Conventional separators applied in lithium batteries face limitations like low porosity, poor electrolyte wettability, lower cation selectivity, and thermal instability, which impact battery performance and safety characteristics. Besides the challenge in separator design, transition metal ion migration from positive electrodes during cycling greatly accelerates capacity fading because of unrestricted diffusion of transition metal cation across the separator. This study explores an innovative strategy for the separator design by incorporating MXene (spraying MXene solution on both sides of the separator), a two-dimensional material, into electrospun Polyacrylonitrile/Polyetherimide membranes with the function of cation selection. Li+ can be accelerated, and its transference number increases along with the anion limitation in the MXene layer. Ni, Co, and Mn ion dissolution from the positive electrode is inhibited due to the cation selectivity of the MXene layer. Leveraging electrospinning advantages, the resultant membranes exhibit high porosity, excellent liquid absorption, mechanical strength, and superior thermal properties. Benefiting from MXene's layered structure and excellent adsorption ability, the membrane significantly inhibits the dissolution of transition metal ions while enabling smooth lithium deposition due to its cation selectivity. Eventually, the Li||NMC811 batteries deliver outstanding cyclic performance (91.3% capacity retention after 200 cycles) and robust lithium dendrite suppression (800 hours of stable cycling). Moreover, the MXene-modified membrane demonstrates exceptional electrolyte wettability, significantly improving ionic transference number (0.67) and conductivity (1.6 mS cm-1). Modification of membrane surfaces with MXene offers insights into addressing transition metal ion migration from the positive electrode material perspective, providing a promising avenue for high-performance LIBs.

High ionic conductivity is the key point in the development of new solid‐state electrolytes. Herein, a combining strategy of anion (O 2− ) doping and structure distortion is applied to enhance the Li + ion conductivity in Li 15 P 4 S 16 Cl 3 , thus converting the nonionic conductor into fast ionic conductor. Solid‐state 6 Li nuclear magnetic resonance analysis shows redistribution of Li + ions in Li 15 P 4 S 16 Cl 3 with O 2− doping or local structure distortion via ball milling, indicating energy changes at different lithium sites. As a result, the activation energy is reduced from 0.50 to 0.35 eV for the ball‐milled Li 15 P 4 S 15.6 O 0.4 Cl 3 , and the ionic conductivity is enhanced from 10 −9 to 10 −4 S cm −1 . The electrochemical stability of Li 15 P 4 S 15.6 O 0.4 Cl 3 is broadened at the anode side as well. The symmetric cell Li|Li 15 P 4 S 15.6 O 0.4 Cl 3 |Li can cycle more than 1000 h with negligible voltage increase. The LiCoO 2 |Li 15 P 4 S 15.6 O 0.4 Cl 3 |Li‐Si all‐solid‐state battery demonstrates an initial capacity of 106 mA h g −1 and retains 92% capacity after 200 cycles at 0.5 C, highlighting excellent rate performance and electrochemical stability.

Metal-organic frameworks (MOFs) offer versatile building blocks for high-performance materials across practical applications. Crystallization studies reveal MOF complex pathways crucial for biological and synthetic systems, yet understanding remains incomplete. Here, we employ in-situ liquid phase transmission electron microscopy (LPTEM) to scrutinize the growth dynamics of ZIF-8 in colloidal environments, aiming to deepen our comprehension of MOF crystallization. This study employs in-situ LPTEM to investigate ZIF-8 nanoparticle growth, revealing the combination of classical and non-classical nucleation processes in the same batch leading a challenge to control nanoparticle morphology and size, while heterogeneous nucleation is dominant giving monodispersed nanoparticle at the presence of ZIF-8 seeds in mother solution. Additionally, integrating MOF-derived carbon materials in lithium-ion batteries (LIBs) faces challenges in achieving high-performance, controllable Ndoping and long-term stability. Ultrafast high-temperature sintering (UHS) is utilized to carbonize ZIF-8, regulating N-doping hard carbon with Zn single atoms doping. Results show optimal morphology at 800 degrees C for 20 s, yielding higher concentration of Zn-doping, higher N-doping levels, and good conductivity compared to conventional sintering in tube furnace. LIB tests demonstrate exceptional cycling performance and stability across wide temperatures. This UHS strategy for ZIF-8 contributes to establishing a balance between Zn-N-doping and the degree of graphitization, thus providing an interdisciplinary approach that offers efficient MOF derivative synthesis for promising wide temperature range applications of LIBs.

