In Situ Polymerization of a Self-Healing Polyacrylamide-Based Eutectogel as an Electrolyte for Zinc-Ion Batteries.

Gel electrolytes have attracted extensive attention in flexible batteries. However, the traditional hydrogel electrolyte is not enough to solve the fundamental problems of zinc anodes, such as dendrite growth, side reactions, and freezing failure at temperatures below zero, which seriously restricts the development of zinc-ion batteries. As a flexible energy storage device, the zinc-ion battery inevitably undergoes multiple stretches, bends, folds, or twists in daily use. Here, a self-healing and stretchable eutectogel, designated as deep eutectic solvent-acrylamide eutectic gel (DA-ETG), was developed as a solid-state electrolyte for zinc-ion batteries. This gel was prepared by immobilizing a high-concentration ZnCl2 deep eutectic solvent (DES) into a polyacrylamide matrix through in situ polymerization under ultraviolet light. The eutectogel electrolyte showed exceptional mechanical properties with a maximum fracture strength of 0.6 MPa and a high ionic conductivity of 6.4 × 10-4 S cm-1. The in situ polymerization of the DA-ETG electrolyte in the assembly of a full solid-state zinc-ion battery increased the electrode-electrolyte interface area contact, reduced the ion transport distance between the electrode and electrolyte, minimized the internal resistance, and enhanced the battery's long-term cycling stability. Using the DA-ETG electrolyte, a remarkably high capacity of 580 mAh g-1 at 0.1 A g-1 was achieved by the zinc-ion battery, and a considerable capacity of 234 mAh g-1 was maintained even at 5 A g-1, showing exceptional rate performance. After 2000 cycles at 2 A g-1, the cell with the eutectogel retained a capacity of 85% with a cycling efficiency close to 98%, which demonstrated excellent cycling stability. The self-healing function enabled the prepared soft battery to be reused multiple times, with full contact between the electrode and electrolyte interface, and without device failures.

Nanoparticulate ZrNi: In Situ Disproportionation Effectively Enhances Hydrogen Cycling of MgH2.

High thermal stability and sluggish absorption/desorption kinetics are still important limitations for using magnesium hydride (MgH2) as a solid-state hydrogen storage medium. One of the most effective solutions in improving hydrogen storage properties of MgH2 is to introduce a suitable catalyst. Herein, a novel nanoparticulate ZrNi with 10-60 nm in size was successfully prepared by co-precipitation followed by a molten-salt reduction process. The 7 wt % nano-ZrNi-catalyzed MgH2 composite desorbs 6.1 wt % hydrogen starting from ∼178 °C after activation, lowered by 99 °C relative to the pristine MgH2 (∼277 °C). The dehydrided sample rapidly absorbs ∼5.5 wt % H2 when operating at 150 °C for 8 min. The remarkably improved hydrogen storage properties are reasonably ascribed to the in situ formation of ZrH2, ZrNi2, and Mg2NiH4 caused by the disproportionation reaction of nano-ZrNi during the first de-/hydrogenation cycle. These catalytic active species are uniformly dispersed in the MgH2 matrix, thus creating a multielement, multiphase, and multivalent environment, which not only largely favors the breaking and rebonding of H-H bonds and the transfer of electrons between H- and Mg2+ but also provides multiple hydrogen diffusion channels. These findings are of particularly scientific importance for the design and preparation of highly active catalysts for hydrogen storage in light-metal hydrides.

Quasi-Solid Electrolyte Interphase Boosting Charge and Mass Transfer for Dendrite-Free Zinc Battery.

