The implementation of all-solid-state batteries (ASSBs) is regarded as an important step toward next-generation energy storage systems, in particular for electric vehicles and portable electronics. This may be achieved through application layered Ni-rich oxide cathode materials such Li1+x(Ni1–y–zCoyMnz)1–xO2 (NCM) with high specific capacity thiophosphate-based solid electrolytes. Here, the profound effect that secondary particle size active material has on ASSB cells comprising NCM622 (60%...

Bulk-type all-solid-state batteries (SSBs) are receiving much attention as next-generation energy storage technology with potentially improved safety and higher power densities (over a wider operating temperature range) compared to conventional Li-ion (LIBs). However, practical implementation of SSBs faces number hurdles, such issues related interfacial stability between the solid electrolyte (SE) other active inactive electrode constituents. One approach effectively prevent or mitigate side...

Large-scale industrial application of all-solid-state-batteries (ASSBs) is currently hindered by numerous problems. Regarding thiophosphate-based ASSBs, interfacial reactions with the solid electrolyte are considered a major reason for capacity fading. On positive electrode side, cathode active material coating addresses these issues and improves ASSB performance. Yet, working principle often remains unclear, protection concepts on way to long-term stable ASSBs remain empirical. In this...

Abstract Solid‐state batteries (SSBs) currently attract great attention as a potentially safe electrochemical high‐energy storage concept. However, several issues still prevent SSBs from outperforming today's lithium‐ion based on liquid electrolytes. One major challenge is related to the design of cathode active materials (CAMs) that are compatible with superionic solid electrolytes (SEs) interest. This perspective, gives brief overview required properties and possible challenges for...

Superionic solid electrolytes (SEs) are essential for bulk-type solid-state battery (SSB) applications. Multicomponent SEs recently attracting attention their favorable charge-transport properties, however a thorough understanding of how configurational entropy (ΔSconf ) affects ionic conductivity is lacking. Here, we successfully synthesized series halogen-rich lithium argyrodites with the general formula Li5.5 PS4.5 Clx Br1.5-x (0≤x≤1.5). Using neutron powder diffraction and 31 P...

The formation of gaseous side products in liquid electrolyte-based lithium-ion batteries has been intensively studied recent years and identified as being one the sources degradation (an indication electrolyte electrode instabilities). Herein, we demonstrate, to our knowledge for first time, that gassing can also arise all-solid-state battery cells made Ni-rich layered oxide cathode materials thiophosphate-based solid electrolytes. Combining isotopic labeling, titration quantitative...

All-inorganic solid-state batteries (SSBs) currently attract much attention as next-generation high-density energy-storage technology. However, to make SSBs competitive with conventional Li-ion batteries, several obstacles and challenges must be overcome, many of which are related interface stability issues. Protective coatings can applied the electrode materials mitigate side reactions solid electrolyte, lithium transition metal oxides, such LiNbO3 or Li2ZrO3, being well established in...

Solution-based trimethylaluminum treatment of NCM811 cathode material leads to drying and coating in a single step therefore improved cycling performance.

Gas evolution in conventional lithium-ion batteries using Ni-rich layered oxide cathode materials presents a serious issue that is responsible for performance decay and safety concerns, among others. Recent findings revealed gas also occurred bulk-type solid-state batteries. To further clarify the effect electrolyte has on gassing, we report this work-to best of our knowledge-the first study comparing with NCM622 material different types, specifically solid (β-Li3PS4 Li6PS5Cl) versus liquid...

Measures to improve the cycling performance and stability of bulk-type all-solid-state batteries (SSBs) are currently being developed with goal substituting conventional lithium-ion battery (LIB) technology. As known from liquid electrolyte-based LIBs, layered oxide cathode materials undergo volume changes upon (de)lithiation, causing mechanical degradation because particle fracture, among others. Unlike solid electrolytes, electrolytes somewhat capable accommodating morphological changes....

Bulk-type solid-state batteries (SSBs) constitute a promising next-generation technology for electrochemical energy storage. However, in order SSBs to become competitive with mature battery technologies, (electro)chemically stable, superionic solid electrolytes are much needed. Multicomponent or high-entropy lithium argyrodites have recently attracted attention their favorable material characteristics. In the present work, we report on increasing configurational entropy of Li6+aP1–xMxS5I...

