Dual-Seed Strategy for High-Performance Anode-Less All-Solid-State Batteries.

Interest in all-solid-state batteries (ASSBs), particularly the anode-less type, has grown alongside the expansion of the electric vehicle (EV) market, because they offer advantages in terms of their energy density and manufacturing cost. However, in most anode-less ASSBs, the anode is covered by a protective layer to ensure stable lithium (Li) deposition, thus requiring high temperatures to ensure adequate Li ion diffusion kinetics through the protective layer. This study proposes a dual-seed protective layer consisting of silver (Ag) and zinc oxide (ZnO) nanoparticles for sulfide-based anode-less ASSBs.

Insights from Li and Zn systems for advancing Mg and Ca metal batteries.

The inherent limitations of lithium (Li)-ion batteries have sparked interest in exploring alternative technologies, especially those relying on metallic anodes: monovalent Li and divalent zinc (Zn), magnesium (Mg), and calcium (Ca) metals. In particular, Mg and Ca metal batteries offer significant advantages based on the natural abundance of their raw materials and high energy-storage capabilities resulting from the bivalency of the carrier ions. Yet, these battery systems are far from commercialization, and the lack of reliable electrolytes constitutes a primary concern.

Interfacial Stabilization by Prelithiated Trithiocyanuric Acid as an Organic Additive in Sulfide-Based All-Solid-State Lithium Metal Batteries.

Sulfide-based all-solid-state battery (ASSB) with a lithium metal anode (LMA) is a promising candidate to surpass conventional Li-ion batteries owing to their inherent safety against fire hazards and potential to achieve a higher energy density. However, the narrow electrochemical stability window and chemical reactivity of the sulfide solid electrolyte towards the LMA results in interfacial degradation and poor electrochemical performance. In this direction, we introduce an organic additive approach, that is the mixing of prelithiated trithiocyanuric acid, LiTCA, with LiPSCl, to establish a stable interface while preserving high ionic conductivity.

Non-Electroconductive Polymer Coating on Graphite Mitigating Electrochemical Degradation of PTFE for a Dry-Processed Lithium-Ion Battery Anode.

Polytetrafluoroethylene (PTFE)-based dry process for lithium-ion batteries is gaining attention as a battery manufacturing scheme can be simplified with drastically reducing environmental damage. However, the electrochemical instability of PTFE in a reducing environment has hampered the realization of the high-performance dry-processed anode. In this study, we present a non-electroconductive and highly ionic-conductive polymer coating on graphite to mitigate the electrochemical degradation of the PTFE binder and minimize the coating resistance.

Toward Practical Multivalent Ion Batteries with Quinone-Based Organic Cathodes.

Multivalent ion batteries have emerged as promising solutions to meet the future demands of energy storage applications, offering not only high energy density but also diverse socio-economic advantages. Among the various options for cathodes, quinone-based organic compounds have gained attention as suitable active materials for multivalent ion batteries due to their well-aligned ion channels, flexible structures, and competitive electrochemical performance. However, the charge carriers associated with anions that are often exploited in multivalent ion battery systems operate by way of a "non-rocking-chair" mechanism, which requires the use of an excess amount of electrolyte and results in a significant decrease in the energy density.

Carrageenan as a Sacrificial Binder for 5 V LiNi Mn O Cathodes in Lithium-Ion Batteries.

5 V-class LiNi Mn O (LNMO) with its spinel symmetry is a promising cathode material for lithium-ion batteries. However, the high-voltage operation of LNMO renders it vulnerable to interfacial degradation involving electrolyte decomposition, which hinders long-term and high-rate cycling. Herein, this longstanding challenge presented by LNMO is overcome by incorporating a sacrificial binder, namely, λ-carrageenan (CRN), a sulfated polysaccharide.

Rationally Designed Solution-Processible Conductive Carbon Additive Coating for Sulfide-based All-Solid-State Batteries.

Sulfide-based all-solid-state batteries (ASSBs) have emerged as promising candidates for next-generation energy storage systems owing to their superior safety and energy density. A conductive agent is necessarily added in the cathode composite of ASSBs to facilitate electron transport therein, but it causes the decomposition of the solid electrolyte and ultimately the shortening of lifetime. To resolve this dilemmatic situation, herein, we report a rationally designed solution-processible coating of zinc oxide (ZnO) onto vapor-grown carbon fiber as a conductive agent to reduce the contact between the carbon additive and the solid electrolyte and still maintain electron pathways to the active material.

