A self-healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteries.

Oxide ceramic electrolytes (OCEs) have great potential for solid-state lithium metal (Li) battery applications because, in theory, their high elastic modulus provides better resistance to Li dendrite growth. However, in practice, OCEs can hardly survive critical current densities higher than 1 mA/cm. Key issues that contribute to the breakdown of OCEs include Li penetration promoted by grain boundaries (GBs), uncontrolled side reactions at electrode-OCE interfaces, and, equally importantly, defects evolution (e.

A Self-Healing, Flowable, Yet Solid Electrolyte Suppresses Li-Metal Morphological Instabilities.

Lithium metal (Li) solid-state batteries encounter implementation challenges due to dendrite formation, side reactions, and movement of the electrode-electrolyte interface in cycling. Notably, voids and cracks formed during battery fabrication/operation are hot spots for failure. Here, a self-healing, flowable yet solid electrolyte composed of mobile ceramic crystals embedded in a reconfigurable polymer network is reported.

Alkaline Earth Bismuth Fluorides as Fluoride-Ion Battery Electrolytes.

Fluoride-ion batteries have several potential advantages over lithium-ion batteries. Materials development is still needed, however, to realize electrolytes with sufficiently high anion conductivity and compatibility with anode and cathode layers. Fluoride compounds are difficult to synthesize directly as single crystals but can be realized from oxide film precursors via topotactic chemistry techniques.

Interrogation of 3d Transition Bimetallic Nanocrystal Nucleation and Growth Using Electron Microscope and Synchrotron X-ray Techniques.

Understanding the nucleation and growth mechanism of 3d transition bimetallic nanocrystals (NCs) is crucial to developing NCs with tailored nanostructures and properties. However, it remains a significant challenge due to the complexity of 3d bimetallic NCs formation and their sensitivity to oxygen. Here, by combining electron microscopy and synchrotron X-ray techniques, we elucidate the nucleation and growth pathways of Fe-Ni NCs.

Atomic Origin of Chemomechanical Failure of Layered Cathodes in All-Solid-State Batteries.

The ever-increasing demand for safety has thrust all-solid-state batteries (ASSBs) into the forefront of next-generation energy storage technologies. However, the atomic mechanisms underlying the failure of layered cathodes in ASSBs, as opposed to their counterparts in liquid electrolyte-based lithium-ion batteries (LIBs), have remained elusive. Here, leveraging artificial intelligence-enhanced super-resolution electron microscopy, we unravel the atomic origins dictating the chemomechanical degradation of technologically crucial high-Ni layered oxide cathodes in ASSBs.

A Water-in-Salt Electrolyte for Room-Temperature Fluoride-Ion Batteries Based on a Hydrophobic-Hydrophilic Salt.

Realizing room-temperature, efficient, and reversible fluoride-ion redox is critical to commercializing the fluoride-ion battery, a promising post-lithium-ion battery technology. However, this is challenging due to the absence of usable electrolytes, which usually suffer from insufficient ionic conductivity and poor (electro)chemical stability. Herein we report a water-in-salt (WIS) electrolyte based on the tetramethylammonium fluoride salt, an organic salt consisting of hydrophobic cations and hydrophilic anions.

Making Plasticized Polymer Electrolytes Stable Against Sodium Metal for High-Energy Solid-State Sodium Batteries.

Solid polymer electrolytes based on plastic crystals are promising for solid-state sodium metal (Na) batteries, yet their practicality has been hindered by the notorious Na-electrolyte interface instability issue, the underlying cause of which remains poorly understood. Here, by leveraging a model plasticized polymer electrolyte based on conventional succinonitrile plastic crystals, we uncover its failure origin in Na batteries is associated with the formation of a thick and non-uniform solid electrolyte interphase (SEI) and whiskery Na nucleation/growth. Furthermore, we design a new additive-embedded plasticized polymer electrolyte to manipulate the Na deposition and SEI formulation.

Reversible Cl/Cl redox in a spinel MnO electrode.

A unique prospect of using halides as charge carriers is the possibility of the halides undergoing anodic redox behaviors when serving as charge carriers for the charge-neutrality compensation of electrodes. However, the anodic conversion of halides to neutral halogen species has often been irreversible at room temperature due to the emergence of diatomic halogen gaseous products. Here, we report that chloride ions can be reversibly converted to near-neutral atomic chlorine species in the MnO electrode at room temperature in a highly concentrated chloride-based aqueous electrolyte.

