Copious Dislocations Defect in Amorphous/Crystalline/Amorphous Sandwiched Structure P-NiMoO4 Electrocatalyst toward Enhanced Hydrogen Evolution Reaction.

The design and synthesis of efficient, inexpensive, and long-term stable heterostructured electrocatalysts with high-density dislocations for hydrogen evolution reaction in alkaline media and seawater are still a great challenge. An amorphous/crystalline/amorphous sandwiched structure with abundant dislocations were synthesized through thermal phosphidation strategies. The dislocations play an important role in the hydrogen evolution reactions. Copious dislocation defects, combined with cracks, and the synergistic interfacial effect between crystalline phase and amorphous phase regulate the electronic structure of electrocatalyst, provide more active sites, and thus endow the electrocatalysts with excellent catalytic activity under alkaline water and seawater. The overpotentials of P-NiMoO4 at 10 mA/cm2 in 1 M KOH aqueous solution and seawater are 45 and 75 mV, respectively. Additionally, the P-NiMoO4 electrocatalyst exhibits long-term stability over 100 h. This study provides a simple approach for synthesizing amorphous/crystalline/amorphous sandwiched non-noble-metal electrocatalysts with abundant dislocations for hydrogen evolution reaction.

Porous N-Doped Carbon Decorated with Atomically Dispersed Independent Dual Metal Sites from Energetic Zeolite Imidazolate Frameworks as Bidirectional Catalysts for Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries have ultrahigh theoretical specific capacity and energy density, which are considered to be very promising energy storage devices. However, the slow redox kinetics of polysulfides are the main reason for the rapid capacity decay of Li-S batteries. A reasonable electrocatalyst for the Li-S battery should reduce the reaction barrier and accelerate the reaction kinetics of the bidirectional catalytic conversion of lithium polysulfides (LiPSs), thereby reducing the cumulative concentration of LiPSs in the electrolyte. In this report, porous N-doped carbon nanofibers decorated with independent dual metal sites as catalysts for Li-S batteries were fabricated in one step using a fusion-foaming method. Experimental and theoretical analyses demonstrate that the synergistic effect of independent dual metal sites provides strong LiPS affinity, improved electronic conductivity, and enhanced redox kinetics of polysulfides. Therefore, the assembled Li-S battery exhibits high rate performance (discharge specific capacity of 771 mA h g-1 at 2C) and excellent cycle stability (capacity decay rate of 0.51% after 1000 cycles at 1C).

Three-dimensional carbon network-supported black phosphorus-cobalt heterojunctions: An efficient electrocatalyst for high-rate oxygen evolution.

Black phosphorus (BP), as a burgeoning two-dimensional material, has shown good electrocatalytic activity due to its unique electronic structure and abundant active sites.However, the presence of lone pair electrons in black phosphorus leads to its poor stability and rapid degradation in an oxygen/water environment, which greatly limits its practical application. Herein, BP-Co heterojunctions were synthesized on carbon nanotube@nitrogen-doped carbon (BP-Co/CNT@NC) by the pyrolysis of ZnCo-zeolitic imidazolate frameworks and subsequent solvothermal treatment. The BP-Co Schottky junction improved the electrocatalytic stability of BP, modulated its electronic structure, improved its conductivity and electron transfer during the electrocatalytic reaction. Density functional theory calculation was used to confirm the electron transfer and redistribution at the interface between BP and Co, which constructed an oppositely charged region and formed a strong built-in field. Energy band configuration analysis revealed a narrowed band gap because of the formation of BP-Co Schottky junction. Consequently, the optimized BP-Co/CNT@NC exhibited a superior oxygen evolution reaction (OER) performance, a low overpotential of 370 mV@100 mA/cm2, with a small Tafel slope of 40 mV/dec and good long-term stability. Particularly, the catalyst has an excellent OER performance at the high current density of 100-400 mA/cm2. This strategy improves the stability of BP electrocatalysts and strengthens their utilization in electrocatalytic applications.

Room-Temperature Laser Planting of High-Loading Single-Atom Catalysts for High-Efficiency Electrocatalytic Hydrogen Evolution.