Surface Overpotential as a Key Metric for the Discharge-Charge Reversibility of Aqueous Zinc-Ion Batteries.

Aqueous zinc-ion batteries (AZIBs) are receiving increasing attention for power-grid energy storage systems. Nevertheless, warranting long-term reversible operation is not trivial owing to uncontrolled interfacial phenomena related to zinc dendritic growth and parasitic reactions. Herein, the addition of hexamethylphosphoramide (HMPA) to the electrolyte revealed the surface overpotential (|η|) to be a key metric of the reversibility.

Naked metallic skin for homo-epitaxial deposition in lithium metal batteries.

Regulating the morphology of lithium plating is the key to extending the cycle life of lithium metal batteries. Fatal dendritic growth is closely related to out-of-plane nucleation on the lithium metal surface. Herein, we report a nearly perfect lattice match between the lithium metal foil and lithium deposits by removing the native oxide layer using simple bromine-based acid-base chemistry.

Entropymetry for detecting microcracks in high-nickel layered oxide cathodes.

Electric vehicles (EVs) are imposing ever-challenging standards on the lifetime and safety of lithium-ion batteries (LIBs); consequently, real-time nondestructive monitoring of battery cell degradation is highly desired. Unfortunately, high-nickel (Ni) layered oxides, the preferred LIB cathodes for EVs, undergo performance degradation originating from microcrack formation during cycling. Entropymetry is introduced as a real-time analytic tool for monitoring the evolution of microcracks in these cathodes along the state of charge.

Hierarchically Porous Ferroelectric Layer with the Aligned Dipole Moment for a High-Performance Aqueous Zn Metal Battery.

Rechargeable aqueous Zn metal batteries (AZMBs) are desirable because of the advantages of metallic Zn and aqueous media. However, AZMBs suffer from limited cyclability and low Coulombic efficiency, originating from uncontrolled dendrite growth and side reactions such as hydrogen gas evolution and corrosion. A hierarchically porous poly(vinylidene difluoride) (PVDF) protection layer with ferroelectric β-phases is formed on the Zn metal using a simple electrospinning method.

Cationic Additive with a Rigid Solvation Shell for High-Performance Zinc Ion Batteries.

Despite substantial progresses, in aqueous zinc ion batteries (AZIBs), developing zinc metal anodes with long-term reliable cycling capabilities is nontrivial because of dendritic growth and related parasitic reactions on the zinc surface. Here, we exploit the tip-blocking effect of a scandium (Sc ) additive in the electrolyte to induce uniform zinc deposition. Additional to the tri-valency of Sc , the rigidity of its hydration shell effectively prevents zinc ions from concentrating at the surface tips, enabling highly stable cycling under challenging conditions.

Lithium-Metal Batteries: From Fundamental Research to Industrialization.

Lithium-metal batteries (LMBs) are representative of post-lithium-ion batteries with the great promise of increasing the energy density drastically by utilizing the low operating voltage and high specific capacity of metallic lithium. LMBs currently stand at a point of transition at which the accumulation of knowledge from fundamental research is being translated into large-scale commercialization. This review summarizes the available strategies for addressing the intrinsic shortcomings of LMBs, such as the suppression of dendritic growth and parasitic reactions from the material to the electrode to the cell level.

Room-Temperature Anode-Less All-Solid-State Batteries via the Conversion Reaction of Metal Fluorides.

All-solid-state batteries (ASSBs) that employ anode-less electrodes have drawn attention from across the battery community because they offer competitive energy densities and a markedly improved cycle life. Nevertheless, the composite matrices of anode-less electrodes impose a substantial barrier for lithium-ion diffusion and inhibit operation at room temperature. To overcome this drawback, here, the conversion reaction of metal fluorides is exploited because metallic nanodomains formed during this reaction induce an alloying reaction with lithium ions for uniform and sustainable lithium (de)plating.

Fluorinated ether electrolyte with controlled solvation structure for high voltage lithium metal batteries.

The development of new solvents is imperative in lithium metal batteries due to the incompatibility of conventional carbonate and narrow electrochemical windows of ether-based electrolytes. Whereas the fluorinated ethers showed improved electrochemical stabilities, they can hardly solvate lithium ions. Thus, the challenge in electrolyte chemistry is to combine the high voltage stability of fluorinated ethers with high lithium ion solvation ability of ethers in a single molecule.

Corrosion as the origin of limited lifetime of vanadium oxide-based aqueous zinc ion batteries.