The practical applications of zinc metal batteries are plagued by the dendritic propagation of its metal anodes due to the limited transfer rate of charge and mass at the electrode/electrolyte interphase. To enhance the reversibility of Zn metal, a quasi-solid interphase composed by defective metal-organic framework (MOF) nanoparticles (D-UiO-66) and two kinds of zinc salts electrolytes is fabricated on the Zn surface served as a zinc ions reservoir. Particularly, anions in the aqueous electrolytes could be spontaneously anchored onto the Lewis acidic sites in defective MOF channels. With the synergistic effect between the MOF channels and the anchored anions, Zn2+ transport is prompted significantly. Simultaneously, such quasi-solid interphase boost charge and mass transfer of Zn2+, leading to a high zinc transference number, good ionic conductivity, and high Zn2+ concentration near the anode, which mitigates Zn dendrite growth obviously. Encouragingly, unprecedented average coulombic efficiency of 99.8% is achieved in the Zn||Cu cell with the proposed quasi-solid interphase. The cycling performance of D-UiO-66@Zn||MnO2 (~ 92.9% capacity retention after 2000 cycles) and D-UiO-66@Zn||NH4V4O10 (~ 84.0% capacity retention after 800 cycles) prove the feasibility of the quasi-solid interphase.

Surface-modified and sulfide electrolyte-infiltrated LiNi0.6Co0.2Mn0.2O2 cathode for all-solid-state lithium batteries.

Sulfide-based all-solid-state lithium batteries (ASSLBs) with high-voltage Ni-rich layered cathodes have shown great potential in energy storage systems. However, the application of ASSLBs is hindered by severe interface issues and poor solid-solid contact between cathodes and sulfide electrolytes. In this work, a suitably thin Li1.5Al0.5Ge1.5(PO4)3 (LAGP) coating (0.41 mS cm-1) is introduced onto the surface of single-crystal LiNi0.6Co0.2Mn0.2O2 particles to mitigate interface side reactions. Subsequently, sheet-type electrodes are fabricated by the infiltration of Li10GeP2S12 to fill the voids and achieve highly dense solid-solid contact, thus preventing contact loss. The Li10GeP2S12-infiltrated ASSLBs with a LAGP buffer layer display a high initial discharge capacity of 141.5 mAh g-1 at 0.05 C and ultrastable cycling for 100 cycles at 0.1 C. An effective fabrication method for highly dense electrodes is proposed in this work, which provides a new direction for scalable industrial production.

Ionic Conductivity Enhancement of Li2ZrCl6 Halide Electrolytes via Mechanochemical Synthesis for All-Solid-State Lithium-Metal Batteries.

Superionic halides have returned to the spotlight of solid electrolytes because of their satisfactory ionic conductivity, soft texture, and stability toward high-voltage electrode materials. Among them, Li2ZrCl6 has aroused interests since abundant Zr element can reduce the cost of large-scale synthesis. However, the related research is very limited, including the detailed parameters during synthesis and the possible strategies for enhancing ionic conductivity. In this work, we have systematically investigated the effects of synthesis parameters on the structure and ionic conductivity of Li2ZrCl6 during the ball-milling annealing process. It is found that mild heat treatment (100 °C) can largely enhance the ionic conductivity of ball-milled electrolytes by 2-3 times, which has not been previously reported. Such enhancement is mainly attributed to the network-like micromorphology composed of nanorods, nanowires, or nanoballs, which is beneficial for lithium ion migration. Finally, the modified Li2ZrCl6 (4.46 × 10-4 S cm-1 @ RT) is also proved to be applicable in LiNi0.8Mn0.1Co0.1O2/ Li2ZrCl6/ Li6PS5Cl/Li-In all-solid-state lithium metal batteries (ASSLMBs). It presents high initial charge capacity of 176.4 mAh g-1 and satisfactory cycle stability since a discharge capacity of 90.8 mAh g-1 is maintained after 40 cycles at 0.1 C. The Li2ZrCl6 electrolytes synthesized via the mechanochemical method is promising to be applied in the high-voltage ASSLMBs, and its ionic conductivity can be enhanced by the strategies provided in our work.

MgCr2O4-Modified CuO/Cu2O for High-Temperature Thermochemical Energy Storage with High Redox Activity and Sintering Resistance.

