ACS Applied Energy Materials
·
2021
·
IF 6.024
Jingyu Ma,Xiaoyan Ma,Chengchen Luo,Xinghua Guan,Fang Chen,Yibo Chen,Jingwen Tu
The low ionic conductivity and mechanical strength are important factors impeding the application of solid polymer electrolytes. Herein, we design synthesize an organic/inorganic hybrid star-shaped polymer of octa(poly(methyl methacrylate)–poly(poly(ethylene glycol) methyl ether methacrylate) cage oligomeric silsesquioxanes (POSS–(PMMA–PPEGMEM)8) by one-step free atom transfer radical polymerization (ATRP), and compound with Li6.4La3Zr1.4Ta0.6O12 (LLZTO) to prepare a composite polymer electrolyte membrane (LP-CPEM). The star-shaped structure of the POSS–(PMMA–PPEGMEM)8 induced by octachloropropyl polyhedral cage oligomeric silsesquioxane (OCP-POSS) is beneficial to reduce the crystallinity of polymer and increase the movement of the polymer chain to form a continuous interconnected ion migration channel. The LLZTO fillers in the LP-CPEM could simultaneously hinder the orderly arrangement of polymer chains and provide other ion transport paths to increase the ion conductivity of LP-CPEM. The LP-CPEM with 7.5 wt % LLZTO has higher ionic conductivity of 3.8 × 10–4 S cm–1 at 30 °C and high mechanical strength (5.2 MPa). Additionally, Li/Li symmetric cells demonstrate stable constant current charging/discharging during 1000 h at 0.1 mA cm–2, and the all-solid-state batteries fabricated by the LP-CPEM exhibit good cyclic stability. It is promising for the development of next-generation high-safety all-solid-state lithium metal batteries.
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DOI
高影响因子
IONICS
·
2021
·Vol. 27
·期 8
·3339-3346
·
IF 2.817
Liu Huirong,Li Jianling,Feng Wei,Han Guimei
Commercial lithium-ion batteries have safety risks due to the use of electrolyte-containing flammable organic solvents. The development of all solid-state lithium ion batteries with solid electrolyte is a feasible technical way to improve the safety of batteries. In this work, PVDF-based composite solid-state electrolytes (CSEs) were prepared by coupling Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) and polyvinylidene fluoride (PVDF). The electrochemical performance and interfacial compatibility between composite electrolyte and electrode were improved by the combination of appropriate amount of Li-ion-conducting particles and the insulating polymer. The corresponding solid-state battery of LiFePO 4 |PVDF-LLZTO-CSE| Li is fabricated and delivers initial discharge capacity of 162.4 mAh g -1 , and coulomb efficiency is approximately 98.5%. And the solid-state battery exhibits satisfactory rate capability and cycling stability at room temperature. This study suggests that a combination of the lithium garnet particles and insulating polymer is one of the promising methods to solve the problem of liquid electrolyte.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态离子学
·
电池技术
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高影响因子
Journal of Materiomics
·
2022
·Vol. 9
·期 3
·568-576
·
IF 8.589
Qiujun Wang,Weiqi Zhu,Ya Su,Di Zhang,Zhaojin Li,Huan Wang,Huilan Sun,Bo Wang,Dan Zhou,Li-Zhen Fan
Lithium metal batteries based on solid electrolytes are considered as promising candidates with high energy density and safety. However, the weak solid-solid contact between electrolyte and electrode can easily lead to interface instability and lithium ions discontinuous migration, which seriously reduces the electrochemical performance of the battery. Herein, we construct a soft gel interfacial layer to improve the stability of the solid-solid interface between electrolyte and electrode by means of polyester-based monomers and imidazole-based ionic liquids. Based on this, garnet-type Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) particles as inorganic ceramic filler were introduced in the layer to obtain composite electrolytes with high ionic conductivity (up to 1.1 × 10 −3 S/cm at 25 °C). As a result, the assembled lithium symmetric battery of Li|THCE-15%LLZTO|Li suggests excellent cycling stability with 700 h at 0.1 mA/cm 2 at 50 °C, and the lithium metal batteries of LFP|THCE-15%LLZTO|Li delivers high initial discharge capacity of 128.2 mA ·h/g with capacity retain of 75.48% after 150 cycles at 2 C. This work paves a new route to build safe and stable lithium metal batteries with synergistic introduction of composite electrolytes between electrolyte and electrode using soft gel interfacial layer and inorganic filler.