Composite solid-state electrolytes (SSEs) can improve the flexibility of the oxide SSEs to decrease the interfacial resistance between the electrolytes and the electrodes. However, the ceramic nanofillers within the composite SSEs suffer from the agglomeration at high concentrations, decreasing the ion conductivities. In this study, a continuous nanocrystal Li6.5La3Zr1.5Ta0.5O12 (LLZTO) skeleton is prepared by the ultrafast high-temperature sintering (UHS) together with tape-casting. Due to the short sintering time of-5 s from precursors, the LLZTO grains are restrained to-300 nm with limited Li loss. Even with trace solvent (3 wt%), the composite SSE membrane exhibits an ion conductivity of 5 x 10-4 S center dot cm- 1,-50 times higher than the DOL electrolyte (1 x 10-5 S center dot cm- 1, 8 wt% solvent), which further proves the high Li-ion conductivity of the nanocrystal LLZTO skeleton. The composite SSE membrane exhibits a critical current density of 3.4 mA center dot cm- 2, among the highest reported values for ceramic-polymer SSEs. The Li/composite SSEs/Li symmetric cells can cycle -120 h at the current density from 0.2 to 0.4 mA center dot cm- 2. The LiFePO4/LLZTO-PEGDA composite SSEs/Li full cell exhibits a high specific discharge capacity of-150 mAh center dot g- 1 for-50 cycles with a Coulombic efficiency of-97%. To explore the processability of the membrane with large size, we also demonstrate a pouch cell (2 cm x 5 cm) with a high specific capacity of-150 mAh center dot g-1 for-25 cycles and a capacity retention of-94.5%. This work paves a new way to manufacture the nanocrystal ceramic SSE skeleton for high energy density all-solid-state batteries.

Garnet-type Li7La3Zr2O12 (LLZO) has high ionic conductivity and good compatibility with lithium metal. High-temperature processing has been proven an effective method to decrease the interface resistance of cathode|LLZO. However, its application is still hindered by the interlayer co-diffusion with the cathode and high sintering temperature (>1200 & DEG;C). In this work, a new garnet-type composite solid-state electrolyte (SSE) Li6.54La2.96Ba0.04Zr1.5Nb0.5O12-LiCoO2 (LLBZNO-LCO) is firstly proposed to improve the chemical stability and electrochemical properties of garnet with high-temperature processing. Small doses of LCO (3%) can significantly decrease the LCO|SSE interface resistance from 121.2 to 10.1 X cm2, while the sintering temperature of garnet-type LLBZNO decreases from 1230 to 1000 & DEG;C. The all-solid-state battery based on the sintered LLBZNO-LCO SSE exhibits excellent cycling stability. Our approach achieves an enhanced LCO|SSE interface and an improved sintering activity of garnet SSE, which provides a new strategy for optimizing the comprehensive performance of garnet SSE.& COPY; 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.

Solid electrolyte membranes face a huge challenge in achieving satisfactory interfacial contact with electrodes, which severely impairs the rate performance and cycle life of solid-state lithium batteries. In this work, we fabricated an ultrathin solid polymer electrolyte (SPE) membrane, and based on it we demonstrated the interfacial contact optimization strategy by in-situ polymerization. The free-stranding PVDF-HFP-LiTFSI membrane with a thickness of 20 mu m shows an ionic conductivity of 1.2 x 10-4 S cm- 1 at room temperature. The poly (ethylene glycol) diacrylate-based in-situ polymerized electrolyte tightly connects the cathode and the SPE membrane, decreasing the interfacial resistance from 9380 Cd cm2 to 1100 Cd cm2. Compared with the traditional method employing liquid electrolyte for interfacial wetting, extended electrochemical window (4.6 V) and much improved thermal stability are obtained. Full cell employing LiFePO4 cathode and lithium metal anode shows an initial capacity of 138.9 mAh g-1 under a charge/discharge rate of 0.5C (85 mA g-1) at 60 degrees C, with a capacity retention ratio of 84.9% and a high average Coulombic efficiency (98.7%) after 300 cycles, remarkably better than those of its liquid electrolyte-used counterpart. Our work demonstrates that the application of in-situ polymerization into interfacial contact improvement between SPE and cathode possesses wide application prospects.