Metal oxides as high-temperature thermochemical energy storage systems with high energy density based on the gas-solid reaction are a critical demand for the future development of concentrated solar power plants. A copper-based system has high enthalpy change and low cost, but its serious sintering leads to poor reactivity. In this study, MgCr2O4 is decorated on the CuO/Cu2O surface to effectively increase the sintering temperature and alleviate the sintering problem. The re-oxidation degree is increased from 46 to 99.9%, and the reaction time is shortened by 3.7 times. The thermochemical energy density of storage and release reach -818.23 and 812.90 kJ/kg, respectively. After 600 cycles, the oxidation activity remains 98.77%. Material characterization elucidates that nanosized MgCr2O4 is uniformly loaded on the surface of CuO/Cu2O during the reversible reaction, and there is a strong interaction between metal oxides and prompter. Density functional theory (DFT) calculation further confirms that CuO/Cu2O-MgCr2O4 has large binding energy and the formation energy of copper vacancy increases, which can effectively inhibit sintering. The modification mechanism of CuO/Cu2O by MgCr2O4 is revealed, which can provide guidance for the reasonable design of thermochemical energy storage materials with sintering resistance and redox activity.

A Silk Protein-Based Eutectogel as a Freeze-Resistant and Flexible Electrolyte for Zn-Ion Hybrid Supercapacitors.

A eutectogel (ETG) based on immobilizing a zinc salt deep eutectic solvent (DES) in a silk protein backbone is prepared by a coagulating bath method as a solid electrolyte for Zn-ion hybrid supercapacitors (ZHSCs). The Zn salt DES is composed by ethylene glycol (EG), urea, choline chloride (ChCl), and zinc chloride (ZnCl2) with a molar ratio of 6:10:3:3. A strong bonding of the DES liquid to the silk protein backbone is formed between protein macromolecules and the DES due to plenty of hydrogen bonds in both materials. The as-prepared ETG membrane is dense and has no obvious void defects, which possesses a fracture strength of 7.58 MPa and environmental stability. As a solid electrolyte, the ETG membrane exhibits a higher Zn2+ transference number of about 0.60 and a high ionic conductivity (12.31 mS cm-1 at room temperature and 3.63 mS cm-1 at -20 °C). A ZHSC (Zn∥ETG∥C) with the silk protein-based ETG electrolyte is assembled by Zn and active carbon as the anode and the cathode, respectively, which delivers a specific capacitance of 342.8 F g-1 at a current density of 0.2 A g-1 and maintains excellent cycling stability with 80% capacitance retention after 20,000 cycles at a high current rate (5 A g-1) at room temperature. Moreover, the Zn∥ETG∥C device can safely work under a lower temperature of about -18 °C and damaging situations, such as folding states and even cutting tests. The interface evolutions between the Zn anode and the ETG electrolyte are explored, and it was found that a ZnCO3/Zn(CH2OCO2)2 solid electrolyte interphase is in situ formed on the Zn anode, which can inhibit the growth of Zn dendrites. This work provides a new way to fabricate advanced electrolytes for applications in Zn-ion hybrid supercapacitors.

A Novel Ethanol-Mediated Synthesis of Superionic Halide Electrolytes for High-Voltage All-Solid-State Lithium-Metal Batteries.