Despite stunning progress in single-atom catalysis (SAC), it remains a grand challenge to yield a high loading of single atoms (SAs) anchored on substrates. Herein, we report a one-step laser-planting strategy to craft SAs of interest under an atmospheric temperature and pressure on various substrates including carbon, metals, and oxides. Laser pulses render concurrent creation of defects on the substrate and decomposition of precursors into monolithic metal SAs, which are immobilized on the as-produced defects via electronic interactions. Laser planting enables a high defect density, leading to a record-high loading of SAs of 41.8 wt %. Our strategy can also synthesize high-entropy SAs (HESAs) with the coexistence of multiple metal SAs, regardless of their distinct characteristics. An integrated experimental and theoretical study reveals that superior catalytic activity can be achieved when the distribution of metal atom content in HESAs resembles the distribution of their catalytic performance in a volcano plot of electrocatalysis. The noble-metal mass activity for a hydrogen evolution reaction within HESAs is 11-fold over that of commercial Pt/C. The laser-planting strategy is robust, opening up a simple and general route to attaining an array of low-cost, high-density SAs on diverse substrates under ambient conditions for electrochemical energy conversion.

Stabilizing Solid-state Lithium Metal Batteries through In Situ Generated Janus-heterarchical LiF-rich SEI in Ionic Liquid Confined 3D MOF/Polymer Membranes.

Pursuing high power density lithium metal battery with high safety is essential for developing next-generation energy-storage devices, but uncontrollable electrolyte degradation and the consequence formed unstable solid-electrolyte interface (SEI) make the task really challenging. Herein, an ionic liquid (IL) confined MOF/Polymer 3D-porous membrane was constructed for boosting in situ electrochemical transformations of Janus-heterarchical LiF/Li3 N-rich SEI films on the nanofibers. Such a 3D-Janus SEI-incorporated into the separator offers fast Li+ transport routes, showing superior room-temperature ionic conductivity of 8.17×10-4  S cm-1 and Li+ transfer number of 0.82. The cryo-TEM was employed to visually monitor the in situ formed LiF and Li3 N nanocrystals in SEI and the deposition of Li dendrites, which is greatly benefit to the theoretical simulation and kinetic analysis of the structural evolution during the battery charge and discharge process. In particular, this membrane with high thermal stability and mechanical strength used in solid-state Li||LiFePO4 and Li||NCM-811 full cells and even in pouch cells showed enhanced rate-performance and ultra-long life spans.

Sulfur-deficient MoS2-carbon hollow nanospheres for synergistic trapping and electrocatalytic conversion of polysulfides.

Lithium-sulfur battery is one of the most promising candidates for next-generation energy storage systems, but the serious shuttle effect and sluggish reaction kinetics of polysulfides impair its practical applications. Herein, sulfur-deficient MoS2/carbon hollow nanospheres (MoS2-CHNs) are firstly synthesized by a NaCl-template pyrolysis and employed as sulfur host for lithium-sulfur batteries. TEM analysis reveals that carbon hollow nanospheres existing in the composite are the backbones that help to immobilize the ultrathin MoS2 nanosheets and ensure their large specific surface area. The MoS2 nanosheets consist of 5-10 layers of MoS2 with rich sulfur vacancies. The first principle calculation demonstrates that sulfur vacancy led to an intensively enhanced binding energy (-4.70 eV) towards Li2S6 compared to the pristine MoS2 (-1.57 eV). It suppressed the shuttle effect efficiently. The catalytic experiments reveal that MoS2-CHNs have a superior ability for the nucleation of Li2S and bidirectional electrocatalytic capability for the conversion of polysulfide. The large storage space inside MoS2-CHNs can work as a reservoir for intermediate polysulfides to substantially reduce the concentration overpotential. Due to this advantageous structural design of MoS2-CHNs electrode, its reversible capacity remains 1139 mAh g-1 after 100 cycles at 0.2C, and 600 mAh g-1 after 500 cycles at 5C with a sulfur loading of 5 mg cm-2. Even though the sulfur loading increases to 10 mg cm-2, the Li-S battery delivers a stable capacity of 978 mAh g-1 after 50 cycles at 0.2C. So the MoS2-CHNs demonstrate a promising application for high-energy Li-S batteries.

Chemical Energy-Driven Lithiation Preparation of Defect-Rich Transition Metal Nanostructures for Electrocatalytic Hydrogen Evolution.

