A High‐Performance Li–B–H Electrolyte for All‐Solid‐State Li Batteries

Highly Li‐ion conductive Li₄(BH₄)₃I@SBA‐15 is synthesized by confining the LiI doped LiBH₄ into mesoporous silica SBA‐15. Uniform nanoconfinement of P6₃ mc phase Li₄(BH₄)₃I in SBA‐15 mesopores leads to a significantly enhanced conductivity of 2.5 × 10^?4 S cm^?1 with a Li‐ion transference number of 0.97 at 35 °C. The super Li‐ion mobility in the interface layer with a thickness of 1.2 nm between Li₄(BH₄)₃I and SBA‐15 is believed to be responsible for the fast Li‐ion conduction in Li₄(BH₄)₃I@SBA‐15. Additionally, Li₄(BH₄)₃I@SBA‐15 also exhibits a wide apparent electrochemical stability window (0 to 5 V vs Li/Li⁺) and a superior Li dendrite suppression capability (critical current density 2.6 mA cm^?2 at 55 °C) due to the formation of stable interphases. More importantly, Li₄(BH₄)₃I@SBA‐15‐based Li batteries using either high‐capacity sulfur cathode or high‐voltage oxide cathode show excellent electrochemical performances, making Li₄(BH₄)₃I@SBA‐15 a very attractive electrolyte for next‐generation all‐solid‐state Li batteries.     

In Situ Formation of Li3P Layer Enables Fast Li+ Conduction across Li/Solid Polymer Electrolyte Interface

Solid‐state polymer electrolytes provide better flexibility and electrode contact than their ceramic counterparts, making them a worthwhile pursuit for all‐solid‐state lithium‐metal batteries. However, their large Li/solid state electrolyte interfacial resistance, small critical current density, and rapid lithium dendrite growth during cycling still limit their viability. Owing to these restrictions, all‐solid‐state cells with solid polymer electrolytes must be cycled above room‐temperature and with a small current density. These problems can be mitigated with an in situ formed artificial solid electrolyte interphase that rapidly conducts Li⁺ ions. Herein, a Li₃P layer formed in situ at the Li‐metal/solid polymer electrolyte interphase is reported that significantly reduces the electrode/electrolyte interfacial resistance. Additionally, this layer increases the wettability of the solid polymer by the metallic lithium anode, allowing for the critical current density of lithium symmetric cells to be doubled by homogenizing the current density at the interface. All‐solid‐state Li/Li symmetric cells and Li/LiFePO₄ cells with the Li₃P layer show improved cycling performance with a high current density.     

Enhanced Interfacial Stability of Hybrid‐Electrolyte Lithium‐Sulfur Batteries with a Layer of Multifunctional Polymer with Intrinsic Nanoporosity

The use of lithium‐ion conductive solid electrolytes offers a promising approach to address the polysulfide shuttle and the lithium‐dendrite problems in lithium‐sulfur (Li‐S) batteries. One critical issue with the development of solid‐electrolyte Li‐S batteries is the electrode–electrolyte interfaces. Herein, a strategic approach is presented by employing a thin layer of a polymer with intrinsic nanoporosity (PIN) on a Li⁺‐ion conductive solid electrolyte, which significantly enhances the ionic interfaces between the electrodes and the solid electrolyte. Among the various types of Li⁺‐ion solid electrolytes, NASICON‐type Li_1+xAl_xTi_2‐x(PO₄)₃ (LATP) offers advantages in terms of Li⁺‐ion conductivity, stability in ambient environment, and practical viability. However, LATP is susceptible to reaction with both the Li‐metal anode and polysulfides in Li‐S batteries due to the presence of easily reducible Ti⁴⁺ ions in it. The coating with a thin layer of PIN presented in this study overcomes the above issues. At the negative‐electrode side, the PIN layer prevents the direct contact of Li‐metal with the LATP solid electrolyte, circumventing the reduction of LATP by Li metal. At the positive electrode side, the PIN layer prevents the migration of polysulfides to the surface of LATP, preventing the reduction of LATP by polysulfides.     