Halide electrolytes are rising stars among inorganic solid-state electrolytes due to their high ionic conductivity and good compatibility with high-voltage electrodes. However, their traditional synthesis methods including ball-milling annealing are usually energy-intensive and time-consuming compared with liquid-mediated routes. What's more, the only method in aqueous solution is not perfect considering detrimental effect of trace water for battery performances. Here, we propose a novel ethanol-mediated synthesis route for superionic Li3InCl6 electrolyte via energy-friendly dissolution and post-treatment. The organics in ethanol-mediated precursor disappear in form of light gas during post-treatment. And Li3InCl6 with best thermal stability and ionic conductivity (0.79 mS cm-1, 20 °C) can be successfully prepared after postheating for 3 h at 200 °C. Besides, it is also found that the ionic conductivity of Li3InCl6 is positively correlated with peak intensity ratio of (131) plane/(001) plane since crystal plane and preferred orientation can directly affect polyhedrons through which lithium ions migrate in crystalline conductors. The assembled LiNi0.8Co0.1Mn0.1O2/Li3InCl6/Li10GeP2S12/Li-In cell presents high initial charge capacity of 174.8 mAh g-1 at 0.05 C and a good rate performance of 122.9 mAh g-1 at 1 C. Especially, the retention rate of charge capacity can reach 94.8% after 200 cycles. The ethanol-mediated synthesized Li3InCl6 is a novel promising electrolyte which can be coupled with high-voltage cathode for the application of all-solid-state lithium-metal batteries.

Ionic Liquid-Impregnated ZIF-8/Polypropylene Solid-like Electrolyte for Dendrite-free Lithium-Metal Batteries.

Metal-organic framework (MOF)-based solid-like electrolytes have attracted more prospective due to the combined merits of solid-state electrolytes and liquid electrolytes. However, most MOF-based solid-like electrolytes using organic liquid electrolytes cannot fundamentally solve the safety issues of lithium-metal batteries, and the ionic conductivity and mechanical strength of the electrolytes should be further enhanced. Herein, the ionic liquid-impregnated polypropylene (PP) porous membrane with integrally distributed ZIF-8 nanoparticles is designed. The solid-like electrolyte possesses an increased ionic conductivity of 2.09 × 10-4 S cm-1 at 25 °C, lithium-ion transference number (0.45), mechanical strength, electrochemical window, and excellent nanowetted interfaces. Furthermore, the Li symmetrical cell shows excellent Li plating/stripping properties for 550 h at 0.1 mA cm-2 and 0.1 mA h cm-2. The LiFePO4/Li full battery with the solid-like electrolyte demonstrates an excellent rate capability and cycling stability with the initial discharge capacity of 157.9 mA h g-1 and a capacity retention ratio of 91.23% after 450 cycles at 0.2 C. The work offers a new avenue toward MOF-based solid-like electrolytes for high-safety lithium-metal batteries.

Ultrafast Synthesis of I-Rich Lithium Argyrodite Glass-Ceramic Electrolyte with High Ionic Conductivity.

Lithium argyrodites are one of the most promising sulfide electrolytes due to their high ionic conductivity and ductile feature. Among them, Li6 PS5 I (LPSI) exhibits better stability against Li metal but a rather low ionic conductivity (only ≈10-6 S cm-1 ) because of the absence of S2- /I- disorder. Herein, argyrodite Li6- x PS5- x I1+ x glass-ceramic electrolytes with high iodine content are synthesized using ultimate-energy mechanical alloying method. S2- /I- disorder is successfully introduced into the system by doping LiI during this one-pot process. Determined by 6 Li magic angle spinning nuclear magnetic resonance and ab initio molecular dynamics simulations, the introduction of iodine promotes Li+ inter-cage jumps, leading to an enhanced long-range Li+ conducting. The Li5.6 PS4.6 I1.4 glass-ceramic electrolyte (LPSI1.4 -gc) possesses high ionic conductivity (2.04 mS cm-1 ) and excellent stability against Li metal. The Li symmetric cell with the LPSI1.4 -gc electrolyte demonstrates ultralong cycling stability over 3200 h at 0.2 mA cm-2 . LiCoO2 /Li6 PS5 Cl/Li all-solid-state battery applying LPSI1.4 -gc as the anode interlayer also presents prominent cycling and rate performance. This work provides a novel type of electrolyte with high ionic conductivity and stability against Li metal.

Al-Modified CuO/Cu2O for High-Temperature Thermochemical Energy Storage: from Reaction Performance to Modification Mechanism.

