redox Reactions Mechanism Enabling High‐Rate Long‐Life Aqueous Zinc‐Ion Battery198Inhibiting VOPO 4 ⋅ x H 2 O Decomposition and Dissolution in Rechargeable Aqueous Zinc Batteries to Promote Voltage and Capacity Stabilities186Methods and Protocols for Reliable Electrochemical Testing in Post-Li Batteries (Na, K, Mg, and Ca)141A Zn(ClO4)2 Electrolyte Enabling Long-Life Zinc Metal Electrodes for Rechargeable Aqueous Zinc Batteries156Achievements, Challenges, and Prospects of Calcium Batteries428Emerging rechargeable aqueous aluminum ion battery: Status, challenges, and outlooks178Electronic Structure Regulation of Layered Vanadium Oxide via Interlayer Doping Strategy toward Superior High‐Rate and Low‐Temperature Zinc‐Ion Batteries458Zinc anode-compatible in-situ solid electrolyte interphase via cation solvation modulation953Low-cost MgFexMn2-xO4 cathode materials for high-performance aqueous rechargeable magnesium-ion batteries137High‐Energy Interlayer‐Expanded Copper Sulfide Cathode Material in Non‐Corrosive Electrolyte for Rechargeable Magnesium Batteries201Layered intercalation compounds: Mechanisms, new methodologies, and advanced applications147A Stable Solid Electrolyte Interphase for Magnesium Metal Anode Evolved from a Bulky Anion Lithium Salt187Manipulating the ion-transfer kinetics and interface stability for high-performance zinc metal anodes1297Fundamentals and perspectives in developing zinc-ion battery electrolytes: a comprehensive review918Understanding the nature of the passivation layer enabling reversible calcium plating155Vanadium‐Based Nanomaterials: A Promising Family for Emerging Metal‐Ion Batteries482Issues and Future Perspective on Zinc Metal Anode for Rechargeable Aqueous Zinc‐ion Batteries763Rechargeable Alkali-Ion Battery Materials: Theory and Computation264A Universal Approach to Aqueous Energy Storage via Ultralow‐Cost Electrolyte with Super‐Concentrated Sugar as Hydrogen‐Bond‐Regulated Solute176Opportunities and Challenges for Organic Electrodes in Electrochemical Energy Storage961Scientific Challenges for the Implementation of Zn-Ion Batteries2110Covalent–Organic Frameworks: Advanced Organic Electrode Materials for Rechargeable Batteries622Recent Advances in Rechargeable Magnesium‐Based Batteries for High‐Efficiency Energy Storage241Engineering of Polyanion Type Cathode Materials for Sodium‐Ion Batteries: Toward Higher Energy/Power Density260Charge storage mechanism of MOF-derived Mn2O3 as high performance cathode of aqueous zinc-ion batteries186Tuning the Kinetics of Zinc‐Ion Insertion/Extraction in V 2 O 5 by In Situ Polyaniline Intercalation Enables Improved Aqueous Zinc‐Ion Storage Performance559Zinc–Organic Battery with a Wide Operation‐Temperature Window from −70 to 150 °C258Energy storage emerging: A perspective from the Joint Center for Energy Storage Research344Electroactive Covalent Organic Frameworks: Design, Synthesis, and Applications217Current status and future directions of multivalent metal-ion batteries1519Strategies to Enable Reversible Magnesium Electrochemistry: From Electrolytes to Artificial Solid–Electrolyte Interphases154Ion-Solvent Chemistry-Inspired Cation-Additive Strategy to Stabilize Electrolytes for Sodium-Metal Batteries202Ultrathin VSe2 Nanosheets with Fast Ion Diffusion and Robust Structural Stability for Rechargeable Zinc‐Ion Battery Cathode256Architecting a Stable High-Energy Aqueous Al-Ion Battery360Challenges and Opportunities for Multivalent Metal Anodes in Rechargeable Batteries149Operando pH Measurements Decipher H + /Zn 2+ Intercalation Chemistry in High-Performance Aqueous Zn/δ-V 2 O 5 Batteries241Engineering stable Zn-MnO2 batteries by synergistic stabilization between the carbon nanofiber core and birnessite-MnO2 nanosheets shell139High-power Mg batteries enabled by heterogeneous enolization redox chemistry and weakly coordinating electrolytes374Promises and Challenges of Next-Generation “Beyond Li-ion” Batteries for Electric Vehicles and Grid Decarbonization1612A comprehensive review on the prospects of multi-functional carbon nano onions as an effective, high- performance energy storage material142Principles of interlayer-spacing regulation of layered vanadium phosphates for superior zinc-ion batteries254The metamorphosis of rechargeable magnesium batteries271The Renaissance of Proton Batteries162Electrolyte Strategies toward Better Zinc-Ion Batteries761An Energetic CuS–Cu Battery System Based on CuS Nanosheet Arrays158Guest-species-incorporation in manganese/vanadium-based oxides: Towards high performance aqueous zinc-ion batteries138Opportunities and challenges for aqueous metal-proton batteries138Tetradiketone macrocycle for divalent aluminium ion batteries141Interlayer Modification of Pseudocapacitive Vanadium Oxide and Zn(H2O)n2+ Migration Regulation for Ultrahigh Rate and Durable Aqueous Zinc‐Ion Batteries192An Ultrahigh Performance Zinc‐Organic Battery using Poly(catechol) Cathode in Zn(TFSI)2‐Based Concentrated Aqueous Electrolytes180Recent Advances in Conversion-Type Electrode Materials for Post Lithium-Ion Batteries137Molecular Tailoring of an n/p‐type Phenothiazine Organic Scaffold for Zinc Batteries159Challenges and design strategies for high performance aqueous zinc ion batteries190Bilayered VOPO4⋅2H2O Nanosheets with High‐Concentration Oxygen Vacancies for High‐Performance Aqueous Zinc‐Ion Batteries166Solvation sheath reorganization enables divalent metal batteries with fast interfacial charge transfer kinetics604Current Design Strategies for Rechargeable Magnesium-Based Batteries208Ion migration and defect effect of electrode materials in multivalent-ion batteries161Electrolyte/electrode interfacial electrochemical behaviors and optimization strategies in aqueous zinc-ion batteries316Nonaqueous rechargeable aluminum batteries168Hydrogen Bond‐Functionalized Massive Solvation Modules Stabilizing Bilateral Interfaces181Simultaneous Incorporation of V and Mn Element into Polyanionic NASICON for High Energy‐Density and Long‐Lifespan Zn‐Ion Storage145Theory-guided experimental design in battery materials research156Atomic‐Scale Design of Anode Materials for Alkali Metal (Li/Na/K)‐Ion Batteries: Progress and Perspectives149Rechargeable Batteries for Grid Scale Energy Storage1765Recent progress in the design of advanced MXene/metal oxides-hybrid materials for energy storage devices158Alloying Strategy for High-Performance Zinc Metal Anodes201A practical perspective on the potential of rechargeable Mg batteries138Progress in 3D-MXene Electrodes for Lithium/Sodium/Potassium/Magnesium/Zinc/Aluminum-Ion Batteries283Zinc-ion batteries for stationary energy storage481On Energy Storage Chemistry of Aqueous Zn-Ion Batteries: From Cathode to Anode206The rise of high-entropy battery materials175Review of cathode materials for sodium-ion batteries180Roadmap for Next-Generation Electrochemical Energy Storage Technologies: Secondary Batteries and Supercapacitors149

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