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[Display omitted] • A PVDF/CA/LATP CSE is developed via a facile solution-casting process. • PVDF/CA ratio and LATP fractions affect CSE's crystallinity and structural porosity. • The optimized CSE exhibits a high ionic conductivity of 4.9 × 10-4 S cm−1. • The optimized CSE possesses a wide electrochemical window up to 5.0 V vs. Li/Li+. • An LFP-based cell containing PVDF/CA/LATP CSE delivers over 160 mAh g−1 capacity. To enhance energy density and secure the safety of lithium-ion batteries, developing solid-state electrolytes is a promising strategy. In this study, a composite solid-state electrolyte (CSE) composed of poly(vinylidene difluoride) (PVDF)/cellulose acetate (CA) matrix, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt, and Li 1.3 Al 0.3 Ti 1.7 (PO 4) 3 (LATP) fillers is developed via a facile solution-casting method. The PVDF/CA ratio, LiTFSI, and LATP fractions affect the crystallinity, structural porosity, and thermal and electrochemical stability of the PVDF/CA/LATP CSE. The optimized CSE (4P1C-40LT/20F) presents a high ionic conductivity of 4.9 × 10-4 S cm−1 and a wide electrochemical window up to 5.0 V vs. Li/Li+. A lithium iron phosphate-based cell containing the CSE delivers a high discharge capacity of over 160 mAh g−1 at 25 °C, outperforming its counterpart containing PVDF/CA polymer electrolyte. It also exhibits satisfactory cycling stability at 1C with approximately 90 % capacity retention at the 200th cycle. Additionally, its rate performance is promising, demonstrating a capacity retention of approximately 80 % under varied rates (2C/0.1C). The increased amorphous region, Li+ transportation pathways, and Li+ concentration of the 4P1C-40LT/20F CSE membrane facilitate Li+ migration within the CSE, thus improving the battery performance. [ABSTRACT FROM AUTHOR]

Due to their higher safety, stability and energy density, all-solid-state batteries will be promising candidates for the next generation of lithium battery systems. The acquisition of high-performance solid-state electrolytes is pivotal in the actualization of all-solid-state batteries. By uniformly dispersing nanoscale Li1.3Al0.3Ti1.7(PO4)3 (LATP) powders into polyethylene oxide (PEO)-LiClO4 at varying mass ratios, a composite electrolyte membrane of approximately 50 μm thickness was prepared using the casting method. Subsequent characterization of these materials, accomplished through X-ray diffraction, scanning electron microscopy, electrochemical impedance spectroscopy, and cyclic charge–discharge tests, unveiled intriguing findings. Although the beneficial effect of LATP on the conductivity of PEO is somewhat limited, it demonstrates a capability to reduce the interface impedance between polyethylene oxide and lithium metal, thereby enhancing interface stability. This research provides constructive insights and prompts for designing composite electrolytes for future all-solid-state batteries. [ABSTRACT FROM AUTHOR]

Highlights: This study introduces an innovative 3D-printed electrolyte with vertically aligned ion transport network, which contains well-dispersed nanoscale Ta-doped Li7La3Zr2O12 in a poly(ethylene glycol) diacrylate matrix. The 3DSE architecture enables efficient ion transport across the Li/electrolyte and electrolyte/cathode interfaces, which allows for increased active material mass loading and enhanced interfacial adhesion. The p-3DSE Li symmetric cell displays an impressive critical current density value of 1.92 mA cm−2 and stable operation for 2600 h at room temperature. Full cells using p-3DSE achieve notable areal capacities. Improving the long-term cycling stability and energy density of all-solid-state lithium (Li)-metal batteries (ASSLMBs) at room temperature is a severe challenge because of the notorious solid–solid interfacial contact loss and sluggish ion transport. Solid electrolytes are generally studied as two-dimensional (2D) structures with planar interfaces, showing limited interfacial contact and further resulting in unstable Li/electrolyte and cathode/electrolyte interfaces. Herein, three-dimensional (3D) architecturally designed composite solid electrolytes are developed with independently controlled structural factors using 3D printing processing and post-curing treatment. Multiple-type electrolyte films with vertical-aligned micro-pillar (p-3DSE) and spiral (s-3DSE) structures are rationally designed and developed, which can be employed for both Li metal anode and cathode in terms of accelerating the Li+ transport within electrodes and reinforcing the interfacial adhesion. The printed p-3DSE delivers robust long-term cycle life of up to 2600 cycles and a high critical current density of 1.92 mA cm−2. The optimized electrolyte structure could lead to ASSLMBs with a superior full-cell areal capacity of 2.75 mAh cm−2 (LFP) and 3.92 mAh cm−2 (NCM811). This unique design provides enhancements for both anode and cathode electrodes, thereby alleviating interfacial degradation induced by dendrite growth and contact loss. The approach in this study opens a new design strategy for advanced composite solid polymer electrolytes in ASSLMBs operating under high rates/capacities and room temperature. [ABSTRACT FROM AUTHOR]

