Textured ceramics with anisotropic ionic conductivity are poised to establish superior ion transport pathways in solid-state electrochemical devices. However, their preparation methods remain a challenge. Here, we develop a gas-solid reactive sintering technique that successfully fabricates a variety of textured lithium ceramics, including electrolyte and electrode materials. These textured lithium ceramic electrolytes exhibit large columnar grains perpendicular to the surface. The textured electrodes indicate an out-of-plane crystallographic texture. As a result, the Li-ion transport pathways across the grain boundary plane are avoided in the textured lithium ceramic with low tortuosity, resulting in great ionic conductivity enhancement by 42 times compared to its traditional equiaxed counterpart. In addition, both Monte Carlo simulation and finite element analysis support the experimental results. This innovative gas-solid reactive sintering technique can extend to prepare various structured and functional ceramics with tailored structures and properties.

High-entropy electrolytes have attracted extensive attention for their potential to overcome the limits of traditional materials. However, confirming the accurate synthesis of a single-phase high-entropy electrolyte remains a challenge. Herein, we develop a quinary garnet electrolyte of cubic phase with high resistance to air corrosion. By employing a straightforward method that analyzes the variations of diffraction peak intensity, we can evaluate the feasibility of high-entropy doping, the degree of cubic phase, and the extent of H+/Li+ exchange. Meanwhile, ambient pressure X-ray photoelectron spectroscopy is utilized to investigate the degradation of garnet electrolyte by H2O, with the failure mechanism further elucidated by nuclear magnetic resonance analysis. On this basis, the high-entropy garnet electrolyte demonstrated increased cubic phase content and better air stability, compared with traditional counterpart. Consequently, a higher current critical density is achieved, facilitating the integration of commercial cathodes with high area capacities into the quasi-solid-state batteries. Our findings provide an effective method for synthesizing and evaluating high entropy electrolytes.

Garnet-type solid electrolyte cubic Li7La3Zr2O12 (c-LLZO) emerges as a promising candidate for establishing reliable and high-performance lithium-ion batteries. Its extreme sensitivity to electron irradiation poses a significant challenge in atomically resolving its structure using conventional transmission electron microscopy (TEM) techniques. We demonstrate that the combination of low-dose four-dimensional scanning TEM (4D-STEM) with multislice ptychographic retrieval methodology manages to achieve a sub-Angstrom resolution and the direct visualization of lithium atoms within c-LLZO. The distribution of lithium in depth direction is also obtained. This work provides atomic-scale insights into the distribution of light elements within irradiation-sensitive dense crystals, paving the way for investigating the microstructure-property relationship.

Ultrathin solid‐polymer‐electrolytes (SPEs) are the most promising alternative substituting for the conventional liquid electrolyte to enable high‐energy‐density, safe lithium‐metal‐batteries (LMBs). Nevertheless, developing ultrathin SPEs with both high ionic conductivity, and strong Li dendrite retardant is still a significant challenge. Here a scalable fabrication of high‐performance ultrathin (≈7.8 µm) polycarbonate‐based electrolyte (UPCE) is proposed via electrolyte structural engineering, phase separation‐derived poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVH) porous scaffold, without use of additional liquid additives. The rational electrolyte structural modulation with 1‐fluoro‐4‐(1‐methylethenyl)benzene (FMB) enables a weakened Li + ‐polymer interaction due to weak Li + solvation with fluorine, benzene ring, facilitates the formation of LiF‐rich solid‐electrolyte‐interphase on Li metal surface. As a result, the designed UPCE delivers a high ionic conductivity of 4.8 × 10 −4 S cm −1 , an ultrahigh critical current density of 11.5 mA cm −2 at 25 °C. The solid‐state Li symmetric cell attains unprecedented ultralong cycling over 6000 h at 0.5 mA cm −2 . Furthermore, the Li|LiCoO 2 cell cycles stably over 1500 cycles at a high operating voltage of 4.5 V, and the pouch cell can achieve a high energy density of 495 Wh kg −1 excluding the packaging. This work offers a new pathway inspiring efforts to commercialize ultrathin SPEs for high‐energy solid‐state LMBs.

The growth of lithium dendrites and propagation of cracks within solid electrolytes present significant challenges to the safety of solid-state lithium-metal batteries, whose underlying failure mechanism remains unclear. Herein, we report a previously overlooked failure mechanism in garnet electrolyte, driven by stress-induced localized phase transition that accelerates Li dendrite short-circuiting. Employing Bragg coherent diffraction imaging, we reveal heterogeneous strain fields and dislocation proliferation within solid-electrolyte grains generated by Li dendrites. Transmission electron microscopy results directly confirm a cubic-to-tetragonal phase transition in the dendrite-penetrated regions. Molecular dynamics simulations further demonstrate that this transition is driven by GPa-level stresses generated by dendrite penetration, accompanied by lattice distortion, point defects and dislocations, which collectively reduce the critical stress for crack propagation. This work provides atomic-scale evidence that stress-induced phase transition is a critical factor in solid-electrolyte failure, identifying new principles for designing dendrite-resistant solid electrolytes for next-generation batteries.