Intercalated Electrolyte with High Transference Number for Dendrite‐Free Solid‐State Lithium Batteries

Solid‐state lithium (Li) batteries using solid electrolytes and Li anodes are highly desirable because of their high energy densities and intrinsic safety. However, low ambient‐temperature conductivity and poor interface compatibility of solid electrolytes as well as Li dendrite formation cause large polarization and poor cycling stability. Herein, a high transference number intercalated composite solid electrolyte (CSE) is prepared by the combination of a solution‐casting and hot‐pressing method using layered lithium montmorillonite, poly(ethylene carbonate), lithium bis(fluorosulfonyl)imide, high‐voltage fluoroethylene carbonate additive, and poly(tetrafluoroethylene) binder. The electrolyte presents high ionic conductivity (3.5 × 10^?4 S cm^?1), a wide electrochemical window (4.6 V vs Li⁺/Li), and high ionic transference number (0.83) at 25 °C. In addition, a 3D Li anode is also fabricated via a facile thermal infusion strategy. The synergistic effect of high transference number intercalated electrolyte and 3D Li anode is more favorable to suppress Li dendrites in a working battery. The solid‐state batteries based on LiFePO₄ (Al₂O₃ @ LiNi_0.5Co_0.2Mn_0.3O₂), CSE, and 3D Li deliver admirable cycling stability with discharge capacity 145.9 mAh g^?1 (150.7 mAh g^?1) and capacity retention 91.9% after 200 cycles at 0.5 C (92.0% after 100 cycles at 0.2 C) at 25 °C. This work affords a splendid strategy for high‐performance solid‐state battery.     

A Mixed Lithium‐Ion Conductive Li2S/Li2Se Protection Layer for Stable Lithium Metal Anode

Constructing artificial solid‐electrolyte interphase (SEI) on the surface of Li metal is an effective approach to improve ionic conductivity of surface SEI and buffer Li dendrite growth of Li metal anode. However, constructing of homogenous ideal artificial SEI is still a great challenge. Here, a mixed lithium‐ion conductive Li₂S/Li₂Se (denoted as LSSe) protection layer, fabricated by a facile and inexpensive gas–solid reaction, is employed to construct stable surface SEI with high ionic conductivity. The Li₂S/Li₂Se‐protected Li metal (denoted as LSSe@Li) exhibits a stable dendrite‐free cycling behavior over 900 h with a high lithium stripping/plating capacity of 3 mAh cm^?2 at 1.5 mA cm^?2 in the symmetrical cell. Compared to bare Li anode, full batteries paired with LiFePO₄, sulfur/carbon, and LiNi_0.6Co_0.2Mn_0.2O₂ cathodes all present better battery cycling and rate performance when LSSe@Li anode is used. Moreover, Li₂Se exhibits a lower lithium‐ion migration energy barrier in comparison with Li₂S which is proved by density functional theory calculation.     

Highly‐Cyclable Room‐Temperature Phosphorene Polymer Electrolyte Composites for Li Metal Batteries

Despite significant interest toward solid‐state electrolytes owing to their superior safety in comparison to liquid‐based electrolytes, sluggish ion diffusion and high interfacial resistance limit their application in durable and high‐power density batteries. Here, a novel quasi‐solid Li⁺ ion conductive nanocomposite polymer electrolyte containing black phosphorous (BP) nanosheets is reported. The developed electrolyte is successfully cycled against Li metal (over 550 h cycling) at 1 mA cm^?2 at room temperature. The cycling overpotential is dropped by 75% in comparison to BP‐free polymer composite electrolyte indicating lower interfacial resistance at the electrode/electrolyte interfaces. Molecular dynamics simulations reveal that the coordination number of Li⁺ ions around (trifluoromethanesulfonyl)imide (TFSI^?) pairs and ethylene‐oxide chains decreases at the Li metal/electrolyte interface, which facilitates the Li⁺ transport through the polymer host. Density functional theory calculations confirm that the adsorption of the LiTFSI molecules at the BP surface leads to the weakening of N and Li atomic bonding and enhances the dissociation of Li⁺ ions. This work offers a new potential mechanism to tune the bulk and interfacial ionic conductivity of solid‐state electrolytes that may lead to a new generation of lithium polymer batteries with high ionic conduction kinetics and stable long‐life cycling.     