Copyright of Acta Materiae Compositae Sinica is the property of Acta Materiea Compositae Sinica Editorial Department and its content may not be copied or emailed to multiple sites or posted to a listserv without the copyright holder's express written permission. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)

In pursuit of safer lithium-ion batteries, research is veering towards all-solid-state lithium batteries (ASSLBs) featuring solid electrolytes due to the safety concerns and low metal interfacial compatibility of liquid electrolytes. ASSLBs combined with composite solid electrolytes (CSEs) incorporating NASICON-type active fillers are especially appealing because of their inherent safety, ease of production, and high energy density. This study introduces a Li 1 · 5 Al 0.5 Ge 1.5 (PO 4) 3 (LAGP) framework created via tape casting and in situ thermal polymerization, achieving a CSE with notable ionic conductivity (0.791 mS cm−1), electrochemical stability up to 5.09 V, and a lithium-ion transference number of 0.72 at 30 °C. The Li|CSE|Li cell demonstrates low overpotential over 1000 h, and the Li|CSE|NCM811 coin cell delivers a discharge capacity of 180.9 mAh g−1, maintaining 84.6 % capacity after 200 cycles. Moreover, the Li|CSE|NCM811 pouch cell upholds a capacity of 116.41 mAh g−1 after 100 cycles, underscoring the 3D LAGP framework and in situ polymerization's role in enhancing ASSLB safety and functionality. The composite solid electrolyte, synthesized through a straightforward one-step in-situ polymerization process within a three-dimensional LAGP framework, exhibits excellent ionic conductivity and demonstrates superior electrochemical performance in all-solid-state lithium batteries. [Display omitted] • Composite Solid Electrolyte with 3D LAGP framework is synthesized. • The CSE showed the ionic conductivity of 7.91 × 10−4 S cm−1 at 30 °C. • The Li.|CSE|Li cell shows excellent stability over 1000 h with low over potential. • The Li.|CSE|NCM cell delivers excellent rate capability, and long cyclability. • The coin and pouch type cells show the applicability of the CSE. [ABSTRACT FROM AUTHOR]

Benefitting from the synergistic effect of the continuous 3D NZSP framework and PEO/PVDF-HFP asymmetric polymer electrolyte layer, the novel composite solid electrolyte for solid-state sodium metal batteries exhibits ultrahigh ion transference number and stability. [Display omitted] • A novel 3D-NZSP solid electrolyte was synthesized via using NaCl as the templatewe. • The 3D-15PNZSPP exhibits an outstanding transference number of 0.82 at temperature of 30 °C. • The Na/3D-15PNZSPP/Na symmetric cell can cycle for 700 h with a small overpotential. • The assembled Na 0.67 Li 0.24 Mn 0.76 O 2 /3D-15PNZSPP/Na batteries demonstrate remarkable cycling stability. The combination of a Na-ion conducting filler and polymer matrix in composite solid electrolyte (CSE) presents a promising and attractive strategy for improving the energy density and safety of the sodium-metal batteries. The agglomeration and precipitation of inorganic ceramic fillers in the polymer matrix present a major challenge leading to the decreased Na ion conductivity property and transference number, increased interfacial resistance, and worsened mechanical properties of CSEs. Herein, we introduce a novel composite solid electrolyte (denoted as 3D-15PNZSPP), comprising a three-dimensional interconnected porous Na 3 Zr 2 Si 2 PO 12 framework integrated with an asymmetric polymer electrolyte layer, which not only offers continuous conductive pathways and high mechanical strength for Na ions transfer, but also enhances the interfacial compatibility and expands the electrochemical stability window. The 3D-15PNZSPP CSE shows a high Na+ conductivity of 7.6 × 10−4 S cm−1 and an outstanding transference number of 0.82 at temperature of 30 °C. These characteristics enable the Na/3D-15PNZSPP/Na symmetric cell to cycle for over 700 h with a small overpotential. More importantly, the assembled all solid-state Na 0.67 Li 0.24 Mn 0.76 O 2 /3D-15PNZSPP/Na batteries demonstrate remarkable cycling stability and high rate capability, indicating a promising and facile strategy for designing ultra-safe and high-performance solid-state sodium metal batteries. [ABSTRACT FROM AUTHOR]

