Ultrafast Sintering of Dense LiLaZrO Membranes for Li Metal All-Solid-State Batteries.

Ultrafast sintering (UFS) is a compelling approach for fabricating LiLaZrO (LLZO) solid-state electrolytes (SSEs), paving the way for advancing and commercializing Li-garnet solid-state batteries. Although this method is commonly applied to the sintering of LLZO ceramics, its use for producing dense, phase-pure LLZO SSEs has thus far been primarily limited to millimeter-thick pellets, which are unsuitable for commercial solid-state batteries. This study presents ultrafast sintering as a highly effective approach for fabricating self-standing, dense, 45 µm-thick LLZO membranes.

On the interfacial phenomena at the LiLaZrO (LLZO)/Li interface.

Research on the LiLaZrO (LLZO)/Li interface is essential for improving the performance of LLZO-based solid-state batteries. In this comment, the authors present an analysis of the key interfacial phenomena at the LLZO/Li interface, highlighting recent developments and unresolved issues.

Building Solid-State Batteries: Insights from Swiss Research Labs.

This review article delves into the growing field of solid-state batteries as a compelling alternative to conventional lithium-ion batteries. The article surveys ongoing research efforts at renowned Swiss institutions such as ETH Zurich, Empa, Paul Scherrer Institute, and Berner Fachhochschule covering various aspects, from a fundamental understanding of battery interfaces to practical issues of solid-state battery fabrication, their design, and production. The article then outlines the prospects of solid-state batteries, emphasizing the imperative practical challenges that remain to be overcome and highlighting Swiss research groups' efforts and research directions in this field.

Garnet-Based Solid-State Li Batteries with High-Surface-Area Porous LLZO Membranes.

Rechargeable garnet-based solid-state Li batteries hold immense promise as nonflammable, nontoxic, and high energy density energy storage systems, employing LiLaZrO (LLZO) with a garnet-type structure as the solid-state electrolyte. Despite substantial progress in this field, the advancement and eventual commercialization of garnet-based solid-state Li batteries are impeded by void formation at the LLZO/Li interface at practical current densities and areal capacities beyond 1 mA cm and 1 mAh cm, respectively, resulting in limited cycling stability and the emergence of Li dendrites. Additionally, developing a fabrication approach for thin LLZO electrolytes to achieve high energy density remains paramount.

Nitrile-functionalized Poly(siloxane) as Electrolytes for High-Energy-Density Solid-State Li Batteries.

In the quest to replace liquid Li-ion electrolytes with safer and non-toxic solid counterparts for Li-ion batteries, polysiloxane polymers have attracted considerable attention as they offer low glass transition temperatures, stability with metallic lithium, and versatility in chemical functionalization of the backbone. Herein, we present the synthesis of Li-ion conductive polysiloxane-based polymers functionalized with 60 % nitrile groups per chain unit. The synthesis procedure is based on the reaction of poly-(dimethylsiloxane-co-methylvinylsiloxane) polymer with 2-cyanoethanethiol, followed by the addition of lithium bis (trifluoromethanesulfonyl) imide.

Standardizing critical current density measurements in lithium garnets.

The formation of Li dendrites at the Li/electrolyte interface at practically relevant current densities (> 1 mA cm) is a critical issue hindering the deployment of non-flammable and non-toxic LiLaZrO (LLZO) electrolyte in solid-state batteries. In this comment, the authors argue for an agreement to standardize measurements of the critical current density at which Li dendrites begin to penetrate the LLZO solid-state electrolyte.

Pyrochlore-Type Iron Hydroxy Fluorides as Low-Cost Lithium-Ion Cathode Materials for Stationary Energy Storage.

Pyrochlore-type iron (III) hydroxy fluorides (Pyr-IHF) are appealing low-cost stationary energy storage materials due to the virtually unlimited supply of their constituent elements, their high energy densities, and fast Li-ion diffusion. However, the prohibitively high costs of synthesis and cathode architecture currently prevent their commercial use in low-cost Li-ion batteries. Herein, a facile and cost-effective dissolution-precipitation synthesis of Pyr-IHF from soluble iron (III) fluoride precursors is presented.

Advances and challenges of aluminum-sulfur batteries.

The search for cost-effective stationary energy storage systems has led to a surge of reports on novel post-Li-ion batteries composed entirely of earth-abundant chemical elements. Among the plethora of contenders in the 'beyond lithium' domain, the aluminum-sulfur (Al-S) batteries have attracted considerable attention in recent years due to their low cost and high theoretical volumetric and gravimetric energy densities (3177 Wh L and 1392 Wh kg). In this work, we offer an overview of historical and present research pursuits in the development of Al-S batteries with particular emphasis on their fundamental problem-the dissolution of polysulfides.

Thermal synthesis of conversion-type bismuth fluoride cathodes for high-energy-density Li-ion batteries.