Transition metal nanostructures are widely regarded as important catalysts to replace the precious metal Pt for hydrogen evolution reaction (HER) in water splitting. However, it is difficult to obtain uniform-sized and ultrafine metal nanograins through general high-temperature reduction and sintering processes. Herein, a novel method of chemical energy-driven lithiation is introduced to synthesize transition metal nanostructures. By taking advantage of the slow crystallization kinetics at room temperature, more surface and boundary defects can be generated and remained, which reduce the atomic coordination number and tune the electronic structure and adsorption free energy of the metals. The obtained Ni nanostructures therein exhibit excellent HER performance. In addition, the bimetal of Co and Ni shows better electrocatalytic kinetics than individual Ni and Co nanostructures, reaching 100 mA cm-2 at a low overpotential of 127 mV. The high HER performance originates from well-formed synergistic effect between Ni and Co by tuning the electronic structures. Density functional theory simulations confirm that the bimetallic NiCo possesses a low Gibbs free energy of hydrogen adsorption, which are conducive to enhance its intrinsic activity. This work provides a general strategy that enables simultaneous defect engineering and electronic modulation of transition metal catalysts to achieve an enhancement in HER performance.

Zero-Strain High-Capacity Silicon/Carbon Anode Enabled by a MOF-Derived Space-Confined Single-Atom Catalytic Strategy for Lithium-Ion Batteries.

Developing zero-strain electrode materials with high capacity is crucial for lithium-ion batteries (LIBs). Here, a new zero-strain composite material made of ultrasmall Si nanodots (NDs) within metal organic framework-derived nanoreactors (Si NDs⊂MDN) through a novel space-confined catalytic strategy is reported. The unique Si NDs⊂MDN anode features a low strain (<3%) and a high theoretical lithium storage capacity (1524 mAh g-1 ) which far surpasses the traditional single-crystal counterparts that suffer from a low capacity delivery. The zero-strain property is evidenced by substantial characterizations including ex/in situ transmission electron microscopy and mechanical simulations. The Si NDs⊂MDN exhibits superior cycling stability and high reversible capacity (1327 mAh g-1 at 0.1 A g-1 after 100 cycles) in half-cells and high energy density (366 Wh kg-1 after 300 cycles) in a full cell. This study reports a new catalog of zero-strain electrode material with significantly improved capacity beyond the traditional single-crystal zero-strain materials.

FeNi2P three-dimensional oriented nanosheet array bifunctional catalysts with better full water splitting performance than the full noble metal catalysts.

The 3D (three-dimensional) oriented nanosheet array FeNi2P electrocatalyst grown on carbon cloth (FeNi2P/CC) is explored in this work. This unique 3D oriented nanosheet array structure can expose more catalytic active sites, promote the penetration of electrolyte solution on the catalyst surface, and facilitate the transfer of ions, thus speeding up the kinetic process of Hydrogen evolution reaction (HER) and Oxygen evolution reaction (OER). At the current densities of 10 mA/cm2 in 1 M KOH solution, the HER overpotential (71 mV) of the FeNi2P/CC self-supporting electrode is very close to that of noble metal HER catalyst of 20% Pt/C (54 mV), and its OER overpotential (210 mV) is 34% lower than that of the precious metal OER catalyst of RuO2 (318 mV), demonstrating the excellent electrocatalytic performance of the FeNi2P/CC catalyst. Moreover, the cell voltage for full water splitting (at 10 mA/cm2 current densities) of the FeNi2P/CC bifunctional electrode cell is 1.52 V, which is 3.8% lower than that of the full noble-metal electrode reference cell (RuO2 || Pt/C, 1.58 V), suggesting that this FeNi2P/CC bifunctional catalyst is likely to replace precious metals to reduce the costs in full water splitting application. According to density functional theory (DFT) calculation results, the introduction of iron atom can change the electronic structure of the Ni2P, so it can reduce the adsorption energy of hydrogen and oxygen, and facilitate the adsorption and desorption of hydrogen and oxygen on the surface of the catalyst, improving its performance of HER and OER.

Mo/P Dual-Doped Co/Oxygen-Deficient Co3O4 Core-Shell Nanorods Supported on Ni Foam for Electrochemical Overall Water Splitting.

The exploration for low-cost bifunctional materials for highly efficient overall water splitting has drawn profound research attention. Here, we present a facile preparation of Mo-P dual-doped Co/oxygen-deficient Co3O4 core-shell nanorods as a highly efficient electrocatalyst. In this strategy, oxygen vacancies are first generated in Co3O4 nanorods by lithium reduction at room temperature, which endows the materials with bifunctional characteristics of the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER). A Co layer doped with Mo and P is further deposited on the surface of the Co3O4-x nanorods to enhance the electrocatalytic hydrolysis performance. As a result, the overpotentials of HER and OER are only 281 and 418 mV at a high current density of 100 mA cm-2 in 1.0 M KOH, respectively. An overall water electrolytic cell using CoMoP@Co3O4-x nanorods as both electrodes can reach 10 mA cm-2 at 1.614 V with outstanding durability. The improvement is realized by the synergistic effect of oxygen vacancies, Mo/P doping, and core-shell heterostructures for modulating the electronic structure and producing more active sites, which suggests a promising method for developing cost-effective and stable electrocatalysts.