A New Strategy to Effectively Suppress the Initial Capacity Fading of Iron Oxides by Reacting with LiBH4

In this work, a new facile and scalable strategy to effectively suppress the initial capacity fading of iron oxides is demonstrated by reacting with lithium borohydride (LiBH₄) to form a B‐containing nanocomposite. Multielement, multiphase B‐containing iron oxide nanocomposites are successfully prepared by ball‐milling Fe₂O₃ with LiBH₄, followed by a thermochemical reaction at 25–350 °C. The resulting products exhibit a remarkably superior electrochemical performance as anode materials for Li‐ion batteries (LIBs), including a high reversible capacity, good rate capability, and long cycling durability. When cycling is conducted at 100 mA g^?1, the sample prepared from Fe₂O₃–0.2LiBH₄ delivers an initial discharge capacity of 1387 mAh g^?1. After 200 cycles, the reversible capacity remains at 1148 mAh g^?1, which is significantly higher than that of pristine Fe₂O₃ (525 mAh g^?1) and Fe₃O₄ (552 mAh g^?1). At 2000 mA g^?1, a reversible capacity as high as 660 mAh g^?1 is obtained for the B‐containing nanocomposite. The remarkably improved electrochemical lithium storage performance can mainly be attributed to the enhanced surface reactivity, increased Li⁺ ion diffusivity, stabilized solid‐electrolyte interphase (SEI) film, and depressed particle pulverization and fracture, as measured by a series of compositional, structural, and electrochemical techniques.     

Low Resistance–Integrated All‐Solid‐State Battery Achieved by Li7La3Zr2O12 Nanowire Upgrading Polyethylene Oxide (PEO) Composite Electrolyte and PEO Cathode Binder

All‐solid‐state lithium metal battery is the most promising next‐generation energy storage device. However, the low ionic conductivity of solid electrolytes and high interfacial impedance with electrode are the main factors to limit the development of all‐solid‐state batteries. In this work, a low resistance–integrated all‐solid‐state battery is designed with excellent electrochemical performance that applies the polyethylene oxide (PEO) with lithium bis(trifluoromethylsulphonyl)imide as both binder of cathode and matrix of composite electrolyte embedded with Li₇La₃Zr₂O₁₂ (LLZO) nanowires (PLLN). The PEO in cathode and PLLN are fused at high temperature to form an integrated all‐solid‐state battery structure, which effectively strengthens the interface compatibility and stability between cathode and PLLN to guarantee high efficient ion transportation during long cycling. The LLZO nanowires uniformly distributed in PLLN can increase the ionic conductivity and mechanical strength of composite electrolyte efficiently, which induces the uniform deposition of lithium metal, thereby suppressing the lithium dendrite growth. The Li symmetric cells using PLLN can stably cycle for 1000 h without short circuit at 60 °C. The integrated LiFePO₄/PLLN/Li batteries show excellent cycling stability at both 60 and 45 °C. The study proposed a novel and robust battery structure with outstanding electrochemical properties.     