Halide solid-state electrolytes are promising for next-generation all-solid-state lithium-ion batteries due to their high ionic conductivity and wide electrochemical windows. While most research focuses on close-packed crystal structures, nonclose-packed frameworks─exemplified by UCl3-type structures─offer unique advantages in enhancing lithium-ion transport via reduced diffusion barriers. Here, we report a new family of UCl3-type crystalline oxychloride electrolytes, Li0.388+xLa0.475Ta0.238Cl3-xOx (0 ≤ x ≤ 0.388, LLTCO), synthesized via rapid high-energy shake milling. The material with an optimized composition (x = 0.15) exhibits high ionic conductivity above 2 mS cm-1 at 30 °C, oxidative stability exceeding 5 V vs Li/Li+, and excellent mechanical compressibility. Moreover, the LLTCO-based Li-Li symmetric cells show a long cycle life, indicating their strong capacity to suppress lithium dendrite formation. Spectroscopy analyses reveal the successful incorporation of oxygen, which preferentially substitutes Cl- around Ta5+ sites without compromising crystallinity, even at a high oxygen content. The oxygen incorporation further promotes the formation of Li environments with fast dynamics, accounting for the enhanced conductivity. All-solid-state batteries utilizing the optimized oxychloride electrolyte in conjunction with Ni-rich cathodes demonstrate enhanced reversible capacities compared to their undoped counterparts. This work highlights the benefits of nonclose-packed UCl3-type oxychloride electrolytes, offering new design strategies for high-performance all-solid-state batteries.

Limiting the amount of lithium (Li) metal anode is critical for achieving high‐energy density in solid‐state Li‐metal full cells. However, the inherently low mechanical properties of bare Li metal limit the fabrication of freestanding ultrathin films. Herein, a free‐standing, lightweight, and robust Li‐limited anode with a thickness of 25 µm is designed to enable high‐energy‐density solid‐state full cells. This Li‐limited anode is fabricated by evaporating a controlled amount of Li metal on cellulose fiber matrix coated with silver (Ag) nanoparticles, denoted as cellulose@Ag/limited Li (CALL). Notably, CALL exhibits an extra low nucleation overpotential (2.2 mV) in the solid polymer electrolyte based Li symmetric cells and demonstrates stable cycling for over 300 h at 0.2 mA cm −2 . Coupled with the high‐mass‐loading LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathode, the solid‐state Li‐metal full cells present an initial specific capacity of 200 mAh g −1 and sustain stable cycling over 100 cycles. The pouch cell delivers a high energy density of 401.1 Wh kg −1 . Furthermore, the in situ Li deposition observation and in situ stress monitoring reveal the uniform strain distribution in CALL, underpinning its superior electrochemical performance. This work proposes a simple yet effective method for fabricating ultrathin Li films, advancing the development of high‐energy‐density solid‐state Li‐metal full cells.

To enhance the compatibility between the electrolyte and electrode in a Li metal all-solid-state battery, a composite polymer electrolyte (CPE) modified with a metal-organic framework (MOF) is utilized. The Mg ligands in Mg-MOF-74 are connected to the F site in polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) and lithium salt, forming a robust cross-linking network. Due to the abundant pores in the Mg-MOF-74 skeleton, this cross-linking membrane not only secures the polymer chains but also provides large and uniform Li+ transport channels. The CPE membrane demonstrates high ionic conductivity (2.94 x 10(-4) S.cm(-1)) and a wide electrochemical stability window (4.95 V). Utilizing a high-voltage LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode, the allsolid-state battery exhibits stable cycle performance and an exceptional capacity retention rate of 90.16 % after 100 cycles.

