Search

In the current challenging energy storage and conversion landscape, solid‐state lithium metal batteries with high energy conversion efficiency, high energy density, and high safety stand out. Due to the limitations of material properties, it is difficult to achieve the ideal requirements of solid electrolytes with a single‐phase electrolyte. A composite solid electrolyte is composed of two or more different materials. Composite electrolytes can simultaneously offer the advantages of multiple materials. Through different composite methods, the merits of various materials can be incorporated into the most essential part of the battery in a specific form. Currently, more and more researchers are focusing on composite methods for combining components in composite electrolytes. The ion transport capacity, interface stability, machinability, and safety of electrolytes can be significantly improved by selecting appropriate composite methods. This review summarizes the composite methods used for the components of composite electrolytes, such as filler blending, embedded framework, and multilayer bonding. It also discusses the future development trends of all‐solid‐state lithium batteries (ASSLBs). [ABSTRACT FROM AUTHOR]

This study explores multi-component garnet-based materials as solid electrolytes for all-solid-state lithium batteries. Through a combination of computational and experimental approaches, we investigate the thermodynamic and structural properties of lithium lanthanum zirconium oxide garnets doped with various elements. Applying density functional theory, the influence of dopants on the thermodynamic stability of these garnets was studied. Probable atomic configurations and their impact on materials' properties were investigated with the focus on understanding the influence of these configurations on structural stability, phase preference, and ionic conductivity. In addition to the computational study, series of cubic-phase garnet compounds were synthesized and their electrochemical performance was evaluated experimentally. Our findings reveal that the stability of cubic phase in doped Li-garnets is primarily governed by enthalpy, with configurational entropy playing a secondary role. Moreover, we establish that the increased number of doping elements significantly enhances the cubic phase's stability. This in-depth understanding of materials' properties at atomic level establishes the basis for optimizing high-entropy ceramics, contributing significantly to the advancement of solid-state lithium batteries and other applications requiring innovative material solutions. [ABSTRACT FROM AUTHOR]

Copyright of Journal of Zhengzhou University (Natural Science Edition) is the property of Journal of Zhengzhou University (Natural Science Edition) Editorial Office 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.)

The Li dendrite problem triggered by the inhomogeneous deposition of Li and the reduction of Li+ in the electrolyte has seriously hindered the practical application of garnet‐based solid‐state batteries. To address this issue, a multifunctional double layer (MDL) based on the phenomenon of segregation during welding is introduced between the garnet and the Li anode. BiLi3/LiCl3 interlayer with a double‐layer structure is constructed by modulating the cooling rate. The LiCl3 enriched on the electrolyte side exhibits extremely low electronic conductivity, effectively blocking electrons and preventing electrolyte attack. On the anode side, the BiLi3‐enriched layer regulates local current distribution, ensuring uniform deposition/exfoliation of Li and preventing dendrite formation at the interface. Furthermore, this welding‐based preparation method achieves a strong and secure connection between the metal electrode and the ceramic electrolyte. Hence, this Li|LLZTO‐MDL|Li battery with double‐layer special structural interfacial modification can realize a high critical current density of 2.9 mA cm−2 and can be stably cycled for more than 10 000 h at 0.3 mA cm−2. [ABSTRACT FROM AUTHOR]

One of the effective methods to improve the energy density and safety of lithium metal batteries is to use composite solid electrolytes with high voltage and good performance. However, the low ionic conductivity at room temperature and the unsatisfactory Li+ migration number of composite solid electrolytes lead to the growth of lithium dendrites and the increase of internal resistance, which restricts the industrialization of composite electrolytes for solid-state lithium batteries. This work prepares a Li6.4La3Zr1.4Ta0.6O12 (LLZTO)/polyethylene oxide (PEO)/polyvinylidene fluoride (PVDF) composite electrolyte. In this "polymer in ceramic" type electrolyte, the combination of PEO with PVDF and LLZTO reduces the crystallinity of PEO and promotes the rapid migration of Li+ along the PEO polymer molecular chain through complexation and decomplexation. At the same time, LLZTO, which has an excellent ion conduction function, introduces new ion conduction channels when combined with PEO and PVDF, thereby further improving ion conductivity. The LP82 composite electrolyte has a Li+ migration number of 0.78 and an electrochemical stability window of 5.5 V and exhibits excellent flexibility. The Li/LP82 electrolyte/Li battery has a relatively stable voltage of 0.04 V at 0.1 mA cm−2 and a stable cycling of 1000 h. The discharge specific capacity of the LiFePO4/LP82/Li battery is 144.4 mA h g−1 at 0.1 C after 180 cycles, and the capacity retention is 90.7%. This work provides a good reference for the preparation of composite electrolytes with simple processes, high voltage, and high performance. [ABSTRACT FROM AUTHOR]