High‐Performance Solid Polymer Electrolytes Filled with Vertically Aligned 2D Materials

Solid state lithium metal batteries are the most promising next‐generation power sources owing to their high energy density and safety. Solid polymer electrolytes (SPE) have gained wide attention due to the excellent flexibility, manufacturability, lightweight, and low‐cost processing. However, fatal drawbacks of the SPE such as the insufficient ionic conductivity and Li⁺ transference number at room temperature restrict their practical application. Here vertically aligned 2D sheets are demonstrated as an advanced filler for SPE with enhanced ionic conductivity, Li⁺ transference number, mechanical modulus, and electrochemical stability, using vermiculite nanosheets as an example. The vertically aligned vermiculite sheets (VAVS), prepared by the temperature gradient freezing, provide aligned, continuous, run‐through polymer‐filler interfaces after infiltrating with polyethylene oxide (PEO)‐based SPE. As a result, ionic conductivity as high as 1.89 × 10^?4 S cm^?1 at 25 °C is achieved with Li⁺ transference number close to 0.5. Along with their enhanced mechanical strength, Li|Li symmetric cells using VAVS–CSPE are stable over 1300 h with a low overpotential. LiFePO₄ in all‐solid‐state lithium metal batteries with VAVS–CSPE could deliver a specific capacity of 167 mAh g^?1 at 0.1 C at 35 °C and 82% capacity retention after 200 cycles at 0.5 C.     

High Voltage,Transition Metal Complex Enables Efficient Electrochemical Energy Storage in a Li‐Ion Battery Full Cell

Efficient energy storage systems impact profoundly the renewable energy future. The performance of current electrical energy storage technologies falls well short of requirements for using electrical energy efficiently in transportation, commercial, and residential applications. This paper explores the possibility by using transition‐metal‐based complexes as active materials in a Li‐ion battery full cell that synergizes the concept of both lithium‐ion batteries and redox flow batteries. A cathode made from transition metal complex, [Fe(bpy)₃](BF₄)₂, exhibits high discharge voltage approaching 4 V (vs Li/Li⁺). When coupled with a Li₄Ti₅O₁₂ anode, the Li‐ion full battery exhibits a cell voltage exceeding 2.2 V and decent cycling efficiencies with Coulombic efficiency and energy/voltage efficiencies above 99% and 92%/93%, respectively. Such a Li‐ion battery full cell offers distinct features such as low cost and flexibility in molecular structure design. The result reveals a generic design route toward iron‐based complexes as cathode materials with good electrochemical performances.     

Design of a Multifunctional Interlayer for NASCION‐Based Solid‐State Li Metal Batteries

NASCION‐type Li conductors have great potential to bring high capacity solid‐state batteries to realization, related to its properties such as high ionic conductivity, stability under ambient conditions, wide electrochemical stability window, and inexpensive production. However, their chemical and thermal instability toward metallic lithium (Li) has severely hindered attempts to utilize Li as anode material in NASCION‐based battery systems. In this work, it is shown how a tailored multifunctional interlayer between the solid electrolyte and Li anode can successfully address the interfacial issues. This interlayer is designed by creating a quasi‐solid‐state paste in which the functionalities of LAGP (Li_1.5Al_0.5Ge_1.5(PO₄)₃) nanoparticles and an ionic liquid (IL) electrolyte are combined. In a solid‐sate cell, the LAGP‐IL interlayer separates the Li metal from bulk LAGP and creates a chemically stable interface with low resistance (≈5 Ω cm²) and efficiently prevents thermal runaway at elevated temperatures (300 °C). Solid‐state cells designed with the interlayer can be operated at high current densities, 1 mA cm^?2, and enable high rate capability with high safety. Here developed strategy provides a generic path to design interlayers for solid‐state Li metal batteries.     

Toward Optimal Performance and In‐Depth Understanding of Spinel Li4Ti5O12 Electrodes through Phase Field Modeling