Towards enhancement of the energy density of Li-ion batteries, BiF has recently attracted considerable attention as a compelling conversion-type cathode material due to its high theoretical capacity of 302 mAh g, average discharge voltage of ca. 3.0 V vs.

Bilayer Dense-Porous Li La Zr O Membranes for High-Performance Li-Garnet Solid-State Batteries.

Li dendrites form in Li La Zr O (LLZO) solid electrolytes due to intrinsic volume changes of Li and the appearance of voids at the Li metal/LLZO interface. Bilayer dense-porous LLZO membranes make for a compelling solution of this pertinent challenge in the field of Li-garnet solid-state batteries (SSB). Lithium is thus stored in the pores of the LLZO, thereby avoiding i) dynamic changes of the anode volume and ii) the formation of voids during Li stripping due to increased surface area of the Li/LLZO interface.

Methodological Studies of the Mechanism of Anion Insertion in Nanometer-Sized Carbon Micropores.

Dual-ion hybrid capacitors (DIHCs) are a promising class of electrochemical energy storage devices intermediate between batteries and supercapacitors, exhibiting both high energy and power density, and generalizable across wide chemistries beyond lithium. In this study, a model carbon framework material with a periodic structure containing exclusively 1.2 nm width pores, zeolite-templated carbon (ZTC), was investigated as the positive electrode for the storage of a range of anions relevant to DIHC chemistries.

Perspective on design and technical challenges of Li-garnet solid-state batteries.

Solid-state Li-ion batteries based on Li-garnet LiLaZrO (LLZO) electrolyte have seen rapid advances in recent years. These solid-state systems are poised to address the urgent need for safe, non-flammable, and temperature-tolerant energy storage batteries that concomitantly possess improved energy densities and the cycle life as compared to conventional liquid-electrolyte-based counterparts. In this vision article, we review present research pursuits and discuss the limitations in the employment of LLZO solid-state electrolyte (SSE) for solid-state Li-ion batteries.

On the feasibility of all-solid-state batteries with LLZO as a single electrolyte.

Replacement of Li-ion liquid-state electrolytes by solid-state counterparts in a Li-ion battery (LIB) is a major research objective as well as an urgent priority for the industry, as it enables the use of a Li metal anode and provides new opportunities to realize safe, non-flammable, and temperature-resilient batteries. Among the plethora of solid-state electrolytes (SSEs) investigated, garnet-type Li-ion electrolytes based on cubic LiLaZrO (LLZO) are considered the most appealing candidates for the development of future solid-state batteries because of their low electronic conductivity of ca. 10 S cm (RT) and a wide electrochemical operation window of 0-6 V vs.

Monodisperse CoSb nanocrystals as high-performance anode material for Li-ion batteries.

Towards enhancement of the power density of Li-ion batteries (LIBs), antimony-based intermetallic compounds have recently attracted considerable attention as compelling anode materials owing to their high rate capability as compared to state-of-the-art graphite anodes. Here we report a facile colloidal synthesis of monodisperse CoSb nanocrystals (NCs) as a model intermetallic anode material for LIBs via the reaction between Co NCs and SbCl in oleylamine under reducing conditions. We found that ca.

Aluminum electrolytes for Al dual-ion batteries.

In the search for sustainable energy storage systems, aluminum dual-ion batteries have recently attracted considerable attention due to their low cost, safety, high energy density (up to 70 kWh kg), energy efficiency (80-90%) and long cycling life (thousands of cycles and potentially more), which are needed attributes for grid-level stationary energy storage. Overall, such batteries are composed of aluminum foil as the anode and various types of carbonaceous and organic substances as the cathode, which are immersed in an aluminum electrolyte that supports efficient and dendrite-free aluminum electroplating/stripping upon cycling. Here, we review current research pursuits and present the limitations of aluminum electrolytes for aluminum dual-ion batteries.

Silicon oxycarbide-antimony nanocomposites for high-performance Li-ion battery anodes.

Silicon oxycarbide (SiOC) has recently regained attention in the field of Li-ion batteries, owing to its effectiveness as a host matrix for nanoscale anode materials alloying with Li. The SiOC matrix, itself providing a high Li-ion storage capacity of 600 mA h g-1, assists in buffering volumetric changes upon lithiation and largely suppresses the formation of an unstable solid-electrolyte interface. Herein, we present the synthesis of homogeneously embedded Sb nanoparticles in a SiOC matrix with the size of 5-40 nm via the pyrolysis of a preceramic polymer.

Colloidal Antimony Sulfide Nanoparticles as a High-Performance Anode Material for Li-ion and Na-ion Batteries.

To maximize the anodic charge storage capacity of Li-ion and Na-ion batteries (LIBs and SIBs, respectively), the conversion-alloying-type SbS anode has attracted considerable interest because of its merits of a high theoretical capacity of 946 mAh g and a suitable anodic lithiation/delithiation voltage window of 0.1-2 V vs. Li/Li.

