A Li-Rich Fluorinated Lithium Zirconium Chloride Solid Electrolyte for 4.8 V-Class All-Solid-State Batteries.

Chloride solid-state electrolytes (SEs) represent an important advance for applications in all-solid-state batteries (ASSBs). Among various chloride SEs, lithium zirconium chloride (LiZrCl) is an attractive candidate considering the high natural abundance of Zr. However, LiZrCl meets the challenge in practical ASSBs because of its limited ionic conductivity and instability when paired with high-voltage cathodes.

Mechanochemically Enabled Metastable Niobium Tungsten Oxides.

Metastable compounds have greatly expanded the synthesizable compositions of solid-state materials and have attracted enormous amounts of attention in recent years. Especially, mechanochemically enabled metastable materials synthesis has been very successful in realizing cation-disordered materials with highly simple crystal structures, such as rock salts. Application of the same strategy for other structural types, especially for non-close-packed structures, is peculiarly underexplored.

Promoting high-voltage stability through local lattice distortion of halide solid electrolytes.

Stable solid electrolytes are essential to high-safety and high-energy-density lithium batteries, especially for applications with high-voltage cathodes. In such conditions, solid electrolytes may experience severe oxidation, decomposition, and deactivation during charging at high voltages, leading to inadequate cycling performance and even cell failure. Here, we address the high-voltage limitation of halide solid electrolytes by introducing local lattice distortion to confine the distribution of Cl, which effectively curbs kinetics of their oxidation.

Sustainable Anionic Redox by Inhibiting Li Cross-Layer Migration in Na-Based Layered Oxide Cathodes.

The irrational utilization of an anionic electron often accompanies structural degradation with an irreversible cation migration process upon cycling in sodium-layered oxide cathodes. Moreover, the insufficient understanding of the anionic redox involved cation migration makes the design strategies of high energy density electrodes even less effective. Herein, a P3-NaLiFeMnO (P3-NLFM) cathode is proposed with the in-plane disordered Li distribution after an in-depth remolding of the Li ribbon-ordered P3-NaLiMnO (P3-NLM) layered oxide.

NaCrZrCl: A New Halide-Based Fast Sodium-Ion Conductor.

All-solid-state batteries employing solid electrolytes (SEs) have received widespread attention due to their high safety. Recently, lithium halides are intensively investigated as promising SEs while their sodium counterparts are less studied. Herein, a new sodium-ion conductor with a chemical formula of NaCrZrC is reported, which exhibits high room temperature ionic conductivity of 0.

Novel Low-Strain Layered/Rocksalt Intergrown Cathode for High-Energy Li-Ion Batteries.

Both layered- and rocksalt-type Li-rich cathode materials are drawing great attention due to their enormous capacity, while the individual phases have their own drawbacks, such as great volume change for the layered phase and low electronic and ionic conductivities for the rocksalt phase. Previously, we have reported the layered/rocksalt intergrown cathodes with nearly zero-strain operation, while the use of precious elements hinders their industrial applications. Herein, low-cost 3d Mn ions are utilized to partially replace the expensive Ru ions, to develop novel ternary Li-rich cathode material Li[RuMnNi]O.

Enhancing Ionic Transport and Structural Stability of Lithium-Rich Layered Oxide Cathodes via Local Structure Regulation.

Lithium-rich manganese-based layered oxides (LRM) have garnered considerable attention as cathode materials due to their superior performance. However, the inherent structural degradation and obstruction of ion transport during cycling lead to capacity and voltage decay, impeding their practical applications. Herein, an Sb-doped LRM material with local spinel phase is reported, which has good compatibility with the layered structure and provides 3D Li diffusion channels to accelerate Li transport.

A New Zinc Salt Chemistry for Aqueous Zinc-Metal Batteries.

Aqueous zinc-ion batteries (ZIBs) are promising energy storage solutions with low cost and superior safety, but they suffer from chemical and electrochemical degradations closely related to the electrolyte. Here, a new zinc salt design and a drop-in solution for long cycle-life aqueous ZIBs are reported. The salt Zn(BBI) with a rationally designed anion group, N-(benzenesulfonyl)benzenesulfonamide (BBI ), has a special amphiphilic molecular structure, which combines the benefits of hydrophilic and hydrophobic groups to properly tune the solubility and interfacial condition.