研究领域:
电化学
·
材料科学
·
能源存储
·
固体离子学
·
界面工程
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DOI
高影响因子
ACS Applied Energy Materials
·
2020
·
IF 4.473
Tao Wei,Zao-Hong Zhang,Zhi-Meng Wang,Qi Zhang,Yu-sheng Ye,Jia-Hao Lu,Zia ur Rahman,Zhi-Wei Zhang
Solid composite electrolytes (SCEs) are regarded as an effective solution to ensure safety and enhance the energy density of lithium-based batteries. This work reports an ultrathin SCE membrane (∼ 15 μm) based on Li6.4La3Zr1.4Ta0.6O12/PVDF-HFP/LiTFSI/succinonitrile; it not only possesses good ionic conductivity (6.53 × 10–4 S cm–1 with a little amount of liquid electrolyte) at 30 °C and a satisfactory lithium ion transfer number (0.55 without electrolyte), but also exhibits excellent thermal and mechanical properties. A symmetric cell with SCE succinonitrile-10% (SN-10%) can be continuously cycled without short circuit at 0.2 mA cm–2 for about 340 h. Moreover, a high reversible discharge capacity of 150.2 mAh g–1 at 0.5 C was maintained by the cell (LiFePO4/SCE SN-10%/Li) after 269 cycles at room temperature. Notably, a capacity of about 100 mAh g–1 at 5 C was also obtained. This work might guide the improvement of future solid-state lithium/sodium metal batteries and lithium–sulfur batteries, even for wearable flexible batteries.
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DOI
高影响因子
COMPOSITES SCIENCE AND TECHNOLOGY
·
2021
·
IF 8.528
Fangyan Zhu,Samson Ho-Sum Cheng,Yi Xu,Wenchao Liao,Kangqiang He,Dazhu Chen,Chengzhu Liao,Xin Cheng,Jiaoning Tang,Robert K.Y. Li,Chen Liu
The polymer composite electrolytes, especially garnet ceramic Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 reinforced polyethylene oxide (PEO), are expected to be the most promising substitute for commercial liquid electrolytes in lithium metal batteries due to their good safety, easy-manufacturing and flexibility. However, their insufficient ionic conductivity and instability towards reductive Li anode at room temperature are the long-standing issues. In this work, a dual-salt solid composite electrolyte with superior ambient-temperature electrochemical performance is designed by regulating polyethylene oxide/lithium perchlorate/Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 composite electrolyte with additive lithium tetrafluoroborate (LL@PL). The stable solid electrolyte interphase with LiF, B–F, and Li–B–O formed on lithium metal effectively induces even Li deposition and strengthens the compatibility of electrolyte/Li anode interface. The combined action of each composition in the electrolyte guarantees the efficient ion immigration kinetic and suppresses the lithium dendrite growth of solid-state batteries. The Li symmetric cells using [email protected] can steadily cycle for 1700 h without short circuit. An 80% capacity retention is achieved for LiFePO 4 | [email protected] |Li cell after 350 cycles at 25 °C. The electrochemical stability of the composite electrolyte is extended to 4.6 V and the assembled cell works well with LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode. This study proposed a promising polymer composite electrolyte for solid-state lithium metal batteries with superior performance.
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DOI
高影响因子
Applied Materials Today
·
2022
·
IF 8.663
Jiawen Sun,Meng Tian,Hongchun Dong,Zhengyi Lu,Lin Peng,Yi Rong,Ruizhi Yang,Jie Shu,Chao Jin
Developing solid state lithium batteries (SSLBs) is an essential step to overcome current safety and energy density issues of traditional Li-ion batteries. As the core component of SSLBs, a solid electrolyte with high ionic conductivity, great physical and chemical properties is still under exploration. Herein, a novel “polymer in ceramic” composite polymer-ceramic electrolytes (CPEs) is reported, which is composed of a polyether sulfone (PESF) polymer and cubic Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) ceramic with high contents (up to 80 wt. %). The as-prepared PESF-LLZTO CPEs possess good heat resistance and high mechanical strength to maintain structural integrity. The optimized 0.2PESF-0.8LLZTO CPEs exhibits an excellent ionic conductivity of 4.13×10 −4 S cm −1 with a t Li + value as high as 0.64 at 20 °C after wetted by trace wetting agent (6.0 ul cm −2 ). More impressively, the ionic conductivity is still reached 1.49×10 −4 S cm −1 at -10 °C and 9.42×10 −4 S cm −1 at 80 o C. Meanwhile, the 0.2PESF-0.8LLZTO CPEs shows a broad electrochemical window (≤4.8 V vs. Li + /Li) and an excellent compatibility with Li metal. Density functional theory calculations and 6 Li solid-state NMR characterizations suggest that strong interactions among LLZTO, PESF and wetting agents contribute to the enhanced conductivity. As a proof for practical application, the Li||0.2PESF-0.8LLZTO CPEs||LiFePO 4 full cells deliver a specific discharge capacity of 133.2 mAh g −1 at 2.0 C, and successfully run over 80 cycles at 0.5 C without capacity attenuation at 20 °C. The full cell also demonstrates a possibility for the application at low temperature down to -10 o C and high temperature up to 60 o C. This work brings a new perspective for high-performance SSLBs.