Next-generation concentrated solar power plants with high-temperature energy storage requirements stimulate the pursuit of advanced thermochemical energy storage materials. Copper oxide emerges as an attractive option with advantages of high energy density and low cost. But its easy sinterability limits its reversibility and cyclic stability performance. In this work, aluminum-doped copper oxides are synthesized and evaluated via thermogravimetric analysis. The reversibility of Cu-Al oxides reaches 99.5% in the first redox cycle and maintains 81.1% of the initial capacity after 120 cycles. The Al element can modify the CuO particle surface in the form of CuAl2O4, which separates the copper oxide particles from each other during redox cycles to avoid agglomeration and participates in the redox reaction. Through DFT analysis, the introduction of Al is found to increase the formation energy of copper vacancies in copper oxides, which helps avoid the sintering problem and thus improves the oxidation rate. This study provides a generalizable operational mechanism of element doping and can serve as a guideline for the optimization of high-performance materials in thermochemical energy storage.

Single-Crystal-Layered Ni-Rich Oxide Modified by Phosphate Coating Boosting Interfacial Stability of Li10 SnP2 S12 -Based All-Solid-State Li Batteries.

All-solid-state lithium batteries (ASSLBs) adopting sulfide electrolytes and high-voltage layered oxide cathodes have moved into the mainstream owing to their superior safety and immense potential in high energy density. However, the poor electrochemical compatibility between oxide cathodes and sulfide electrolytes remains a challenge for high-performance ASSLBs. In this study, a nanoscale Li1.4 Al0.4 Ti1.6 (PO4 )3 (LATP) phosphate coating is reasonably constructed on the surface of single-crystal LiNi0.6 Co0.2 Mn0.2 O2 particles to achieve cathode/electrolyte interfacial stability. The conformal LATP layer with inherent high-voltage stability can effectively suppress the oxidation decomposition of the electrolyte and demonstrate chemical inertness to both the oxide cathode and Li10 SnP2 S12 electrolyte. ASSLBs with an LATP-modified cathode exhibited a high initial discharge capacity (152.1 mAh g-1 ), acceptable rate capability, and superior cycling performance with a capacity retention of 87.6% after 100 cycles at 0.1 C. Interfacial modification is an effective approach for achieving high-performance sulfide-based ASSLBs with superior interfacial stability.

Heterovalent Cation Substitution to Enhance the Ionic Conductivity of Halide Electrolytes.

Application of halide electrolytes including Li3InCl6 in all-solid-state lithium-metal batteries is still challenging due to the instability with lithium metal and limited ionic conductivity compared with liquid electrolytes and some sulfides. Here, through Zr substitution, a novel Li2.9In0.9Zr0.1Cl6 electrolyte is synthesized through the ball milling and subsequent annealing process. The ionic conductivity of Li2.9In0.9Zr0.1Cl6 (1.54 mS cm-1 at 20 °C) is nearly double that of original Li3InCl6 (0.88 mS cm-1 at 20 °C). Such conductivity enhancement is mainly attributed to the enlarged interplanar spacing and lattice volume, improved concentration of lithium-ion vacancies created by introducing higher-valence Zr4+, and the change of the preferred orientation from the (001) plane to the (131) plane. As a result, the all-solid-state lithium-metal batteries (ASSLMBs) assembled with the Li2.9In0.9Zr0.1Cl6 electrolyte also demonstrate a higher charge/discharge capacity, better cycle stability, and rate performance during cycling without an extra lithium source at the anode side.

Regulating thermochemical redox temperature via oxygen defect engineering for protection of solar molten salt receivers.