Multifunctional Protection Layers via a Self-Driven Chemical Reaction To Stabilize Lithium Metal Anodes.

The Li metal anode is considered one of the most potential anodes due to its highest theoretical specific capacity and the lowest redox potential. However, the scalable preparation of safe Li anodes remains a challenge. In the present study, a LiF-rich protection layer has been developed using self-driven chemical reactions between the Li3xLa2/3-xTiO3/polyvinylidene fluoride/dimethylacetamide (LLTO/PVDF/DMAc) solution and the Li metal. After coating the LLTO/PVDF/DMAc solution to Li foil, PVDF reacted with Li spontaneously to form LiF, and the accompanying Ti4+ ions (in LLTO) were reduced to Ti3+ to form a mixed ionic and electronic conductor LixLLTO. The protective layer can redistribute the Li-ion transport, regulate the even Li deposition, and inhibit the Li dendrite growth. When paired with LiFePO4, NCM811, and S cathodes, the batteries have demonstrated excellent capacity retention and cycling stability. More importantly, a volumetric energy density of 478 Wh L-1 and 78% capacity retention after 310 cycles have been achieved by using a S/LixLLTO-Li pouch cell. This work provides a feasible avenue to provide large-scale preparation of safe Li anodes for the next-generation pouch-type Li-S batteries as ideal power sources for flexible electronic devices.

A dual-phase alloy with ultrahigh strength-ductility synergy over a wide temperature range.

High-entropy alloys (HEAs), as an emerging class of materials, have pointed a pathway in developing alloys with interesting property combinations. Although they are not exempted from the strength-ductility trade-off, they present a standing chance in overcoming this challenge. Here, we report results for a precipitation-strengthening strategy, by tuning composition to design a CoNiV-based face-centered cubic/B2 duplex HEA. This alloy sustains ultrahigh gigapascal-level tensile yield strengths and excellent ductility from cryogenic to elevated temperatures. The highest specific yield strength (~150.2 MPa·cm3/g) among reported ductile HEAs is obtained. The ability of the alloy presented here to sustain this excellent strength-ductility synergy over a wide temperature range is aided by multiple deformation mechanisms i.e., twins, stacking faults, dynamic strain aging, and dynamic recrystallization. Our results open the avenue for designing precipitation-strengthened lightweight HEAs with advanced strength-ductility combinations over a wide service temperature range.

Constructing anatase TiO2/Amorphous Nb2O5 heterostructures to enhance photocatalytic degradation of acetaminophen and nitrogen oxide.

TiO2 nanostructures have been one of the most explored metal oxides photocatalysts to apply for environmental remediation. However, its wide band gap results in the underutilization of sunlight for degradation of pollutants. In order to overcome this handicap, the synthesis of TiO2-based composite has brought extraordinary materials. In this study, we design and prepare TiO2/Nb2O5 heterostructures with different molar ratios by using peroxotitanium and peroxoniobium complex as precursors in aqueous solution. The TiO2 exists in the form of anatase while Nb2O5 is amorphous in the composite, leading to a special crystalline TiO2/amorphous Nb2O5 heterostructures. In particular, Nb element is also doped and Ti3+ ions are formed in the TiO2 lattice, leading to a reduced band gap. The unique TiO2/0.25Nb2O5 (Ti:Nb = 2:1) heterostructures can effectively suppress the recombination of photogenerated electrons and holes, and facilitate the charge transfer, resulting in the optimum photocatalytic performance. The nitrogen oxide removal efficiency by TiO2/0.25Nb2O5 is 77.23% in visible light, which is 3.8-folds and 7.0-folds higher than pure TiO2 and Nb2O5. Photocatalytic degradation of acetaminophen by TiO2/0.25Nb2O5 is 90.6% in visible light, which is approximately 2.5-folds higher than pure TiO2 and Nb2O5.

B and cyano groups co-doped g-C3N4 with multiple defects for photocatalytic nitrogen fixation in ultrapure water without hole scavengers.