[Display omitted] All solid-state batteries (ASSBs) are regarded as promising energy storage batteries with high energy density and high safety. The polyethylene oxide (PEO)-based electrolyte with succinonitrile (SN) has attracted critical attention for its high ionic conductivity at room temperature. However, SN can react with Li metal to result in an unstable interface between electrolyte and electrode, which deteriorates the electrochemical performance. In this work, zeolitic imidazolate framework-67 (ZIF-67) is used as a filler to construct composite electrolytes and solve the aforementioned instability issue. The composite electrolyte shows nonflammability, high processability, and a competitive ionic conductivity of 2.78 * 10−5 S/cm at room temperature. Due to the regular dodecahedron structure and abundant Lewis acid sites, the composite electrolyte film exhibits a high Li-ion transference number of 0.654 and a wide electrochemical window of more than 5 V. Moreover, the ZIF-67 helps to construct a uniform and fast ion transport channel and can promote the generation of LiF to prevent SN from contacting Li anode, which contributes to the excellent stability of the Li symmetric batteries cycling for over 1000 h at a current density of 1 mA cm−2. And the assembled LiFePO 4 ||Li batteries based on the composite electrolyte display high discharge specific capacities of 158.6 and 70 mAh g−1 at 60 °C and room temperature, respectively. [ABSTRACT FROM AUTHOR]

Copyright of Journal of South China University of Technology (Natural Science Edition) is the property of South China University of Technology and its content may not be copied or emailed to multiple sites or posted to a listserv without the copyright holder's express written permission. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)

Thin solid‐state electrolytes with nonflammability, high ionic conductivity, low interfacial resistance, and good processability are urgently required for next‐generation safe, high energy density lithium metal batteries. Here, a 3D Li6.75La3Zr1.75Ta0.25O12 (LLZTO) self‐supporting framework interconnected by polytetrafluoroethylene (PTFE) binder is prepared through a simple grinding method without any solvent. Subsequently, a garnet‐based composite electrolyte is achieved through filling the flexible 3D LLZTO framework with a succinonitrile solid electrolyte. Due to the high content of garnet ceramic (80.4 wt%) and high heat‐resistance of the PTFE binder, such a composite electrolyte film with nonflammability and high processability exhibits a wide electrochemical window of 4.8 V versus Li/Li+ and high ionic transference number of 0.53. The continuous Li+ transfer channels between interconnected LLZTO particles and succinonitrile, and the soft electrolyte/electrode interface jointly contribute to a high ambient‐temperature ionic conductivity of 1.2 × 10−4 S cm−1 and excellent long‐term stability of the Li symmetric battery (stable at a current density of 0.1 mA cm−2 for over 500 h). Furthermore, as‐prepared LiFePO4|Li and LiNi0.5Mn0.3Co0.2O2|Li batteries based on the thin composite electrolyte exhibit high discharge specific capacities of 153 and 158 mAh g−1 respectively, and desirable cyclic stabilities at room temperature. [ABSTRACT FROM AUTHOR]