Silica glasses have wide applications in industrial fields due to their extraordinary properties, such as high transparency, low thermal expansion coefficient, and high hardness. However, current methods of fabricating silica glass generally require long thermal treatment time (up to hours) and complex setups, leading to high cost and slow manufacturing speed. Herein, to obtain high-quality glasses using a facile and rapid method, an ultrafast high-temperature sintering (UHS) technique is reported that requires no additional pressure. Using UHS, silica precursors can be densified in seconds due to the large heating rate (up to 102 K s-1 ) of closely placed carbon heaters. The typical sintering time is as short as ≈10 s, ≈1-3 orders of magnitude faster than other methods. The sintered glasses exhibit relative densities of > 98% and high visible transmittances of ≈90%. The powder-based sintering process also allows rapid doping of metal ions to fabricate colored glasses. The UHS is further extended to sinter other functional glasses such as indium tin oxide (ITO)-doped silica glass, and other transparent ceramics such as Gd-doped yttrium aluminum garnet. This study demonstrates an UHS proof-of-concept for the rapid fabrication of high-quality glass and opens an avenue toward rapid discovery of transparent materials.

One of the major challenges in the development of micro-combustors is heat losses that result in flame quenching, and reduced combustion efficiency and performance. In this work, a novel thermal barrier coating (TBC) using hexagonal boron nitride (h-BN) nanosheets as building blocks was developed and applied to a Swiss roll micro-combustor for determining its heat losses with increased temperatures inside the combustor that contributes to improved performance. It was found that by using the h-BN TBC, the combustion temperature of the micro-combustor increased from 850 K to 970 K under the same thermal loading and operational conditions. This remarkable temperature increase using the BN TBC originated from its low cross-plane thermal conductivity of 0.4 W m(-1) K(-1)to mitigate the heat loss from the micro-combustor plates. Such a low thermal conductivity in the h-BN TBC is attributed to its interfacial resistance between the nanosheets. The development of h-BN TBC provides an effective approach to improve thermal management for performance improvements of gas turbine engines, rocket engines, and all various kinds of micro-combustors.

Solid‐state batteries (SSBs) promise better safety and potentially higher energy density than the conventional liquid‐ or gel‐based ones. In practice, the implementation of SSBs often necessitates 3D porous scaffolds made by ceramic solid‐state electrolytes (SSEs). Herein, a general and facile method to sinter 3D porous scaffolds with a range of ceramic SSEs on various substrates at high temperature in seconds is reported. The high temperature enables rapid reactive sintering toward the desired crystalline phase and expedites the surface diffusion of grains for neck growth; meanwhile, the short sintering duration limits the coarsening, thus accurately controlling the degree of densification to preserve desired porous structures, as well as reducing the loss of volatile elements. As a proof‐of‐concept, a composite SSE with a good ionic conductivity (i.e., ≈1.9 × 10 −4 S cm −1 at room temperature) is demonstrated by integrating poly(ethylene oxide) with the 3D porous Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 scaffold sintered by this method. This method opens a new door toward sintering a variety of ceramic‐SSE‐based 3D scaffolds for all‐solid‐state battery applications.

Powder to bulk processes, such as additive manufacturing and metal injection molding (MIM), have enabled great potential for complex metal designing and manufacturing. However, additive manufacturing process normally introduces a high residue stress and textures due to the locally intense temperature. MIM is an excellent batch manufacturing process; nevertheless, it is not suitable for rapid screening and development of new metal compositions and structures due to the slow sintering process. Herein, an ultrafast high‐temperature sintering (UHS) process is reported that enables the rapid synthesis and sintering of bulk metals/alloys and intermetallic compounds. In this process, elemental powders are mixed and pressed into pellets, followed by UHS sintering in just seconds at a temperature between 1000 and 3000 °C. Three representative compositions, including pure metals, intermetallics, and multielement alloys, are demonstrated with a broad range of melting points. The UHS process for metal sintering is nonmaterials specific, in addition to being extremely rapid, which make it suitable for materials discovery. Furthermore, the sintering method does not apply pressure to the samples, making it compatible with 3D printing and other additive manufacturing processes of complex structures. This rapid sintering technique will greatly facilitate the development and manufacturing of metals and alloys.

Ceramics are an important class of materials with widespread applications because of their high thermal, mechanical, and chemical stability. Computational predictions based on first principles methods can be a valuable tool in accelerating materials discovery to develop improved ceramics. It is essential to experimentally confirm the material properties of such predictions. However, materials screening rates are limited by the long processing times and the poor compositional control from volatile element loss in conventional ceramic sintering techniques. To overcome these limitations, we developed an ultrafast high-temperature sintering (UHS) process for the fabrication of ceramic materials by radiative heating under an inert atmosphere. We provide several examples of the UHS process to demonstrate its potential utility and applications, including advancements in solid-state electrolytes, multicomponent structures, and high-throughput materials screening.