Computational modeling is vital for the fundamental understanding of processes in Li‐ion batteries. However, capturing nanoscopic to mesoscopic phase thermodynamics and kinetics in the solid electrode particles embedded in realistic electrode morphologies is challenging. In particular for electrode materials displaying a first order phase transition, such as LiFePO₄, graphite, and spinel Li₄Ti₅O₁₂, predicting the macroscopic electrochemical behavior requires an accurate physical model. Herein, a thermodynamic phase field model is presented for Li‐ion insertion in spinel Li₄Ti₅O₁₂ which captures the performance limitations presented in literature as a function of all relevant electrode parameters. The phase stability in the model is based on ab initio density functional theory calculations and the Li‐ion diffusion parameters on nanoscopic nuclear magnetic resonance (NMR) measurements of Li‐ion mobility, resulting in a parameter free model. The direct comparison with prepared electrodes shows good agreement over three orders of magnitude in the discharge current. Overpotentials associated with the various charge transport processes, as well as the active particle fraction relevant for local hotspots in batteries, are analyzed. It is demonstrated which process limits the electrode performance under a variety of realistic conditions, providing comprehensive understanding of the nanoscopic to microscopic properties. These results provide concrete directions toward the design of optimally performing Li₄Ti₅O₁₂ electrodes.     

High Lithium Ion Conductivity LiF/GO Solid Electrolyte Interphase Inhibiting the Shuttle of Lithium Polysulfides in Long‐Life Li–S Batteries

The “shuttle effect” that stems from the dissolution of polysulfides is the most fatal issue affecting the cycle life of lithium‐sulfur (Li–S) batteries. In order to suppress the “shuttle effect,” a new strategy of using a highly lithium ion conductive lithium fluoride/graphene oxide (LiF/GO) solid electrolyte interphase (SEI) to mechanically prevent the lithium dendrite breakthrough is reported. When utilized in Li–S batteries, the LiF/GO SEI coated separator demonstrates significant feature in mitigating the polysulfide shuttling as observed by in situ UV–vis spectroscopy. Moreover, the restrained “shuttle effect” can also be confirmed by analysis of electrochemical impedance spectroscopy and characterization of lithium dendrites, which indicates that no insulating layer of solid Li₂S₂/Li₂S is found on lithium anode surface. Furthermore, the LiF/GO SEI layer puts out good lithium ion conductivity as its lithium ion diffusion coefficient reaches a high value of 1.5 × 10^?7 cm² s^?1. These features enable a remarkable cyclic property of 0.043% of capacity decay per cycle during 400 cycles.     

Amorphous Dual-Layer Coating: Enabling High Li-Ion Conductivity of Non-Sintered Garnet-Type Solid Electrolyte

Garnet-type oxide Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO) has attracted considerable attention as a highly promising solid state electrolyte. However, its high ionic conductivity is achievable only after high temperature sintering (≈1200 °C) to form dense pellets but with detrimental brittleness and poor contact with electrodes. Herein, a novel strategy to achieve high Li⁺ ion conductivity of LLZTO without sintering is demonstrated. This is realized by ball milling LLZTO together with LiBH₄, which results in a LLZTO composite with unique amorphous dual coating: LiBO₂ as the inner layer and LiBH₄ as the outer layer. After cold pressing the LLZTO composite powders under 300 MPa to form electrolyte pellets, a high Li⁺ ion conductivity of 8.02 × 10^–5 S cm^–1 is obtained at 30 °C, which is four orders of magnitude higher than that of the non-sintered pristine LLZTO pellets (4.17 × 10^–9 S cm^–1). The composite electrolyte displays an ultrahigh Li⁺ transference number of 0.9999 and enables symmetric Li–Li cells to be cycled for 1000 h at 60 °C and 300 h at 30 °C. The significant improvements are attributed to the continuous ionic conductive network among LLZTO particles facilitated by LiBH₄ that is chemically compatible and electrochemically stable with Li metal electrode.     