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Rong-Ao Tong,Linhui Chen,Gang Shao,Hailong Wang,Chang-An Wang
With the increasing demand for higher energy density Lithium-ion batteries, the battery safety issue has gained growing attention. Solid-state electrolytes (SSEs) are considered a promising solution to the volatilization and inflammable problems of the traditional liquid electrolytes . In this work, we propose a novel solvent-free modification process using stearic acid as a modifying agent for LLZTO/PEO hybrid electrolytes. Compared to the conventional solvent-casting process, the new one integrates surface modification and composite in a successive solvent-free step, so it can greatly improve the process efficiency and meet the requirement of green chemistry. Fourier Transform Infrared spectrometry (FTIR), X-Ray Diffraction (XRD) and Transmission Electron Microscope (TEM) observation confirm the structure of the uniform coating layer . The solvent-free modification and composite process are proved to significantly inhibit the agglomeration of LLZTO particles and the side reactions on particle surfaces in the polymer matrix by using Scanning Electron Microscope (SEM) and Thermal Gravimetric-Differential Thermal Analysis (TG-DTA) characterization. Thus, the prepared electrolyte has the ionic conductivity of up to 8.3 × 10 −4 S cm −1 at 70 °C. It has better electrochemical stability as well, which can achieve about 900 cycles in Li symmetric cells with a current density of 0.1 mA cm −2 .
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Tao Wang,Xiaoyan Liu,Ling Xie,Yuyu He,Haining Ji,Liping Wang,Xiaobin Niu,Jian Gao
The application of solid-state electrolyte in lithium metal batteries is a promising technology to meet the demands for next-generation high-energy-density storage systems. Poly (ethylene oxide) (PEO)-based solid polymer electrolytes have been widely studied, but their electrochemical window is too narrow to be compatible with high-voltage cathodes and their mechanical properties are poor as well. Combination of organic and inorganic compounds is an effective approach to solve this limitation. In this study, Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) was surface-modified with a silane coupling agent and compounded with polyacrylonitrile (PAN) to form a 3D nanofiber framework via electrospinning technology, and the PEO-Succinonitrile (SN)-LiTFSI solution was uniformly dispersed in the 3D nanofiber framework to form a continuous Li + transport path. The prepared composite solid electrolytes (CSEs) showed high ionic conductivity (1.58 × 10 −4 S cm −1 at room temperature), a broad electrochemical window (5.1 V, vs. Li/Li + ), and an attractive mechanical strength of 49.4 MPa. In addition, solid-state Li/CSE/NCM811 batteries exhibited high coulombic efficiency and significant stable cycling performance.
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Da Yang,Yaning Liu,Tianqi Yang,Ruyi Fang,Zhen Xiao,Wenkui Zhang,Xinping He,Yongping Gan,Jun Zhang,Xinhui Xia,Hui Huang,Yang Xia
Non-flammable butanedinitrile (SN) is recognized as a highly prospective plasticizer for significantly reducing the operating temperature of polyethylene oxide (PEO)-based solid polymer electrolytes. However, the instability of the lithium anode interface severely hinders the practical application of PEO/SN-based solid polymer electrolytes in room-temperature solid-state lithium metal batteries. In this work, we propose fast-ion conductive Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) nanoparticles as corrosion inhibitors to constructure a multifunctional buffer layer on the surface of PEO/SN-based solid electrolyte (PSE@LLZTO) to stabilize the interface structure of Li anode via a facile spin-coating transfer technique. This LLZTO modified buffer layer with rigid inorganic LLZTO phase and soft organic PEO-LiTFSI phase, not only significantly homogenizes lithium deposition, but also effectively improves the resistance to dendrite formation. Impressively, the LLZTO phase is able to adsorb free SN molecules, preventing them from continuously corroding the Li anode, thereby significantly reinforcing the interface stability. Meanwhile, these rigid LLZTO ceramic particles effectively inhibit lithium dendrite growth. Consequently, the Li symmetric cell demonstrates consistent performance for 1600 h at room temperature, and the LiFePO 4 |PSE@LLZTO|Li cells exhibit a high reversible specific capacity of 146 mA h g −1 with a remarkable capacity retention of 98.4 % after 200 cycles under 0.5C at room temperature. This study offers a feasible approach for the practical utilization of PEO/SN-based solid electrolyte systems in long lifespan solid-state lithium metal batteries.