Abstract Garnet oxide is one of the most promising solid-state electrolytes for solid-state lithium metal batteries. However, the traditional interface modification layers cannot completely block electron migrating from the current collector to the interior of the solid-state electrolyte, which promotes the penetration of lithium dendrites. In this work, a highly electron-blocking interlayer composed of potassium fluorine (KF) is developed to inhibit lithium dendrite growth in garnet oxide Li6.4La3Zr1.4Ta0.6O12 (LLZTO). Thanks to the interlayer of stable KF with large band gap, the electronic conductivity of LLZTO reduces by two orders of magnitude. The Li symmetric cells using KF interlayer show an ultralong cycle life ~3000 hours at 0.2 mA cm-2 and over 350 hours at 0.5 mA cm-2 respectively. Moreover, an ionic liquid of LiTFSI in C4mim-TFSI is screened to wet the cathode interfaces. The solvent-free Li|LLZTO|LiNi0.8Co0.1Mn0.1O2 cells present a high specific capacity, and a long lifespan of 3500 cycles at 2C with an average coulombic efficiency of 99.99%. This work provides a simple and integrated strategy on high-performance solid-state lithium metal batteries.

Garnet-type oxide is one of the most promising solid-state electrolytes (SSEs) for solid-state lithium-metal batteries (SSLMBs). However, the Li dendrite formation in garnet oxides obstructs the further development of the SSLMBs seriously. Here, we report a high-performance garnet oxide by using AlN as a sintering additive and Li as an anode interface layer. AlN with high thermal conductivity can promote the sintering activity of the garnet oxides, resulting in larger particle size and higher relative density. Moreover, Li3N with high ionic conductivity formed at grain boundaries and interface can also improve Li-ion transport kinetics. As a result, the garnet oxide electrolytes with AlN show enhanced thermal conductivity, improved ionic conductivity, reduced electronic conductivity, and increased critical current density (CCD), compared with the counterpart using Al2O3 sintering aid. In addition, Li symmetric cells and Li∣LiFePO4 (Li∣LFP) half cells using the garnet electrolyte with the AlN additive exhibit good electrochemical performances. This work provides a simple and effective strategy for high-performance SSEs.

The development of high-performance, low-cost and large-scale water/seawater splitting bifunctional electro-catalysts still faces huge challenges. Here, we deliver a novel and simple spontaneous redox synthesis strategy to fabricate a self-supported Pt-CoFe(II) layered double hydroxide (LDH) electrocatalyst. The three-dimensional porous structure of the catalyst and the synergistic effect of Pt clusters and CoFe hydroxides jointly contribute to its excellent catalytic activity and enhanced chemical stability. Specifically, in 1 M KOH, the overpotentials for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) of Pt-CoFe(II) LDH at 10 mA cm(-2) are 214 mV and 15 mV, respectively. The catalysts are stable for at least 40 h at high current densities of 100 and 500 mA cm-2. Compared with previously reported electrocatalysts, Pt-CoFe(II) LDHs || Pt-CoFe(II) LDHs overall water (seawater) electrolyzers only require 1.634 (1.651) and 1.798 (1.858) V to reach 100 and 500 mA cm-2 in 1 M KOH water (seawater) electrolyte, confirming the superior catalytic activity of the self-supported Pt-CoFe(II) layered double hydroxide electrocatalysts. This study provides a novel and simple synthesis strategy to prepare advanced water/seawater splitting electrocatalysts, which is highly relevant for commercial applications.

通过浆料刷涂-烧结法在Cf/SiC复合材料表面制备了ZrB2-SiC-B4C超高温陶瓷涂层,研究了浆料中粉末填料、稀释剂的质量分数及高温烧结温度对涂层形貌、成分和相组成的影响.结果 表明:当粉末填料与树脂质量比为1∶1、稀释剂与树脂质量比为1∶2、高温烧结温度为1 500℃时,在Cf/SiC表面可形成致密、结合力强的ZrB2-SiC-B4C涂层.涂层内部相组织均匀,Ra＜1 μm,孔隙率约为4.2％,平均拉伸剪切强度约为5.4MPa.1 500 ℃等温氧化30 h后,有涂层Cf/SiC复合材料的失重率约为10.7％,涂层表面形成了完整的含有ZrO2-SiO2的复合氧化膜,为基体提供了有效的氧化防护.这说明Cf/SiC复合材料表面涂覆ZrB2-SiC-B4C涂层有望满足高温燃流环境的使用要求.

为了提高超高温陶瓷基复合材料的力学性能和耐烧蚀性能,本文采用前驱体浸渍裂解(PIP)工艺制备了C/ZrC-SiC复合材料,研究了锆硅一体化陶瓷前驱体(ZS)的固化-裂解工艺对C/ZrC-SiC复合材料性能的影响.结果 表明:前驱体的裂解温度对复合材料的力学性能影响较大.较高的裂解温度会损坏碳纤维,导致力学性能降低;较低的裂解温度会使碳热还原反应不充分,基体氧含量较高,结构疏松,导致力学性能下降;制备的C/ZrC-SiC复合材料通过了2 850 K的电弧风洞试验考核后线烧蚀率为8.75× 10-4mm/s,呈现出优异的耐烧蚀性能.