The discovery of new solid-state electrolytes (SSEs) can be guided by computation for next-generation Li batteries toward higher energy density and better safety. However, conventional synthetic methods often suffer from severe loss of Li and poor material quality, therefore preventing the promise of the predicted SSE candidates to be realized. In this study, computationally predicted SSEs with desirable material quality are synthesized via an ultrafast sintering technique. Three new garnet-type Li+ conductors, including Li6.5 Nd3 Zr1.5 Ta0.5 O12 (LNZTO), Li6.5 Sm3 Zr1.5 Ta0.5 O12 (LSZTO), and Li6.5 (Sm0.5 La0.5 )3 Zr1.5 Ta0.5 O12 (L-LSZTO), are screened by density functional theory to exhibit good synthesizability and stability. The ultrafast sintering method by Joule heating effectively shorten the sintering time from several hours to <25 s, thereby reducing the Li loss and effectively merging the grains toward high material quality. In agreement with the computational prediction, LNZTO demonstrates the best synthesizability and phase stability, thereby achieving the highest conductivity of 2.3 × 10-4 S cm-1 among the three new SSE candidates. Using a current density of 0.2 mA cm-2 , the Li/LNZTO/Li symmetric cell can cycle for ≈90 h without obvious increase of overpotentials. This study showcases the successful realization of computational predictions by the ultrafast sintering technique for the rapid optimization and screening of high-performance SSEs.

Electric conductors are ubiquitously used for electromagnetic shielding, flexible electronics, and energy storage, with metals and carbon-based compounds as traditional choices for these applications. Here, we develop a conductive wood as a new type of structural electromagnetic interference (EMI) shielding material with combined load-bearing function via delignification and subsequent in situ chemical vapor deposition of polypyrrole (PPy) inside the wood channels. The centimeter-long wood channels are well coated by a layer of interconnected PPy, which provides a high electrical conductivity of 39 S m(-1). Our results demonstrate that 3.5 cm thick conductive wood displays an EMI shielding effectiveness of similar to 58 dB. Moreover, the conductive wood inherits the advanced mechanical strength of natural wood via the carbonization-free process, as the compressive and tensile strengths of the conductive wood are about 3- and 28.7-times higher than those of conventional carbonized wood materials, respectively. This study may pave the way for structural EMI shielding applications using scalable, renewable, and cost-effective biomaterials. Its remarkable advantages, including uniform electrical conductivity, outstanding compressive strength, a controllable material thickness of up to several centimeters, as well as its lightweight and sustainability, ensure strong potential for applications in next-generation structural materials.

Garnet-based solid-state electrolytes (SSEs) are attractive for solid-state lithium metal batteries due to their wide electrochemical window, high conductivity, and excellent stability against lithium metal. However, the risk of short-circuit encumbers the cycle life and capacity of garnet-based solid-state batteries without clear reason or mechanism. Here, reversible short-circuit behavior in the garnet-based solid-state batteries, which differs from the short-circuit in liquid cells, is reported for the first time. In situ neutron depth profiling is adopted to quantitatively measure Li transport, which helps forecast and confirm the reversible nature of the short-circuit in garnet-based batteries. A real-time Li accumulation monitoring system of NMC//CNT/garnet/Li cell is designed to reveal the Li dendrite formation mechanism. The voltage drops of the CNT monitoring electrode during the charging process indicate the formation of Li dendrites inside the garnet bulk, while the smooth voltage profile during the discharging process demonstrates the disappearance of the short-circuit. This is the first confirmation of short-circuit behavior that provides clarification of the Li dendrite formation mechanism in garnet-based solid-state batteries, which is shown to be a reversible process caused by the low ionic conductivity and non-negligible electronic conductivity of garnet SSEs.

A solution-based printing and sintering technique is developed to fabricate a range of high-performance ceramic thin films.

Solid-state lithium batteries using inorganic electrolytes are expected to revolutionize energy storage systems due to their better safety and high energy density. However, their application is greatly hindered by the poor solid-solid interface between the solid-state electrolyte (SSE) and electrodes, particularly the cathode. Herein, we report a facile strategy to address the high cathode/SSE interfacial resistance through rapid, high-temperature microwave soldering. As a proof-of-concept demonstration, we soldered a garnet-type Li7La3Zr2O12 (LLZO) SSE with a V2O5 cathode, which feature high thermal stability and suitable melting temperatures. Our microwave soldering technique can selectively melt the surface of the granular V2O5 and rapidly form an intact and continuous cathode layer with tightly embedded carbon black nanoparticles, leading to a remarkable 690-time increase of the electronic conductivity of cathode. Additionally, the melted V2O5 cathode is conformally soldered to the garnet electrolyte, resulting in a 28-fold decrease of the cathode/garnet interfacial resistance (from 14.4 k Omega cm(2) to 0.5 k Omega cm(2). As a result, this all-solid-state full cell displays a low overall resistance of 0.3 k Omega cm(2) at 100 degrees C, which enables stable cyclability of the battery without the addition of liquid/polymer electrolyte. The fast microwave soldering strategy constitutes a significant step towards the development of the all-solid-state batteries.