An active coating based on thermochemical redox reactions is proposed to protect molten salt receivers from solar flux fluctuation. However, appropriate metal oxides working in the temperature range of 530 and 850°C are still missing. Herein, we put forward an oxygen defect engineering strategy to regulate the thermochemical redox temperatures of perovskites. A tunable temperature range of 426-702°C is obtained by BaCo1-x Mn x O3-δ (x = 0-0.4). It is found that a raised redox temperature can be obtained with the increase of the oxygen vacancy formation energy. For application, BaCo0.8Mn0.2O3-δ is designed as the active protective coating of a lab-scale receiver, which has a thermal capacity of 82.95 kJ kg-1. The smart coating can slow down the temperature rising rate from 8.5°C min-1 to 3°C min-1 in the first 2 min under strong solar radiation, effectively relieving the thermal shock of the receiver.

A Stretchable and Safe Polymer Electrolyte with a Protecting-Layer Strategy for Solid-State Lithium Metal Batteries.

An elastic and safe electrolyte is demanded for flexible batteries. Herein, a stretchable solid electrolyte comprised of crosslinked elastic polymer matrix, poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP), and flameproof triethyl phosphate (TEP) is fabricated, which exhibits ultrahigh elongation of 450%, nonflammability and ionic conductivity above 1 mS cm-1. In addition, in order to improve the interface compatibility between the electrolyte and Li anode and stabilize the solid-electrolyte interphase (SEI), a protecting layer containing poly(ethylene oxide) (PEO) is designed to effectively prevent the anode from reacting with TEP and optimize the chemical composition in SEI, leading to a tougher and more stable SEI on the anode. The LiFePO4/Li cells employing this double-layer electrolyte exhibit an 85.0% capacity retention after 300 cycles at 1 C. Moreover, a flexible battery based on this solid electrolyte is fabricated, which can work in stretched, folded, and twisted conditions. This design of a stretchable double-layer solid electrolyte provides a new concept for safe and flexible solid-state batteries.

Robust Li6PS5I Interlayer to Stabilize the Tailored Electrolyte Li9.95SnP2S11.95F0.05/Li Metal Interface.

All-solid-state lithium-metal batteries (ASSLMBs) with sulfide electrolytes have attracted attention owing to their superior safety and high energy density. However, interfacial instability of sulfide electrolytes against Li metal still hinders their applications. Herein, F-doping is adopted to optimize the structure of Li10SnP2S12. It is demonstrated that the Li9.95SnP2S11.95F0.05 (LSPSF) electrolyte exhibits a high ionic conductivity of 6.4 mS cm-1 because of F-doping, which can reduce the impurity Li2SnS3 and generate Li+ vacancies. In addition, the Li6PS5I (LPSI) glass-ceramic interlayer is employed to enhance the interfacial stability between the sulfide electrolyte and Li metal by restraining the reduction of Sn4+ cations, as indicated by X-ray photoelectron spectroscopy (XPS). As a result, the assembled ASSLMBs with the LPSI interlayer deliver high initial discharge capacity and remarkable cycling stability. This work provides a new design route for manufacturing high-performance ASSLMBs.

Self-Assembled Structure Evolution of MnFe Oxides for High Temperature Thermochemical Energy Storage.

Thermochemical energy storage (TCES) materials have emerged as a promising alternative to meet the high-temperature energy storage requirements of concentrated solar power plants. However, most of the energy storage materials are facing challenges in redox kinetics and cyclic stability. Iron-doped manganese oxide attracts raising attention due to its non-toxicity, low cost, and high energy capacity over 800 °C. However, there are few investigations on the reversibility enhancement of the redox reaction from the microstructural-evolution-mechanism point of view. Herein, bixbyite-type (Mn0.8 Fe0.2 )2 O3 is synthesized and extruded into honeycomb units, which can maintain an 85% initial capacity after 100 redox cycles. It is also found that a self-assembled core-shell MnFe2 O4 @Mn2.7 Fe0.3 O4 structure forms during the reduction step, and then transforms into a homogeneous solid solution of (Mn0.8 Fe0.2 )2 O3 in the following oxidation step. During the reduction step, shells are formed spontaneously from the Mn2.7 Fe0.3 O4 with the MnFe2 O4 as cores due to the lower surface energy, which facilitates the oxygen adsorption and dissociation during subsequent oxidation step. Through the density functional theory calculation, it is revealed that the lower formation energy of oxygen vacancies in the shell contributes to the improvement of oxygen diffusion rate. This study can provide a guideline to design prospective materials for high-temperature TCES.