High-entropy ceramics are attracting large interest because of their unique materials properties. Nevertheless, the effect entropy on lithium transport remains largely elusive. Here, we report, for first time, about medium- and high-entropy polyanionic superionic conductors crystallizing in F–43m space group adopting so-called argyrodite structure. The Li6PS5[Cl0.33Br0.33I0.33], Li6P[S2.5Se2.5][Cl0.33Br0.33I0.33], Li6.5[Ge0.5P0.5][S2.5Se2.5][Cl0.33Br0.33I0.33] were structurally characterized...

All-solid-state batteries (SSBs) are attracting widespread attention as next-generation energy storage devices, potentially offering increased power and densities better safety than liquid electrolyte-based Li-ion batteries. Significant research efforts currently underway to develop stable high-performance bulk-type SSB cells by optimizing the cathode microstructure composition, among others. Electronically conductive additives in positive electrode may have a or negative impact on...

Abstract Solid-state batteries (SSBs) are a promising next step in electrochemical energy storage but plagued by number of problems. In this study, we demonstrate the recurring issue mechanical degradation because volume changes layered Ni-rich oxide cathode materials thiophosphate-based SSBs. Specifically, explore superionic solid electrolytes (SEs) different crystallinity, namely glassy 1.5Li 2 S-0.5P S 5 -LiI and argyrodite Li 6 PS Cl, with emphasis on how they affect cyclability...

Lithium‐ion batteries (LIBs), which utilize a liquid electrolyte, have established prominence among energy storage devices by offering unparalleled and power densities coupled with reliable electrochemical behavior. The development of solid‐state (SSBs), utilizing solid electrolyte layer for ionic conduction between the electrodes, could potentially offer further performance improvements in key areas such as density safety. However, to date, SSBs remain unable match their counterparts. In...

Solid-state batteries (SSBs) have been touted as the next major milestone for electrochemical energy storage, improving safety and enabling higher densities. LiNiO2 (LNO) has long considered a promising cathode material; however, its commercial implementation is complicated by stability issues, including reactivity toward electrolyte components. To address this, detailed study probing behavior of LNO in pellet-stack SSB cells, combination with argyrodite Li6PS5Cl solid (SE) Li4Ti5O12 anode,...

This review article highlights the advantages of niobium as a dopant and coating constituent for improving cycling performance layered Ni-rich oxide cathodes in liquid- solid-electrolyte-based Li-ion batteries.

Abstract The development of improved solid electrolytes (SEs) plays a crucial role in the advancement bulk‐type solid‐state battery (SSB) technologies. In recent years, multicomponent or high‐entropy SEs are gaining increased attention for their advantageous charge‐transport and (electro)chemical properties. However, comprehensive understanding how configurational entropy affects ionic conductivity is largely lacking. Herein we investigate series multication‐substituted lithium argyrodites...

Laboratory research into bulk-type solid-state batteries (SSBs) has been focused predominantly on powder-based, pelletized cells and sufficient to evaluate fundamental limitations tailor the constituents some degree. However, improve experimental reliability for commercial implementation of this technology, competitive slurry-cast electrodes are required. Here, we report application an approach guided by design experiments (DoE) influence type/content polymer binder conductive carbon...

Abstract While still premature as an energy storage technology, bulk solid-state batteries are attracting much attention in the academic and industrial communities lately. In particular, layered lithium metal oxides thiophosphates hold promise cathode materials superionic solid electrolytes, respectively. However, interfacial side reactions between individual components during battery operation usually result accelerated performance degradation. Hence, effective surface coatings required to...

Abstract This short perspective summarizes recent findings on the role of residual lithium present surface layered Ni-rich oxide cathode materials in liquid- and solid-electrolyte based batteries, with emphasis placed carbonate species. Challenges future research opportunities development carbonate-containing protective nanocoatings for inorganic solid-state battery applications are also discussed.

Abstract Superionic conductors are key components of solid‐state batteries (SSBs). Multicomponent or high‐entropy materials, offering a vast compositional space for tailoring properties, have recently attracted attention as novel solid electrolytes (SEs). However, the influence synthetic parameters on ionic conductivity in compositionally complex SEs has not yet been investigated. Herein, effect cooling rate after high‐temperature annealing charge transport multicationic substituted lithium...

The global demand for high energy density batteries, mostly application in electric vehicles, offering increased durability, safety, and sustainability is growing rapidly. In the past, this has been met primarily by development and/or improvement of new/established battery materials technologies. high-entropy design concept—aiming at increasing chemical complexity/occupational disorder—has recently introduced into field electrochemical storage. Various that are seemingly capable...

<italic>Ex situ</italic> and <italic>operando</italic> X-ray diffraction allows determining the state-of-charge of all-solid-state batteries in an indirect manner.