Charge and discharge of lithium ion battery electrodes is accompanied by severe volume changes. In a confined space, the cannot expand, leading to significant pressures induced local microstructural changes within battery. While appear be less critical in batteries with liquid electrolytes, they will more case solid electrolytes even detrimental all-solid-state metal electrode. this work we first summarize, compare, analyze occurring state art electrode materials, based on crystallographic...

In the near future, targets for lithium-ion batteries concerning specific energy and cost can advantageously be met by introducing layered LiNixCoyMnzO2 (NCM) cathode materials with a high Ni content (x ≥ 0.6). Increasing allows utilization of more lithium at given cell voltage, thereby improving capacity but expense cycle life. Here, capacity-fading mechanisms both typical low-Ni NCM = 0.33, NCM111) high-Ni 0.8, NCM811) cathodes are investigated compared from crystallographic...

Two major strategies are currently pursued to improve the energy density of lithium-ion batteries using LiNixCoyMnzO2 (NCM) cathode materials. One is increase fraction redox active Ni (≥80%), which allows larger amounts Li be extracted at a given cutoff voltage (Umax). The other Umax, in particular for medium-Ni content NCM However, accompanying lattice changes ultimately lead capacity fading both cases. Here structural occurring Li1.02NixCoyMnzO2 (with x = 1/3, 0.5, 0.6, 0.7, 0.8 and 0.85)...

Ni-rich LiNixCoyMnzO2 (NCM) cathode materials have great potential for application in next-generation lithium-ion batteries owing to their high specific capacity. However, they are subjected severe structural changes upon (de)lithiation, which adversely affects the cycling stability. Herein, we investigate crystal and electronic structure of NCM811 (80% Ni) at states charge by a combination operando X-ray diffraction (XRD), hard absorption spectroscopy (hXAS), ex situ soft (sXAS), density...

The research and development of advanced nanocoatings for high-capacity cathode materials is currently a hot topic in the field solid-state batteries (SSBs). Protective surface coatings prevent direct contact between material solid electrolyte, thereby inhibiting detrimental interfacial decomposition reactions. This particularly important when using lithium thiophosphate superionic electrolytes, as these exhibit narrow electrochemical stability window, therefore, are prone to degradation...

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...

Abstract The operation of combined mass spectrometry and electrochemistry setups has recently become a powerful approach for the in situ analysis gas evolution batteries. It allows real-time insights mechanistic understanding into different processes, including battery formation, operation, degradation, behavior under stress conditions. Important information is gained on safety stability window as well effect protecting strategies, such surface coatings, dopings, electrolyte additives. This...

Lithiated oxides like Li[Ni x Co y Mn z ]O 2 ( + = 1) with high nickel content ≥ 0.8) can possess specific capacity ≥200 mA h g −1 and have attracted extensive attention as perspective cathode materials for advanced lithium-ion batteries.

Abstract As global energy storage demand increases, sodium‐ion batteries are often considered as an alternative to lithium‐ion batteries. Hexacyanoferrate cathodes, commonly referred Prussian blue analogues (PBAs), of particular interest due their low‐cost synthesis and promising electrochemical response. However, because they consist ~50 wt% cyanide anions, a possible release highly toxic gases poses significant safety risk. Previously, we observed the evolution (CN) 2 during cycling via...

Functional surface coatings were applied on high voltage spinel (LiNi0.5Mn1.5O4; LNMO) and Ni-rich (LiNi0.85Co0.1Mn0.05O2; NCM851005) NCM cathode materials using few-layered 2H tungsten diselenide (WSe2). Simple liquid-phase mixing with WSe2 in 2-propanol low-temperature (130 °C) heat treatment nitrogen flow dramatically improved electrochemical performance, including stable cycling, high-rate lower hysteresis Li coin cells at 30 55 °C. Significantly capacity retention °C [Q401/Q9 of 99% vs...

Layered Ni-rich oxide cathode materials are being explored in an effort to boost the energy density of lithium-ion batteries, especially for automotive applications. Among them, ternary-phase LiNiO2 (LNO) is a promising candidate but brings along various issues, such as poor structural stability. The material prone disordering (Li off-stoichiometry) when prepared by conventional solid-state synthesis, leading presence Ni2+ Li layer. These point defects negatively affect utilization...

Abstract Sodium-ion batteries (SIBs) see intensive research and commercialization efforts, aiming to establish them as an alternative lithium-ion batteries. Among the reported cathode material families for SIBs, Na-deficient P2-type layered oxides are promising candidates, benefiting from fast sodium diffusion therefore high charge/discharge rates. However, upon extraction at potentials, a transition P2 O2 phase occurs, with corresponding change in cell volume resulting particle fracture...

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...

Abstract O3-type layered oxide cathodes, such as NaNi0.5Mn0.5O2, have garnered significant attention due to their high theoretical specific capacity while using abundant and low-cost sodium intercalation species. Unlike the lithium analog (LiNiO2), NaNiO2 (NNO) exhibits poor electrochemical performance resulting from structural instability inferior Coulomb efficiency. To enhance its cyclability for practical application, NNO was modified by titanium substitution yield NaNi0.9Ti0.1O2 (NNTO),...

Currently, cathode manufacturing for lithium-ion batteries requires N-methyl-2-pyrrolidone (NMP) as a coating solvent. With concerns over its petrochemical origins and increasing scrutiny due to undesirable toxicological profile, there is market demand application-specific, less-regulated alternatives. Here, we evaluate γ-valerolactone (GVL), promising green-candidate based on closeness NMP in the Hansen Solubility Space. It has successfully dissolved polyvinylidene fluoride (PVDF) at...

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.

Bulk-type solid-state batteries (SSBs) composed of lithium thiophosphate superionic solid electrolytes (SEs) and high-capacity cathode active materials (CAMs) have recently attracted much attention for their potential application in next-generation electrochemical energy storage. However, compatibility issues between the key components this kind battery system are difficult to overcome. Here, we report on a protective coating that strongly reduces prevalence detrimental side reactions CAM SE...

Solid-state batteries (SSBs) are a promising next-generation energy-storage solution to complement or replace current battery technologies in the wave of automotive electrification. Especially SSBs using sulfide solid electrolytes (SEs) hold great potential; however, (electro)chemical instability when contact with layered oxide cathode active materials (CAMs) remains an obstacle further implementation. SE degradation occurring during cycling adversely affects ion/electron transport and may...

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...

Solid-state batteries (SSBs) utilizing superionic thiophosphate solid electrolytes (SEs), such as argyrodite Li6PS5Cl, are attracting great interest a potential solution for safe, high-energy-density electrochemical energy storage. However, the development of high-capacity cathodes remains major challenge. Herein, we present an effective design strategy to improve cyclability layered Co-free oxide cathode active material (CAM) LiNiO2, consisting surface modification and electrode...

Abstract Invited for this month's cover picture is the group of Torsten Brezesinski at KIT. The shows gases evolving from a Prussian white cathode used in Na‐ion batteries presence either NaPF 6 ‐ or NaClO 4 ‐containing electrolyte. H 2 and CO are detected, as well (CN) , which formation mechanism proposed. Read full text Research Article 10.1002/batt.202300595 .