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产品关联
DOI
PubMed
高影响因子
Small
·
2025
·Vol. 21
·期 40
·e01766
·
IF 12.1
Jinhu Wang,Ziqiang Wu,Kaiwen Wang,Zhuoqi Gong,Yihao Hu,Yao Zhang
Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) solid electrolyte, renowned for its high ionic conductivity and robust safety profile at room-temperature, holds tremendous promise for diverse applications. However, it faces significant challenges, including high interface impedance with lithium and a propensity for lithium dendrite formation. To address these issues, a novel Li 4 (BH 4 ) 3 I/2(d-BN) (LBHIbn) composite buffer layer — exhibiting high ionic conductivity and critical current density — is introduced at the LLZTO|Li interface. Theoretical calculations reveal that LBHIbn, serving as a protective layer of LLZTO, possesses a lower interface energy (0.366 J m −2 ) against lithium metal compared to LiBH 4 (0.434 J m −2 ). Consequently, at 30 °C, the interface impedance of the LLZTO | LBHIbn | Li system is significantly reduced to 4 Ω cm −2 . Simultaneously, the critical current density increases from 0.93 mA cm −2 of LLZTO | Li to 5.29 mA cm −2 (for LLZTO-LBHIbn | Li) with stable lithium-ion plating/stripping cycling demonstrated over 1000 h. Unlike conventional metal-based buffer layers that suffer from limited ionic conductivity, LBHIbn uniquely integrates high ionic conductivity (4.0 × 10−⁴ S cm −1 ) with superior electronic insulation (1.9 × 10−⁹ S cm −1 ), achieving simultaneous reduction of interfacial resistance (4Ω cm 2 at 30 °C) and effective suppression of lithium dendrite growth. This study demonstrates that the LBHIbn interface treatment effectively mitigates the interfacial issues between the LLZTO electrolyte and lithium anode, thereby expanding the potential applicability of hydride and oxide electrolyte materials in all-solid-state batteries
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Yiping Gu,Qi Wei,Yun Hong,Ze Ma,Zihua Wang,Tao Zhang,Xiaoyu She,Wei Lu
Composite polymer electrolytes (CPEs) based on poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) are regarded as promising electrolyte systems for developing high-energy-density solid-state lithium batteries. However, the combination of ceramic fillers and the polymer matrix often leads to poor lithium metal interface stability and limited ion transport. Here, we constructed phosphated LLZTO/PVDF-HFP CPEs synergistically regulated by a dual-salt (LiTFSI-LiBOB) and fluoroethylene carbonate (FEC). Surface phosphation of LLZTO reduces interfacial side reactions, LiBOB alleviates interfacial corrosion at the cathode/Al current collector, while FEC and dual-salt synergistically facilitate the formation of a robust SEI layer and suppress SN-induced nitrile polymerization side reactions. The electrolyte exhibits a wide electrochemical window (5.0 V), a low activation energy (0.285 eV), and an excellent Li + transference number (0.62). Besides, the assembled Li|PHL-DLi-FEC|Li cell exhibits the lifespan of over 1000 h at 0.2 mA cm −2 at both 25 °C and 60 °C. The assembled LiFePO 4 (LFP) |PHL-DLi-FEC|Li cell displays an initial capacity of 144.6 mAh g −1 , 91.9% capacity retention after 500 cycles under 0.5 C, and approaching 100% coulombic efficiency after 500 cycles at 1 C. This work offers new insights into composite polymer electrolytes with stable dual interfaces for solid-state batteries.
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产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Qingya Guo,Fanglin Xu,Lin Shen,Zhiyan Wang,Jia Wang,Hao He,Xiayin Yao
Polyethylene oxide (PEO)/Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) composite solid electrolyte is considered as a promising electrolyte for lithium batteries . However, LLZTO nanoparticles tend to agglomerate in PEO/LLZTO composite polymer electrolyte due to interfacial incompatibility between PEO and LLZTO nanoparticles , which leads to low ionic conductivity , poor interface stability with the electrode, and inferior batteries cycling stability. In order to enhance interfacial compatibility, herein, LLZTO nanoparticles are modified through firstly surface-functionalizing by dopamine coating and then grafting poly (ethylene glycol) (PEG) brush on it via amino and epoxy reaction. As a consequence, the ionic conductivity of LLZTO/PEO composite polymer electrolyte filled with 2 wt% modified LLZTO increases up to 1.1 × 10 − 4 S cm −1 , which is about twice and 20 times in comparison with LLZTO/PEO filled with 2 wt% unmodified LLZTO and PEO electrolytes, respectively. Moreover, high oxidation potential of around 4.8 V and ionic transference number of 0.34 as well as good interface stability with lithium anode are also achieved. Thus, LiFePO 4 ||Li all-solid-state lithium metal batteries based on LLZTO/PEO composite polymer electrolyte filled with 2 wt% modified LLZTO exhibit excellent cyclic stability of 152.3 mAh g −1 with capacity retention of 90.35% at 0.5 C after 500 cycles under 60 °C.
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高影响因子
危险品化学品经营许可证（带存储）