MnEdgeNet for accurate decomposition of mixed oxidation states for Mn XAS and EELS L2,3 edges without reference and calibration.

Accurate decomposition of the mixed Mn oxidation states is highly important for characterizing the electronic structures, charge transfer and redox centers for electronic, and electrocatalytic and energy storage materials that contain Mn. Electron energy loss spectroscopy (EELS) and soft X-ray absorption spectroscopy (XAS) measurements of the Mn L2,3 edges are widely used for this purpose. To date, although the measurements of the Mn L2,3 edges are straightforward given the sample is prepared properly, an accurate decomposition of the mix valence states of Mn remains non-trivial.

Deep-Learning Aided Atomic-Scale Phase Segmentation toward Diagnosing Complex Oxide Cathodes for Lithium-Ion Batteries.

Phase transformation─a universal phenomenon in materials─plays a key role in determining their properties. Resolving complex phase domains in materials is critical to fostering a new fundamental understanding that facilitates new material development. So far, although conventional classification strategies such as order-parameter methods have been developed to distinguish remarkably disparate phases, highly accurate and efficient phase segmentation for material systems composed of multiphases remains unavailable.

Anion-tethered Single Lithium-ion Conducting Polyelectrolytes through UV-induced Free Radical Polymerization for Improved Morphological Stability of Lithium Metal Anodes.

Single Li ion conducting polyelectrolytes (SICs), which feature covalently tethered counter-anions along their backbone, have the potential to mitigate dendrite formation by reducing concentration polarization and preventing salt depletion. However, due to their low ionic conductivity and complicated synthetic procedure, the successful validation of these claimed advantages in lithium metal (Li ) anode batteries remains limited. In this study, we fabricated a SIC electrolyte using a single-step UV polymerization approach.

Hard-Soft Core-Shell Architecture Formation from Cubic Cobalt Ferrite Nanoparticles.

Cubic bi-magnetic hard-soft core-shell nanoarchitectures were prepared starting from cobalt ferrite nanoparticles, prevalently with cubic shape, as seeds to grow a manganese ferrite shell. The combined use of direct (nanoscale chemical mapping via STEM-EDX) and indirect (DC magnetometry) tools was adopted to verify the formation of the heterostructures at the nanoscale and bulk level, respectively. The results showed the obtainment of core-shell NPs (CoFeO@MnFeO) with a thin shell (heterogenous nucleation).

Regulating Cation Interactions for Zero-Strain and High-Voltage P2-type Na Li Co Mn O Layered Oxide Cathodes of Sodium-Ion Batteries.

Deep sodium extraction/insertion of sodium cathodes usually causes undesired Jahn-Teller distortion and phase transition, both of which will reduce structural stability and lead to poor long-cycle reliability. Here we report a zero-strain P2- Na Li Co Mn O cathode, in which the lithium/cobalt substitution contributes to reinforcing the host structure by reducing the Mn /Mn redox, mitigating the Jahn-Teller distortion, and minimizing the lattice change. 94.

Atomically Dispersed Silver Atoms Embedded in NiCo Layer Double Hydroxide Boost Oxygen Evolution Reaction.

Bimetallic layered double hydroxides (LDHs) are promising catalysts for anodic oxygen evolution reaction (OER) in alkaline media. Despite good stability, NiCo LDH displays an unsatisfactory OER activity relative to the most robust NiFe LDH and CoFe LDH. Herein, a novel NiCo LDH electrocatalyst modified with single-atom silver grown on carbon cloth (Ag -NiCo LDH/CC) that exhibits exceptional OER activity and stability in 1.

RadVolViz: An Information Display-Inspired Transfer Function Editor for Multivariate Volume Visualization.

In volume visualization transfer functions are widely used for mapping voxel properties to color and opacity. Typically, volume density data are scalars which require simple 1D transfer functions to achieve this mapping. If the volume densities are vectors of three channels, one can straightforwardly map each channel to either red, green or blue, which requires a trivial extension of the 1D transfer function editor.

Resolving complex intralayer transition motifs in high-Ni-content layered cathode materials for lithium-ion batteries.