Flexible Electrocatalytic Nanofiber Membrane Reactor for Lithium/Sulfur Conversion Chemistry

Severe lithium polysulfide (LiPS) shuttle effects and sluggish electrochemical conversion kinetics constitute bottlenecks in developing fast‐rechargeable, high‐energy, and high‐power Li/S batteries. Here, a flexible and conductive TiN–Ti₄O₇ core‐shell nanofiber (TiNOC) membrane reactor is designed to electrocatalytically mediate Li/S conversion chemistry. The Ti, N, and O atoms in the nanofiber function as electrocatalysts and chemical confinement active sites to initiate long‐chain LiPS conversion and phase change, as well as to suppress soluble LiPS shuttling. With a sulfur cathode‐membrane reactor module configuration, Li/S cells possess a high sulfur utilization of 91.20%, good rate capability of 869.10 mA h g^?1, and high capacity retention of 92.49%, with a coulomb efficiency of 99.57% after 200 cycles at 5 C. Density functional theory (DFT) calculations revealed that the optimized chemisorption configurations facilitate the elongation of Li? S and S? S bonds, as well as charge transfer along Ti? S and Li? N bonds, which favors bond breakage, bond formation, and the activation of solid‐state S₈, Li₂S₂, and Li₂S. Layer‐by‐layer module stacking provides Li/S batteries with a high areal sulfur loading of 12.00 mg cm^?2 to deliver a high areal capacity of 14.40 mA h cm^?2 at 2.26 mA. Two batteries in series can power real‐world applications such as light emitting diode (LED) bulbs with a high energy output of 69.00 mW h.     

A Li–Al–O Solid‐State Electrolyte with High Ionic Conductivity and Good Capability to Protect Li Anode

Using a solid‐state electrolyte (SSE) to stabilize the Li metal anode is widely considered a promising route to develop next‐generation high energy density lithium batteries. Here, a new polycrystalline aluminate‐based SSE (named Li–Al–O SSE) with good capability is introduced to protect Li metal. The SSE is formed on the Li metal surface via a chemical reaction between LiOH and triethylaluminum (TEAL) with the existence of LiTFSI‐based electrolyte. It is a continuous film that consists of polycrystalline LiAlO₂, Li₃AlO₃, Al₂O₃, Li₂CO₃, LiF, and some organic compounds. Such Li–Al–O SSE possesses a room‐temperature ionic conductivity as high as 1.42 × 10^?4 S cm^?1. Meanwhile, it effectively protects the Li anode from the corrosion of H₂O, O₂, and organic solvent, and suppresses the growth of Li dendrite. With the protection of the Li–Al–O SSE, the cycle life of Li|Li symmetric cell and Li|O₂ cell is substantially elongated, indicating that the SSE exhibits an excellent protective effect under both inert and oxidizing circumstances.     

Li6ALa2Ta2O12 (A = Sr, Ba): Novel Garnet‐Like Oxides for Fast Lithium Ion Conduction

Oxides with the nominal chemical formula Li₆ALa₂Ta₂O₁₂ (A = Sr, Ba) have been prepared via a solid‐state reaction in air using high purity La₂O₃, LiOH·H₂O, Sr(NO₃)₂, Ba(NO₃)₂, and Ta₂O₅ and are characterized by powder X‐ray diffraction (XRD) in order to identify the phase formation and AC impedance to determine the lithium ion conductivity. The powder XRD data of Li₆ALa₂Ta₂O₁₂ show that they are isostructural with the parent garnet‐like compound Li₅La₃Ta₂O₁₂. The cubic lattice parameter was found to increase with increasing ionic size of the alkaline earth ions (Li₆SrLa₂Ta₂O₁₂: 12.808(2) Å; Li₆BaLa₂Ta₂O₁₂: 12.946(3) Å). AC impedance results show that both the strontium and barium members exhibit mainly a bulk contribution with a rather small grain‐boundary contribution. The ionic conductivity increases with increasing ionic radius of the alkaline earth elements. The barium compound, Li₆BaLa₂Ta₂O₁₂, shows the highest ionic conductivity, 4.0×10^–5 S cm^–1 at 22 °C with an activation energy of 0.40 eV, which is comparable to other lithium ion conductors, especially with the presently employed solid electrolyte lithium phosphorus oxynitride (Lipon) for all‐solid‐state lithium ion batteries. DC electrical measurements using lithium‐ion‐blocking and reversible electrodes revealed that the electronic conductivity is very small, and a high electrochemical stability (> 6 V/Li) was exhibited at room temperature. Interestingly, Li₆ALa₂Ta₂O₁₂ was found to be chemically stable with molten metallic lithium.     