Aqueous zinc ion batteries are receiving increasing attention for large-scale energy storage systems owing to their attractive features with respect to safety, cost, and scalability. Although vanadium oxides with various compositions have been demonstrated to store zinc ions reversibly, their limited cyclability especially at low current densities and their poor calendar life impede their widespread practical adoption. Herein, we reveal that the electrochemically inactive zinc pyrovanadate (ZVO) phase formed on the cathode surface is the main cause of the limited sustainability.

Integrated Ring-Chain Design of a New Fluorinated Ether Solvent for High-Voltage Lithium-Metal Batteries.

Ether-based electrolytes offer promising features such as high lithium-ion solvation power and stable interface, yet their limited oxidation stability impedes application in high-voltage Li-metal batteries (LMBs). Whereas the fluorination of the ether backbone improves the oxidative stability, the resulting solvents lose their Li -solvation ability. Therefore, the rational molecular design of solvents is essential to combine high redox stability with good ionic conductivity.

Icephobic Coating through a Self-Formed Superhydrophobic Surface Using a Polymer and Microsized Particles.

Icephobic coatings have been extensively studied for decades to overcome the potential damage associated with ice formation in various devices that are operated under harsh weather conditions. Superhydrophobic surface coatings have been applied for icephobic coating applications owing to their low surface energy. In this study, an icephobic coating of a self-formed superhydrophobic surface using polydimethylsiloxane (PDMS) and SiO powder was investigated.

Photochemically driven solid electrolyte interphase for extremely fast-charging lithium-ion batteries.

Extremely fast charging (i.e. 80% of storage capacity within 15 min) is a pressing requirement for current lithium-ion battery technology and also affects the planning of charging infrastructure.

Lithium-Conducting Self-Assembled Organic Nanotubes.

Supramolecular polymers are compelling platforms for the design of stimuli-responsive materials with emergent functions. Here, we report the assembly of an amphiphilic nanotube for Li-ion conduction that exhibits high ionic conductivity, mechanical integrity, electrochemical stability, and solution processability. Imine condensation of a pyridine-containing diamine with a triethylene glycol functionalized isophthalaldehyde yields pore-functionalized macrocycles.

Issues and Advances in Scaling up Sulfide-Based All-Solid-State Batteries.

ConspectusAll-solid-state batteries (ASSBs) are considered to be a next-generation energy storage concept that offers enhanced safety and potentially high energy density. The identification of solid electrolytes (SEs) with high ionic conductivity was the stepping-stone that enabled the recent surge in activity in this research area. Among the various types of SEs, including those based on oxides, sulfides, polymers, and hybrids thereof, sulfide-based SEs have gained discernible attention owing to their exceptional room temperature ionic conductivity comparable even to those of their liquid electrolyte counterparts.

Ionic Liquid Functionalized Gel Polymer Electrolytes for Stable Lithium Metal Batteries.

Metallic lithium (Li) is regarded as the ideal anode material in lithium-ion batteries due to its low electrochemical potential, highest theoretical energy density and low density. There are, however, still significant challenges to be addressed such as Li-dendrite growth and low interfacial stability, which impede the practical application of Li metal anodes. In order to circumvent these shortcomings, herein, we present a gel polymer electrolyte containing imidazolium ionic liquid end groups with a perfluorinated alkyl chain (F-IL) to achieve both high ionic conductivity and Li ion transference number by fundamentally altering the solubility of salt within the gel electrolyte through Lewis-acidic segments in the polymer backbone.

Atomic-scale unveiling of multiphase evolution during hydrated Zn-ion insertion in vanadium oxide.

An initial crystalline phase can transform into another phases as cations are electrochemically inserted into its lattice. Precise identification of phase evolution at an atomic level during transformation is thus the very first step to comprehensively understand the cation insertion behavior and subsequently achieve much higher storage capacity in rechargeable cells, although it is sometimes challenging. By intensively using atomic-column-resolved scanning transmission electron microscopy, we directly visualize the simultaneous intercalation of both HO and Zn during discharge of Zn ions into a VO cathode with an aqueous electrolyte.

Zn-Imidazole Coordination Crosslinks for Elastic Polymeric Binders in High-Capacity Silicon Electrodes.

Recent research has built a consensus that the binder plays a key role in the performance of high-capacity silicon anodes in lithium-ion batteries. These anodes necessitate the use of a binder to maintain the electrode integrity during the immense volume change of silicon during cycling. Here, Zn-imidazole coordination crosslinks that are formed to carboxymethyl cellulose backbones in situ during electrode fabrication are reported.