In this study, a Li 6.5 Ga 0.2 La 2.95 Rb 0.05 Zr 2 O 12 garnet-type solid electrolyte with high ion conductivity was prepared. The particle size was reduced to the nano size through a ball milling process, and the effect of the change in particle size on the all-solid-state batterie was investigated. As all-solid-state batteries have better stability than liquid electrolytes and serve as separators to help increase energy density, much research has been conducted recently. However, their conductivity is much lower than that of the liquid electrolyte. Therefore, an experiment was conducted on the difference in particle size to improve the ionic conductivity and energy density. Reducing the average particle size of the LLZO samples from approximately 10 to 0.6 μm using a ball milling process increased the ionic conductivity of the pellet from 1.27 × 10–3 to 1.58 × 10–3 S cm-1 at 25 °C. The ionic conductivity of the sheet decreased from 2.96 × 10–4 to 2.60 × 10–4 S cm-1 at 70 °C, but lithium transference number increased from 0.56 to 0.64. Therefore, the structural and electrochemical properties of the LLZO-bare and LLZO-ball-milled were investigated using powder X-ray diffraction analysis, field-emission scanning electron microscopy, electrochemical impedance spectroscopy, and galvanostatic measurements. • The particle size of this Ga Rb LLZO material was reduced from 10.1 to 0.61 μm through ball-milling. • The LLZO-ball-milled pellet exhibited a high ionic conductivity of 1.58 × 10−3 S cm−1 at 25 °C • Composite solid electrolytes were prepared via PEO, Ga Rb LLZO and Li salts. • The LLZO-ball-milled was low and stable, even in the symmetric cell overvoltage. • In the coin cell test, LLZO-ball-milled has high discharge capacity and is stable in cycle retention rate and rate characteristics. [ABSTRACT FROM AUTHOR]

• MPEG@LLZTO inhibit its agglomeration in CSE and enhanced the ionic conductivity. • The lightweight design of PLCN maximizes the gravimetric energy density of the ASSBs. • The CN scaffold enhances the temperature endurance and structural robustness of CSE. The lightweight solid electrolyte design in replacement of the flammable liquid electrolyte and polyolefin separator is the key of the energy-dense all-solid-state batteries (ASSBs) construction. However, the technological barriers of scalable manufacturing, retarded ionic conductivity at room temperature as well as the mechanical fragility upon the high-temperature operation restrict the ASSB deployment of practical relevance. In this study, an ultra-lightweight (1.67 mg cm−2), thin (25 μm), high strength and thermally robust (stability up to 180 °C) composite solid electrolyte (CSE) has been designed to address the dilemma by the rational integration of polyethylene glycol monomethyl ethers coated Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 nanofillers (MPEG@LLZTO) with lightweight nanocellulose scaffold. The MPEG coating layer enhances the interfacial compatibility and homogeneous dispersibility of LLZTO nanofiller within the poly (ethylene oxide) (PEO) matrix, while the mechanically flexible and thermally stable nanocellulose scaffold guarantees the formation of the high-temperature endurance and structural robustness for the as-formed CSE layer. Upon the solvent-free, layer stacked-up assembly of the PEO/MPEG@LLZTO-Nanocellulose (PLCN) CSE film with the high-mass-loading LiFePO 4 cathode and thin-layer lithium anode, the ASSB prototype could simultaneously realize the high gravimetric energy density (323 Wh kg−1), cycling stability as well as operation reliability within a wider temperature range (25 °C ∼ 130 °C). [ABSTRACT FROM AUTHOR]

Solid-state electrolyte for solid-state batteries is one of the current hotspots in the research field of high-safety and high energy density lithium metal batteries. This work reports a polymer-in-ceramic and ceramic-in-polymer bilayer ultrathin (∼11 μm) composite solid electrolyte (CSE) membrane by exploiting a spontaneous precipitation of Li 7 La 3 Zr 2 O 12 in a polymer-lithium salt matrix. The polymer-in-ceramic layer is toward a high-voltage cathode, which can effectively inhibit oxidative decomposition of electrolytes. The ceramic-in-polymer layer toward the anode can provide good flexibility. Experimental results show that the CSE bilayer membrane has not only high ionic conductivity but also satisfactory Li+ transference number. It also exhibits excellent thermal and mechanical properties. High-voltage Li||LiCoO 2 (4.5 V) cell employing this CSE membrane exhibits excellent cycling stability (151.18 mAh g−1 at 1 C after 100 cycles), and superior rate performance (124.31 mAh g−1 10 C). This work guides the improvement of both solid state electrolyte membrane and high-voltage solid-state lithium metal batteries. [Display omitted] • An ultrathin (∼11 μm) "polymer-in-ceramic" and "ceramic-in-polymer" bilayer electrolyte membrane is prepared. • The membrane exhibits high-voltage stability performance and excellent mechanical/thermal stability. • The Li||LiCoO2 (4.5 V) cell assembled with the membrane delivers superior cycling stability and high-rate performance. [ABSTRACT FROM AUTHOR]