Solid‐state lithium batteries (SSLBs) have great development prospects in high‐security new energy fields, but face major challenges such as poor charge transfer kinetics, high interface impedance, and unsatisfactory cycle stability. Defect engineering is an effective method to regulate the composition and structure of electrodes and electrolytes, which plays a crucial role in dominating physical and electrochemical performance. It is necessary to summarize the recent advances regarding defect engineering in SSLBs and analyze the mechanism, thus inspiring future work. This review systematically summarizes the role of defects in providing storage sites/active sites, promoting ion diffusion and charge transport of electrodes, and improving structural stability and ionic conductivity of solid‐state electrolytes. The defects greatly affect the electronic structure, chemical bond strength and charge transport process of the electrodes and solid‐state electrolytes to determine their electrochemical performance and stability. Then, this review presents common defect fabrication methods and the specific role mechanism of defects in electrodes and solid‐state electrolytes. At last, challenges and perspectives of defect strategies in high‐performance SSLBs are proposed to guide future research. [ABSTRACT FROM AUTHOR]

For high‐energy‐density lithium batteries, the research and development of solid‐state electrolytes is crucial. Inorganic‐organic composite electrolytes with high mechanical strength and ionic conductivity of inorganic ceramic electrolytes, as well as high interfacial compatibility of polymer electrolytes, have become a current research hotspot. Based on a brief discussion of lithium dendrite growth and Li+ ion transport mechanisms, this article provides a comprehensive review of the nanostructure design and performance of inorganic‐organic composite electrolytes in recent years, and focuses on the mechanism of homogeneous monolayer composite electrolytes and heterogeneous multilayer composite electrolytes to enhance the performance of electrolytes. In addition, the future prospect of inorganic‐organic composite electrolytes is discussed, providing practical guidance for researchers in this field. [ABSTRACT FROM AUTHOR]

Solid electrolyte lithium batteries are the next generation of advanced energy devices. The incorporation of solid electrolytes can significantly improve the safety issue of lithium‐ion batteries. Organic‐inorganic composite solid electrolytes (CSE) are promising candidates for solid‐state batteries, but their application is mainly limited by low ionic conductivity. Many studies have shown that the architecture of ordered inorganic fillers in CSE can act as fast lithium‐ion transfer channels by auxiliary means, thus significantly improving the ionic conductivities. This review summarises the recent advances in CSE with different dimensional inorganic fillers. Various effective strategies for the construction of ordered structures in CSE are then presented. The review concludes with an outlook on the future development of CSE. This review aims to provide researchers with an in‐depth understanding of how to achieve ordered architectures in CSE for advanced solid state lithium batteries. [ABSTRACT FROM AUTHOR]

Poly(vinylidene fluoride) (PVDF)-based composite solid electrolytes (CSEs) are attracting widespread attention due to their superior electrochemical and mechanical properties. However, the PVDF has a strong polar group -CF2-, which easily continuously reacts with lithium metal, resulting in the instability of the solid electrolyte interface (SEI), which intensifies the formation of lithium dendrites. Herein, Tetrafluoro-1,4-benzoquinone (TFBQ) was selected as an additive in trace amounts to the PVDF/Li-based electrolytes. TFBQ uniformly formed lithophilic quinone lithium salt (Li2TFBQ) in the SEI. Li2TFBQ has high lithium-ion affinity and low potential barrier and can be used as the dominant agent to guide uniform lithium deposition. The results showed that PVDF/Li-TFBQ 0.05 with a mass ratio of PVDF to TFBQ of 1:0.05 had the highest ionic conductivity of 2.39 × 10−4 S cm−1, and the electrochemical stability window reached 5.0 V. Moreover, PVDF/Li-TFBQ CSE demonstrated superior lithium dendrite suppression, which was confirmed by long-term lithium stripping/sedimentation tests over 2000 and 650 h at a current of 0.1 and 0.2 mA cm−2, respectively. The assembled solid-state LiNi0.6Co0.2Mn0.2O2||Li cell showed an excellent performance rate and cycle stability at 30 °C. This study greatly promotes the practical research of solid-state electrolytes. [ABSTRACT FROM AUTHOR]

Copyright of Journal of Functional Materials / Gongneng Cailiao is the property of Chongqing Functional Materials Periodical Press 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.)