Slight compositional variation-induced structural disorder-to-order transition enables fast Na storage in layered transition metal oxides.

The omnipresent Na/vacancy orderings change substantially with the composition that inevitably actuate the ionic diffusion in rechargeable batteries. Therefore, it may hold the key to the electrode design with high rate capability. Herein, the influence of Na/vacancy ordering on Na mobility is demonstrated firstly through a comparative investigation in P2-NaNiMnO and P2-NaNiMnO.

Lithiated Prussian blue analogues as positive electrode active materials for stable non-aqueous lithium-ion batteries.

Prussian blue analogues (PBAs) are appealing active materials for post-lithium electrochemical energy storage. However, PBAs are not generally suitable for non-aqueous Li-ion storage due to their instability upon prolonged cycling. Herein, we assess the feasibility of PBAs with various lithium content for non-aqueous Li-ion storage.

Solid-state rigid-rod polymer composite electrolytes with nanocrystalline lithium ion pathways.

A critical challenge for next-generation lithium-based batteries lies in development of electrolytes that enable thermal safety along with the use of high-energy-density electrodes. We describe molecular ionic composite electrolytes based on an aligned liquid crystalline polymer combined with ionic liquids and concentrated Li salt. This high strength (200 MPa) and non-flammable solid electrolyte possesses outstanding Li conductivity (1 mS cm at 25 °C) and electrochemical stability (5.

Layered-rocksalt intergrown cathode for high-capacity zero-strain battery operation.

The dependence on lithium-ion batteries leads to a pressing demand for advanced cathode materials. We demonstrate a new concept of layered-rocksalt intergrown structure that harnesses the combined figures of merit from each phase, including high capacity of layered and rocksalt phases, good kinetics of layered oxide and structural advantage of rocksalt. Based on this concept, lithium nickel ruthenium oxide of a main layered structure (R[Formula: see text]m) with intergrown rocksalt (Fm[Formula: see text]m) is developed, which delivers a high capacity with good rate performance.

Structural and Electrochemical Impacts of Mg/Mn Dual Dopants on the LiNiO Cathode in Li-Metal Batteries.

Doping chemistry has been regarded as an efficient strategy to overcome some fundamental challenges facing the "no-cobalt" LiNiO cathode materials. By utilizing the doping chemistry, we evaluate the battery performance and structural/chemical reversibility of a new no-cobalt cathode material (Mg/Mn-LiNiO). The unique dual dopants drive Mg and Mn to occupy the Li site and Ni site, respectively.

Distinct Surface and Bulk Thermal Behaviors of LiNiMnCoO Cathode Materials as a Function of State of Charge.

Understanding how structural and chemical transformations take place in particles under thermal conditions can inform designing thermally robust electrode materials. Such a study necessitates the use of diagnostic techniques that are capable of probing the transformations at multiple length scales and at different states of charge (SOC). In this study, the thermal behavior of LiNiMnCoO (NMC-622) was examined as a function of SOC, using an array of bulk and surface-sensitive techniques.

Electrical Properties of Hollandite-Type BaGaTiO, KGaTiO, and KMgTiO.

Electrical conductivity and electrochemical catalytic activity for H oxidation of Ti-based hollandite-type BaGaTiO (BGT), KGaTiO (KGT), and KMgTiO (KMT) were investigated, along with the chemical stability of KMT under H at elevated temperature. BGT, KGT, and KMT crystallized in a tetragonal structure with the space-group I4/ m. The electrical conductivity in H increases with increasing Ti content, and the highest total electrical conductivity of 2 S/cm at 800 °C in H was observed for KMT.

Inducing Favorable Cation Antisite by Doping Halogen in Ni-Rich Layered Cathode with Ultrahigh Stability.