B atoms and cyano groups co-doped graphite carbon nitride with nitrogen vacancies (VN-BC-CN) was explored via one-step in-situ route. A series of comprehensive experiments confirmed that B atoms and cyano groups had been doped into the framework of graphite carbon nitride, forming VN-BC-CN catalyst sample with a large number of nitrogen-vacancy defects. As electron acceptors, B and cyano groups could be used as active sites for nitrogen conversion. The defect level caused by nitrogen vacancy led to red shift of the light absorption edge, which resulted in higher separation efficiency of photo-induced carriers and faster transfer rate of photo-induced electrons for the VN-BC-CN catalyst. This VN-BC-CN catalyst had good photocatalytic nitrogen fixation performance in the ultrapure water without any hole-scavengers. The nitrogen photofixation rate of VN-BC-CN (115.53 µmol g-1 h-1) was 25.5 times that of pure carbon nitride (GCN, 4.53 µmol g-1 h-1). Moreover, NH4+ generation rate hardly decreased after 10 h reaction, and the NH4+ generation rate could reach 79.56 µmol g-1 h-1 in the fifth cycle, showing the good photocatalytic stability of the VN-BC-CN catalyst.

The Ghd7 transcription factor represses ARE1 expression to enhance nitrogen utilization and grain yield in rice.

The genetic improvement of nitrogen use efficiency (NUE) of crops is vital for grain productivity and sustainable agriculture. However, the regulatory mechanism of NUE remains largely elusive. Here, we report that the rice Grain number, plant height, and heading date7 (Ghd7) gene genetically acts upstream of ABC1 REPRESSOR1 (ARE1), a negative regulator of NUE, to positively regulate nitrogen utilization. As a transcriptional repressor, Ghd7 directly binds to two Evening Element-like motifs in the promoter and intron 1 of ARE1, likely in a cooperative manner, to repress its expression. Ghd7 and ARE1 display diurnal expression patterns in an inverse oscillation manner, mirroring a regulatory scheme based on these two loci. Analysis of a panel of 2656 rice varieties suggests that the elite alleles of Ghd7 and ARE1 have undergone diversifying selection during breeding. Moreover, the allelic distribution of Ghd7 and ARE1 is associated with the soil nitrogen deposition rate in East Asia and South Asia. Remarkably, the combination of the Ghd7 and ARE1 elite alleles substantially improves NUE and yield performance under nitrogen-limiting conditions. Collectively, these results define a Ghd7-ARE1-based regulatory mechanism of nitrogen utilization, providing useful targets for genetic improvement of rice NUE.

Organic molecule confinement reaction for preparation of the Sn nanoparticles@graphene anode materials in Lithium-ion battery.

Sn@Graphene composites as anode materials in Lithium-ion batteries have attracted intensive interest due to the inherent high capacity. On the other side, the high atomic ratio (Li4.4Sn) induces the pulverization of the electrode with cycling. Thus, suppressing pulverization by designing the structure of the materials is an essential key for improving cyclability. Applying the nanotechnologies such as electrospinning, soft/hard nano template strategy, surface modification, multi-step chemical vapor deposition (CVD), and so on has demonstrated the huge advantage on this aspect. These strategies are generally used for homogeneous dispersing Sn nanomaterials in graphene matrix or constructing the voids in the inner of the materials to obtain the mechanical buffer effect. Unfortunately, these processes induce huge energy consumption and complicated operation. To solve the issue, new nanotechnology for the composites by the bottom-up strategy (Organic Molecule Confinement Reaction (OMCR)) was shown in this report. A 3D organic nanoframes was synthesized as a graphene precursor by low energy nano emulsification and photopolymerization. SnO2 nanoparticles@3D organic nanoframes as the composites precursor were in-situ formed in the hydrothermal reaction. After the redox process by the calcination, the Sn nanoparticles with nanovoids (~100 nm, uniform size) were homogeneously dispersed in a Two-Dimensional Laminar Matrix of graphene nanosheets (2DLMG) by the in-situ patterning and confinement effect from the 3D organic nanoframes. The pulverization and crack of the composites were effectively suppressed, which was proved by the electrochemical testing. The Sn nanoparticles@2DLMG not delivered just the high cyclability during 200 cycles, but also firstly achieved a high specific capacity (539 mAh g-1) at the low loading Sn (19.58 wt%).