Porous Composite Gel Polymer Electrolyte with Interfacial Transport Pathways for Flexible Quasi Solid Lithium-Ion Batteries.

The growing demand for safer energy storage devices leads to wide research on solid-state lithium-ion batteries. However, as an important component in the solid-state battery, the solid-state electrolyte often encounters problems, especially the low conductivity at room temperature, inhibiting the development of solid-state batteries. Here, improved electrochemical performances of lithium-ion batteries are obtained by designing a composite gel polymer electrolyte with a sponge-like structure. The porous composite gel polymer electrolyte (PCGPE) is developed by a facile phase inversion process of poly(vinylidiene fluoride-hexafluoropropylene) (PVdF-HFP) and Li6.4La3Zr1.4Ta0.6O12 (LLZTO). The solid-state nuclear magnetic resonance test proves the continuous porous structure constructs fast Li-ion transport pathways on internal interfaces. As a result, the ionic conductivity of PCGPE is up to 5.45 × 10-4 S cm-1 at room temperature. Moreover, an initial capacity of 142.2 mAh g-1 and 82.6% capacity retention at 1 C after 350 cycles are successfully achieved in flexible LiFPO4//PCGPE//Li batteries.

Fluorinated Interface Layer with Embedded Zinc Nanoparticles for Stable Lithium-Metal Anodes.

Lithium-metal batteries are promising candidates for the next-generation energy storage devices. However, notorious dendrite growth and an unstable interface between Li and electrolytes severely hamper the practical implantation of Li-metal anodes. Here, a robust solid electrolyte interphase (SEI) layer with flexible organic components on the top and plentiful LiF together with lithiophilic Zn nanoparticles on the bottom is constructed on Li metal based on the spray quenching method. The fluorinated interface layer exhibits remarkable stability to shield Li from the aggressive electrolyte and restrain dendrite growth. Accordingly, the modified Li electrode delivers a stable cycling for over 400 cycles at 3 mA cm-2 in symmetric cells. An improved capacity retention is also achieved in a full cell with a LiFePO4 cathode. This novel design of the artificial SEI layer offers rational guidance for the further development of high-energy-density lithium-metal batteries.

Porous Polyamide Skeleton-Reinforced Solid-State Electrolyte: Enhanced Flexibility, Safety, and Electrochemical Performance.

The growing demand for safer lithium-ion batteries draws researchers' attention to solid-state electrolytes. In general, a desired electrolyte should be flexible, mechanically strong, and with high ionic conductivity. A solid-state electrolyte with a polymer as a matrix seems to be able to meet these demands. However, a pure polymer electrolyte lacks sufficient strength to suppress Li dendrites, and hybrids with ceramic components often lead to poor flexibility, both far from satisfactory. Herein, a solid-state electrolyte is designed by employing a mass-produced porous polyamide (PA) film infiltrated with polyethylene oxide (PEO)/lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). The PA/PEO/LiTFSI electrolyte is flexible but robust with a Young's modulus of up to 1030 MPa, ensuring steady Li//Li cycling without short circuit for more than 400 h. Also, the porous structure of the PA film decreases the crystalline regions and effectively enhances the ionic conductivity (2.05 × 10-4 S cm-1 at 30 °C). When cycled at 1C, solid-state LiFePO4//Li batteries assembled with the PA/PEO/LiTFSI electrolyte retain 82% capacity after 300 cycles (60 °C). In addition, a flexible LiFePO4//PA/PEO/LiTFSI//Li pouch cell can also work well in harsh operating environments, such as being folded, crimped, and pierced.