The cation antisite is the most recognizable intrinsic defect type in nickel-rich layered and olivine-type cathode materials for lithium-ion batteries, and important for electrochemical/thermal performance. While how to generate the favorable antisite has not been put forward, herein, by combining first-principles calculation with neutron powder diffraction (NPD) study, a defect inducing the favorable antisite mechanism is proposed to improve cathode stability, that is, halogen substitution facilitates the neighboring Li and Ni atoms to exchange their sites, forming a more stable local octahedron of halide (LOSH). According to the mechanism, it is demonstrated by NPD that F-doping not only induces the antisite formation in layered LiNiCoMnO (LNCM), but also increases the antisite concentration linearly.

Delithiation/lithiation behaviors of three polymorphs of LiVOPO.

LiVOPO4 is an attractive high-voltage cathode with rich polymorphs (α, β and αI). We present here a comparison of the behaviors of three LiVOPO4 polymorphs during delithiation/lithiation. Experimental and computational work suggests that α-LiVOPO4 suffers from more severe conductivity problems among the three forms.

Alleviating oxygen evolution from Li-excess oxide materials through theory-guided surface protection.

Li-excess cathodes comprise one of the most promising avenues for increasing the energy density of current Li-ion technology. However, the first-cycle surface oxygen release in these materials causes cation densification and structural reconstruction of the surface region, leading to encumbered ionic transport and increased impedance. In this work, we use the first principles Density Functional Theory to systematically screen for optimal cation dopants to improve oxygen-retention at the surface.

Insights into B-Site Ordering in Double Perovskite-Type BaCaNbO (0 ≤ x ≤ 0.45): Combined Synchrotron and Neutron Diffraction and Electrical Transport Analyses.

Perovskite-type metal oxides are being used in a wide range of technologies, including fuel cells, batteries, electrolyzers, dielectric capacitors, and sensors. One of their remarkable structural properties is cationic ordering in A or B sites, which affects electrical transport properties under different gaseous atmospheres, and chemical stability under CO and humid conditions. For example, a simple-perovskite-type Y-doped BaCeO forms BaCO and ((Ce,Y)O) under CO at elevated temperature, while B-site-ordered double-perovskite-type BaCaNbO remains chemically stable under the same conditions.

Role of Mn content on the electrochemical properties of nickel-rich layered LiNi(0.8-x)Co(0.1)Mn(0.1+x)O₂ (0.0 ≤ x ≤ 0.08) cathodes for lithium-ion batteries.

Ni-rich layered oxides (Ni content >60%) are promising cathode candidates for Li-ion batteries because of their high discharge capacity, high energy density, and low cost. However, fast capacity fading, poor thermal stability, and sensitivity to the ambient moisture still plague their mass application. In this work, we systematically investigate the effects of Mn content on the structure, morphology, electrochemical performance, and thermal stability of the Ni-rich cathode materials LiNi(0.

Studies on polymorphic sequence during the formation of the 1:1 ordered perovskite-type BaCa(0.335)M(0.165)Nb(0.5)O(3-δ) (M = Mn, Fe, Co) using in situ and ex situ powder X-ray diffraction.

Here, we report a synthetic strategy to control the B-site ordering of the transition metal-doped perovskite-type oxides with the nominal formula of BaCa(0.335)M(0.165)Nb(0.

Synthesis and properties of cholesteric click-phospholes.

Inspired by naturally occurring helical supramolecular architectures, a series of chiral conjugated phospholes with a cholesteryl pendant have been synthesized and characterized. The photophysically and electrochemically active conjugated phosphole species can act as dopants for the formation of chiral liquid crystals. The supramolecular structures were found to be tunable by careful choice of the conjugated headgroup as well as the rigidity of the linker of the new cholesteric phospholes.

Thermochemistry of Sr2Ce(1-x)Pr(x)O4 (x = 0, 0.2, 0.5, 0.8, and 1): variable-temperature and -atmosphere in-situ and ex-situ powder X-ray diffraction studies and their physical properties.

A novel family of metal oxides with a chemical formula of Sr(2)Ce(1-x)Pr(x)O(4) (x = 0, 0.2, 0.5, 0.