A high-energy-density commercial ternary material NCM811 was used as cathode material for lithium metal battery, wth two kinds of bindersol based PVDF and aqueous CMC. As prepared PVDF-HFP/ LLZTO composte membrane was used as the solid electrolyte, and metallic ithium was used as the anode to assemble soiid ithium metal battery. Cyciing performance of the cell was tested at room temperature at a rate of 0. 2 C. Compared to NCM811 cathode using PVDF as the binder, cathode wth the CMC binder has a better stabiy and a higher cycle capacty retention ratio. The discharge capacty of cathode wth the CMC binder after 40 cycles is 137 mAh ⋅ g-1 and the capacty retention rate is 90%. This can be attributed to the good adheson between the binder and NCM particles, which can prevent the cathode crack and detach. However, the specitic dsscharge capacty of the cell wth the CMC binder ss relatively low. This can be attributed to the reaction between high nickel cathode material and aqueous solution, which leads to a decrease of active ithium in the surface of the cathode material. Further improvement ss needed for the commercialization of the CMC binder for NCM811 based cathodes. [ABSTRACT FROM AUTHOR]

Solid‐state lithium battery promises highly safe electrochemical energy storage. Conductivity of solid electrolyte and compatibility of electrolyte/electrode interface are two keys to dominate the electrochemical performance of all solid‐state battery. By in situ polymerizing poly(ethylene glycol) methyl ether acrylate within self‐supported three‐dimensional porous Li1.3Al0.3Ti1.7(PO4)3 framework, the as‐assembled solid‐state battery employing 4.5 V LiNi0.8Mn0.1Co0.1O2 cathode and Li metal anode demonstrates a high Coulombic efficiency exceeding 99% at room temperature. Solid‐state nuclear magnetic resonance results reveal that Li+ migrates fast along the continuous Li1.3Al0.3Ti1.7(PO4)3 phase and Li1.3Al0.3Ti1.7(PO4)3/polymer interfacial phase to generate a fantastic conductivity of 2.0 × 10−4 S cm−1 at room temperature, which is 56 times higher than that of pristine poly(ethylene glycol) methyl ether acrylate. Meanwhile, the in situ polymerized poly(ethylene glycol) methyl ether acrylate can not only integrate the loose interfacial contact but also protect Li1.3Al0.3Ti1.7(PO4)3 from being reduced by lithium metal. As a consequence of the compatible solid‐solid contact, the interfacial resistance decreases significantly by a factor of 40 times, resolving the notorious interfacial issue effectively. The integrated strategy proposed by this work can thereby guide both the preparation of highly conductive solid electrolyte and compatible interface design to boost practical high energy density all solid‐state lithium metal battery. [ABSTRACT FROM AUTHOR]

High room-temperature ionic conductivity and mechanical property are essential for the application of solid electrolyte. In this work, a poly(vinylidene fluoride) (PVDF)-based composite polymer solid electrolyte membrane (CSE) incorporated with Li7La3Zr2O12 (LLZO) fillers and high-strength porous skeleton was prepared. The introduction of LLZO increased the ionic conductivity of PVDF at room temperature by reducing the crystallinity of PVDF matrix, and the addition of skeleton greatly improved the mechanical property of electrolyte membrane and inhibited the growth of lithium dendrites. The prepared PVDF-LLZO CSE has a room-temperature ionic conductivity of 1.75 × 10−4 S/cm, and the tensile strength reaches 95 MPa, which greatly enhanced the ability of lithium dendrite suppression. The assembled LiNi0.6Co0.2Mn0.2O2 (NCM622)/CSE/Li cell shows an initial capacity of 151 mAh/g with a retention capacity of 108 mAh/g after 100 cycles at the current density of 0.5 C. This ultrathin PVDF/LLZO CSE has a great application prospect in solid-state lithium batteries. [ABSTRACT FROM AUTHOR]