Fire retardant coatings have been proven effective at reducing the heat release rate (HRR) of structural materials during burning; yet effective methods for increasing the ignition temperature and delay time prior to burning are rarely reported. Herein, a strong, fire-resistant wood structural material is developed by combining a densification treatment with an anisotropic thermally conductive flame-retardant coating of hexagonal boron nitride (h-BN) nanosheets to produce BN-densified wood. The thermal management properties created by the BN coating provide fast, in-plane thermal diffusion, slowing the conduction of heat through the densified wood, which improves the material's ignition properties. Compared with densified wood without the BN coating, a 41 degrees C enhancement in ignition temperature (T-ig), a twofold increase in ignition delay time (t(ig)), and a 25% decrease in the maximum HRR of BN-densified wood can be achieved. As a proof of concept for scalability, the pieces of the BN-densified wood are fabricated with a length larger than 25 cm, width greater than 15 cm, and thickness more than 7 mm. The improved thermal management, fire resistance, mechanical strength, and scalable production of BN-densified wood position it as a promising structural material for safe and energy-efficient buildings.

High-capacity electrode materials are indispensable for developing high energy density solid-state batteries. The lithium metal anode is attractive because of its high capacity and low electrochemical reduction potential, but its application is hampered by the dendrite issue. The silicon anode is a promising material having high capacity and invulnerability to undergoing dendrite formation, but is limited to the nanometer regime for the thickness of a Si anode. Herein, for the first time, we demonstrate a 1 mu m thick solid-state silicon anode (10 times the typical thickness of Si anodes used in organic electrolyte) as an alternative to Li metal anode for solid-state batteries. This Si anode forms good contact with the garnet-type solid-state electrolyte and maintains structural integrity during the Li ion intercalation and extraction. The Si anode with the garnet electrolyte exhibits a high discharge capacity of 2685 mA h g(-1) and an excellent initial Coulombic efficiency of 83.2%, higher than that of the Si anodes with an organic electrolyte (77.1%). Our mechanics modeling reveals that the strong nanomechanical constraints by the solid garnet electrolyte enables the substantial increase in the critical thickness of the Si anode from just nanometers to micrometers, toward high-capacity solid-state batteries.

Surface contamination and degradation are two main issues leading to performance decay of ceramic-based solid-state electrolytes (SSEs). The typical strategies used to clean surface contaminants and restore ceramic materials involve mechanical polishing or high temperature thermal treatment. However, mechanical polishing can cause other side reactions and cannot clean contaminants on the grain boundaries of SSEs, while conventional thermal treatment using a furnace is often energy-and time-intensive, as the heating and cooling processes are slow. In this work, we for the first time demonstrate a high temperature thermal pulse technique for rapid ceramic surface processing. As a demonstration, we cleaned a garnet-based Li conductive SSE featuring lithium carbonate surface contamination in less than 2 s. The thermal pulsed garnet SSE exhibits an improved ionic conductivity of 3.2 x 10(-4) S/cm-a two-fold increase compared to the starting material. Symmetric cells featuring the thermal pulsed garnet SSE can cycle at current densities up to 500 mu A/cm(2), while control cells short-circuit at a current density of 100 mu A/cm(2).

Thin films of several microns in thickness are ubiquitously used in packaging, electronics, and acoustic sensors. Here we demonstrate that natural wood can be directly converted into an ultrathin film with a record-small thickness of less than 10 μm through partial delignification followed by densification. Benefiting from this aligned and laminated structure, the ultrathin wood film exhibits excellent mechanical properties with a high tensile strength of 342 MPa and a Young’s modulus of 43.6 GPa, respectively. The material’s ultrathin thickness and exceptional mechanical strength enable excellent acoustic properties with a 1.83-times higher resonance frequency and a 1.25-times greater displacement amplitude than a commercial polypropylene diaphragm found in an audio speaker. As a proof-of-concept, we directly use the ultrathin wood film as a diaphragm in a real speaker that can output music. The ultrathin wood film with excellent mechanical property and acoustic performance is a promising candidate for next-generation acoustic speakers.