Silicon Oxycarbide-Tin Nanocomposite as a High-Power-Density Anode for Li-Ion Batteries.

Tin-based materials are an emerging class of Li-ion anodes with considerable potential for use in high-energy-density Li-ion batteries. However, the long-lasting electrochemical performance of Sn remains a formidable challenge due to the large volume changes occurring upon its lithiation. The prevailing approaches toward stabilization of such electrodes involve embedding Sn in the form of nanoparticles (NPs) in an active/inactive matrix.

Zeolite-Templated Carbon as a Stable, High Power Magnesium-Ion Cathode Material.

One strategy to overcome the slow kinetics associated with electrochemical magnesium ion storage is to employ a permanently porous, capacitive cathode material together with magnesium metal as the anode. This strategy has begun to be employed, for example, using framework solids like Prussian blue analogues or porous carbons derived from metal-organic frameworks, but the cycling stability of an ordered, bottom-up synthesized, three-dimensional carbon framework toward magnesiation and demagnesiation in a shuttle-type battery remains unexplored. Zeolite-templated carbons (ZTCs) are a class of ordered porous carbonaceous framework materials with numerous superlative properties relevant to electrochemical energy storage.

Copper sulfide nanoparticles as high-performance cathode materials for Mg-ion batteries.

Rechargeable magnesium batteries are appealing as safe, low-cost systems with high-energy-density storage that employ predominantly dendrite-free magnesium metal as the anode. While significant progress has been achieved with magnesium electrolytes in recent years, the further development of Mg-ion batteries, however, is inherently limited by the lack of suitable cathode materials, mainly due to the slow diffusion of high-charge-density Mg-ions in the intercalation-type host structures and kinetic limitations of conversion-type cathodes that often causes poor cyclic stability. Nanostructuring the cathode materials offers an effective means of mitigating these challenges, due to the reduced diffusion length and higher surface areas.

Transition metal trifluoroacetates (M = Fe, Co, Mn) as precursors for uniform colloidal metal difluoride and phosphide nanoparticles.

We report a simple one-pot synthesis of uniform transition metal difluoride MF (M = Fe, Mn, Co) nanorods based on transition metal trifluoroacetates (TMTFAs) as single-source precursors. The synthesis of metal fluorides is based on the thermolysis of TMTFAs at 250-320 °C in trioctylphosphine/trioctylphosphine oxide solvent mixtures. The FeF nanorods were converted into FeF nanorods by reaction with gaseous fluorine.

Zeolite-Templated Carbon as the Cathode for a High Energy Density Dual-Ion Battery.

Dual-ion batteries (DIBs) are electrochemical energy storage devices that operate by the simultaneous participation of two different ion species at the anode and cathode and rely on the use of an electrolyte that can withstand the high operation potential of the cathode. Under such conditions at the cathode, issues associated with the irreversible capacity loss and the formation of solid-electrolyte interphase at the surface of highly porous electrode materials are far less significant than at lower potentials, permitting the exploration of high surface area, permanently porous framework materials as effective charge storage media. This concept is investigated herein by employing zeolite-templated carbon (ZTC) as a cathode in a dual-ion battery based on a potassium bis(fluorosulfonyl)imide (KFSI) electrolyte.

High-energy-density dual-ion battery for stationary storage of electricity using concentrated potassium fluorosulfonylimide.

Graphite dual-ion batteries represent a potential battery concept for large-scale stationary storage of electricity, especially when constructed free of lithium and other chemical elements with limited natural reserves. Owing to their non-rocking-chair operation mechanism, however, the practical deployment of graphite dual-ion batteries is inherently limited by the need for large quantities of electrolyte solutions as reservoirs of all ions that are needed for complete charge and discharge of the electrodes. Thus far, lithium-free graphite dual-ion batteries have employed moderately concentrated electrolyte solutions (0.

Colloidal Bismuth Nanocrystals as a Model Anode Material for Rechargeable Mg-Ion Batteries: Atomistic and Mesoscale Insights.

At present, the technical progress of secondary batteries employing metallic magnesium as the anode material has been severely hindered due to the low oxidation stability of state-of-the-art Mg electrolytes, which cannot be used to explore high-voltage (>3 V versus Mg/Mg) cathode materials. All known electrolytes based on oxidatively stable solvents and salts, such as Mg(ClO) and Mg bis(trifluoromethanesulfonimide), react with the metallic magnesium anode, forming a passivating layer at its surface and preventing the reversible plating and stripping of Mg. Therefore, in a near-term effort to extend the upper voltage limit in the exploration of future candidate Mg-ion battery cathode materials, bismuth anodes have attracted considerable attention due to their efficient magnesiation and demagnesiation alloying reaction in such electrolytes.