Summary: Herein, the electrochemical characteristics of Li/LiFePO4 battery, comprising a new class of poly (ethylene oxide) (PEO) hosted polymer electrolytes, are reported. The electrolytes were prepared using lithium bis(trifluoromethylsulfonyl)imide (LiTFSI) dopant salt and imidazolium ionic liquid‐based nanofluid (ionanofluid) as the plasticizer. Morphological, thermophysical, electrical, and electrochemical properties of these newly developed electrolytes were studied. Using FT‐IR spectroscopy, the interactions between dopant salt plasticizers and the host polymer, within the electrolytes, were evaluated. The optimized 30 wt% ionanofluid plasticized electrolyte exhibits a room temperature ionic conductivity of 6.33 × 10−3 S cm−1, wide electrochemical voltage window (~4.94 V vs Li/Li+) along with a moderately high value of lithium‐ion transference number (0.47). The values are substantially higher than that of similar wt% IL plasticized electrolyte (7.85 × 10−4 S cm−1, ~4.44 V vs Li/Li+ and ~ 0.28, respectively). Finally, the Li/LiFePO4 battery, comprising optimized 30 wt% ionanofluid plasticized electrolyte, delivers 156 mAh g−1 discharge capacity at 0.1 C rate and able to retain its 92% value after 50 cycles. Such a superior battery performance as compared to the IL plasticized electrolyte cell (137 mAh g−1 and 84% after 50 cycles at the same current rate) would endow this ionanofluid a very promising plasticizer to develop electrolytes for next‐generation lithium polymer battery. [ABSTRACT FROM AUTHOR]

Summary: High ionic conductivity at room temperature (RT) and good ion transport capability at electrode/electrolyte interface are fundamental requirements for high‐rate solid‐state lithium batteries (SSBs). In this work, we designed a poly (propylene carbonate) (PPC)‐based organic/inorganic composite solid electrolyte (CSE) membrane with high filling of tantalum‐doped lithium lanthanum zirconium oxide (LLZTO) and functionalized layers for enhancing the RT rate performance of SSB. The synergistic effect of LLZTO and interfacial functionalized layers endows the NCM622/CSE/Li battery with high‐rate and cycling performances at RT. The SSB with 20% LLZTO‐filled solid electrolyte shows the initial capacities of 162.0, 148.5 and 130.1 mAh g−1 at 1C, 2C, and 3C respectively, with retention capacities of 115.6, 104, and 100.6 mAh g−1 after 150 cycles. This strategy for an organic/inorganic CSE is of great practical significance for the development of high‐rate SSBs. [ABSTRACT FROM AUTHOR]

Copyright of Electronic Components & Materials is the property of Electronic Components & Materials 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.)

SUMMARY Solid polymer composite electrolyte (SPCE) with good safety, easy processability, and high ionic conductivity was a promising solution to achieve the development of advanced solid‐state lithium battery. Herein, through electrospinning and subsequent calcination, the Li0.33La0.557TiO3 nanowires (LLTO‐NWs) with high ionic conductivity were synthesized. They were utilized to prepare polymer composite electrolytes which were composed of poly (ethylene oxide) (PEO), poly (propylene carbonate) (PPC), lithium bis (fluorosulfonyl)imide (LiTFSI), and LLTO‐NWs. Their structures, thermal properties, ionic conductivities, ion transference number, electrochemical stability window, as well as their compatibility with lithium metal, were studied. The results displayed that the maximum ionic conductivities of SPCE containing 8 wt.% LLTO‐NWs were 5.66 × 10−5 S cm−1 and 4.72 × 10−4 S cm−1 at room temperature and 60°C, respectively. The solid‐state LiFePO4/Li cells assembled with this novel SPCE exhibited an initial reversible discharge capacity of 135 mAh g−1 and good cycling stability at a charge/discharge current density of 0.5 C at 60°C. [ABSTRACT FROM AUTHOR]

Employing solid electrolytes in lithium-ion batteries is anticipated to be a solution to some issues originated from their organic electrolytes. However, solid-state lithium batteries had not been practicable, because ionic conductivities of lithium-ion conductive solid electrolytes had been very low. Therefore, many studies aiming at the development of solid-state lithium batteries have been focused on enhancement of ionic transport in solids. They have succeeded in enhancing the conductivity to be comparable to or even higher than that of liquids. At this stage, rate-determining step of the battery reactions is sometimes ionic transport at interface rather than bulk in the battery components. Since anomalous ionic conduction at the interface takes place in space-charge layers with ca. 10 nm in thickness, it will be controlled by 'nanoarchitectonics'. This paper reviews some interfacial nanoarchitectures that control the interfacial ionic conduction to enhance the performance of solid-state lithium batteries. [ABSTRACT FROM AUTHOR]