High-Ni-content layered materials are promising cathodes for next-generation lithium-ion batteries. However, investigating the atomic configurations of the delithiation-induced complex phase boundaries and their transitions remains challenging. Here, by using deep-learning-aided super-resolution electron microscopy, we resolve the intralayer transition motifs at complex phase boundaries in high-Ni cathodes.

Disordered Au Nanoclusters for Efficient Ammonia Electrosynthesis.

The electrochemical nitrogen (N ) reduction reaction (N RR) under mild conditions is a promising and environmentally friendly alternative to the traditional Haber-Bosch process with high energy consumption and greenhouse emission for the synthesis of ammonia (NH ), but high-yielding production is rendered challenging by the strong nonpolar N≡N bond in N molecules, which hinders their dissociation or activation. In this study, disordered Au nanoclusters anchored on two-dimensional ultrathin Ti C T MXene nanosheets are explored as highly active and selective electrocatalysts for efficient N -to-NH conversion, exhibiting exceptional activity with an NH yield rate of 88.3±1.

Hydrogen-substituted graphdiyne-assisted ultrafast sparking synthesis of metastable nanomaterials.

Metastable nanomaterials, such as single-atom and high-entropy systems, with exciting physical and chemical properties are increasingly important for next-generation technologies. Here, we developed a hydrogen-substituted graphdiyne-assisted ultrafast sparking synthesis (GAUSS) platform for the preparation of metastable nanomaterials. The GAUSS platform can reach an ultra-high reaction temperature of 3,286 K within 8 ms, a rate exceeding 10 K s.

Electron energy loss spectroscopy database synthesis and automation of core-loss edge recognition by deep-learning neural networks.

The ionization edges encoded in the electron energy loss spectroscopy (EELS) spectra enable advanced material analysis including composition analyses and elemental quantifications. The development of the parallel EELS instrument and fast, sensitive detectors have greatly improved the acquisition speed of EELS spectra. However, the traditional way of core-loss edge recognition is experience based and human labor dependent, which limits the processing speed.

Oxygen-Loss-Induced Structural Degradation in ε-LiVOPO.

The ε-LiVOPO cathode for Li-ion batteries has attracted wide attention with its multivalent electronic states and improved discharge capacity of over 300 mAh/g. Oxygen loss stands as a potential cause for structural degradations of the ε-LiVOPO cathode and its derivatives but has been barely studied. Through environmental transmission electron microscopy, we probe lattice oxygen loss and the associated structural degradations by spatially and temporally resolving the atomic-scale structural dynamics and phase transformation pathways in ε-LiVOPO.

Activating Single-Atom Ni Site via First-Shell Si Modulation Boosts Oxygen Reduction Reaction.

Atomically dispersed nitrogen-coordinated 3d transition-metal site on carbon support (M-NC) are promising alternatives to Pt group metal-based catalysts toward oxygen reduction reaction (ORR). However, despite the excellent activities of most of M-NC catalysts, such as Fe-NC, Co-NC et al., their durability is far from satisfactory due to Fenton reaction.

Tension-Induced Cavitation in Li-Metal Stripping.

Designing stable Li metal and supporting solid structures (SSS) is of fundamental importance in rechargeable Li-metal batteries. Yet, the stripping kinetics of Li metal and its mechanical effect on the supporting solids (including solid electrolyte interface) remain mysterious to date. Here, through nanoscale in situ observations of a solid-state Li-metal battery in an electron microscope, two distinct cavitation-mediated Li stripping modes controlled by the ratio of the SSS thickness (t) to the Li deposit's radius (r) are discovered.

Super-Hydrophilic Microporous Ni(OH)x/Ni S Heterostructure Electrocatalyst for Large-Current-Density Hydrogen Evolution.

Exploiting active and stable non-precious metal electrocatalysts for alkaline hydrogen evolution reaction (HER) at large current density plays a key role in realizing large-scale industrial hydrogen generation. Herein, a self-supported microporous Ni(OH)x/Ni S heterostructure electrocatalyst on nickel foam (Ni(OH)x/Ni S /NF) that possesses super-hydrophilic property through an electrochemical process is rationally designed and fabricated. Benefiting from the super-hydrophilic property, microporous feature, and self-supported structure, the electrocatalyst exhibits an exceptional HER performance at large current density in 1.