Stabilizing Polymer–Lithium Interface in a Rechargeable Solid Battery

Solid polymer electrolytes (SPEs) are promising candidates for developing high‐energy‐density Li metal batteries due to their flexible processability. However, the low mechanical strength as well as the inferior interfacial regulation of ions between SPEs and Li metal anode limit the suppress ion of Li dendrites and destabilize the Li anode. To meet these challenges, interfacial engineering aiming to homogenize the distribution of Li⁺/electron accompanied with enhanced mechanical strength by Mg₃N₂ layer decorating polyethylene oxide is demonstrated. The intermediary Mg₃N₂ in situ transforms to a mixed ion/electron conducting interlayer consisting of a fast ionic conductor Li₃N and a benign electronic conductor Mg metal, which can buffer the Li⁺ concentration gradient and level the nonuniform electric current distribution during cycling, as demonstrated by a COMSOL Multiphysics simulation. These characteristics endow the solid full cell with a dendrite‐free Li anode and enhanced cycling stability and kinetics. The innovative interface design will accelerate the commercial application of high‐energy‐density solid batteries.     

Fast and Reversible Li Ion Insertion in Carbon‐Encapsulated Li3VO4 as Anode for Lithium‐Ion Battery

Carbon‐encapsulated Li₃VO₄ is synthesized by a facile environmentally benign solid‐state method with organic metallic precursor VO(C₅H₇O₂)₂ being chosen as both V and carbon sources yielding a core–shell nanostructure with lithium introduced in the subsequent annealing process. The Li₃VO₄ encapsulated with carbon presents exceeding rate capability (a reversible capability of 450, 340, 169, and 106 mAh g^?1 at 0.1 C, 10 C, 50 C, and 80 C, respectively) and long cyclic performance (80% capacity retention after 2000 cycles at 10 C) as an anode in lithium‐ion batteries. The superior performance is derived from the structural features of the carbon‐encapsulated Li₃VO₄ composite with oxygen vacancies in Li₃VO₄, which increase surface energy and could possibly serve as a nucleation center, thus facilitating phase transitions. The in situ generated carbon shell not only facilitates electron transport, but also suppresses Li₃VO₄ particle growth during the calcination process. The encouraging results demonstrate the significant potential of carbon encapsulated Li₃VO₄ for high power batteries. In addition, the simple generic synthesis method is applicable to the fabrication of a variety of electrode materials for batteries and supercapacitors with unique core–shell structure with mesoporous carbon shell.     

Intrinsic Lithiophilicity of Li–Garnet Electrolytes Enabling High‐Rate Lithium Cycling

Solid‐state lithium batteries are widely considered as next‐generation lithium‐ion battery technology due to the potential advantages in safety and performance. Among the various solid electrolyte materials, Li–garnet electrolytes are promising due to their high ionic conductivity and good chemical and electrochemical stabilities. However, the high electrode/electrolyte interfacial impedance is one of the major challenges. Moreover, short circuiting caused by lithium dendrite formation is reported when using Li–garnet electrolytes. Here, it is demonstrated that Li–garnet electrolytes wet well with lithium metal by removing the intrinsic impurity layer on the surface of the lithium metal. The Li/garnet interfacial impedance is determined to be 6.95 Ω cm² at room temperature. Lithium symmetric cells based on the Li–garnet electrolytes are cycled at room temperature for 950 h and current density as high as 13.3 mA cm^?2 without showing signs of short circuiting. Experimental and computational results reveal that it is the surface oxide layer on the lithium metal together with the garnet surface that majorly determines the Li/garnet interfacial property. These findings suggest that removing the superficial impurity layer on the lithium metal can enhance the wettability, which may impact the manufacturing process of future high energy density garnet‐based solid‐state lithium batteries.