Tuning the Band Structure of MoS2 via Co9S8@MoS2 Core-Shell Structure to Boost Catalytic Activity for Lithium-Sulfur Batteries.

The introduction of a dual-functional interlayer into lithium-sulfur batteries (LSBs) provides many opportunities for restraining the "shuttle effect" and enhancing sluggish sulfur conversion kinetics. Tuning the band structure of the metal sulfide provides an opportunity to enhance its catalytic activity, which plays an important role in suppressing the "shuttle effect" of lithium polysulfides (LiPSs) in LSBs. Here were present a Co9S8@MoS2 core-shell heterostructure anchored to a carbon nanofiber (Co9S8@MoS2/CNF), developed as an interlayer for suppressing the shuttle effect of LiPSs. The fabricated composite heterostructure is determined to be an effective alternative material that combines the synergistic relationship between chemisorption and electrochemical catalysis. We find that the band structure of the MoS2 shell can be effectively tuned by the Co9S8 core and that the Co9S8@MoS2/CNF can capture the LiPSs, providing excellent catalytic ability to convert LiPSs into Li2S2, with subsequent transformation from Li2S2 to Li2S. Importantly, high capacities of 1002 and 986 mAh g-1 can be retained after 50 cycles with high-sulfur loadings of 6 and 10 mg cm-2. Our results highlight the design of an atomic-scale heterostructure as a multifunctional interlayer providing a synergistic relationship between adsorption and catalysis. The net result is an effective retardation of the shuttling of LiPSs and an enhancement of the electrochemical redox reactions of LiPSs. This work shows great promise toward the development of practical applications of LSBs.

O3-Type Layered Ni-Rich Oxide: A High-Capacity and Superior-Rate Cathode for Sodium-Ion Batteries.

Inspired by its high-active and open layered framework for fast Li+ extraction/insertion reactions, layered Ni-rich oxide is proposed as an outstanding Na-intercalated cathode for high-performance sodium-ion batteries. An O3-type Na0.75 Ni0.82 Co0.12 Mn0.06 O2 is achieved through a facile electrochemical ion-exchange strategy in which Li+ ions are first extracted from the LiNi0.82 Co0.12 Mn0.06 O2 cathode and Na+ ions are then inserted into a layered oxide framework. Furthermore, the reaction mechanism of layered Ni-rich oxide during Na+ extraction/insertion is investigated in detail by combining ex situ X-ray diffraction, X-ray photoelectron spectroscopy, and electron energy loss spectroscopy. As an excellent cathode for Na-ion batteries, O3-type Na0.75 Ni0.82 Co0.12 Mn0.06 O2 delivers a high reversible capacity of 171 mAh g-1 and a remarkably stable discharge voltage of 2.8 V during long-term cycling. In addition, the fast Na+ transport in the cathode enables high rate capability with 89 mAh g-1 at 9 C. The as-prepared Ni-rich oxide cathode is expected to significantly break through the limited performance of current sodium-ion batteries.

Li0.35La0.55TiO3 Nanofibers Enhanced Poly(vinylidene fluoride)-Based Composite Polymer Electrolytes for All-Solid-State Batteries.

Using polymer electrolytes with relatively high mechanical strength, enhanced safety, and excellent flexibility to replace the conventional liquid electrolytes is an effective strategy to curb the Li-dendrite growth in Li-metal batteries (LMBs). However, low ionic conductivity, unsatisfactory thermal stability, and narrow electrochemical window still hinder their applications. Here, we fabricate Li0.35La0.55TiO3 (LLTO) nanofiber-enabled poly(vinylidene fluoride) (PVDF)-based composite polymer electrolytes (CPEs) with enhanced mechanical property and wide electrochemical window. The results show that 15 wt % of LLTO nanofibers synergize with PVDF, giving a flexible electrolyte membrane with significantly improved performance, such as high ionic conductivity (5.3 × 10-4 S cm-1), wide electrochemical window (5.1 V), high mechanical strength (stress 9.5 MPa, strain 341%), and good thermal stability (thermal degradation 410 °C). In addition, an all-solid-state Li-metal battery of sandwich-type LiFePO4/PVDF-CPE (15 wt % of LLTO)/Li delivers satisfactory cycling stability and outstanding rate performance. A reversible capacity of 121 mA h g-1 is delivered at 1 C after 100 cycles. This work exemplifies that the introduction of LLTO nanofibers can improve the electrochemical performances of PVDF-based CPEs used as electrolytes for all-solid-state LMBs.