ACS Applied Energy Materials
·
2025
·
IF 5.5
Zhen Zeng,Shengnan Zhang,Jun Cheng,Yuanyuan Li,Hongqiang Zhang,Xuan Zhou,Haonan Wang,Lijie Ci,Deping Li
Composite solid electrolytes (CSEs) based on inorganic oxide electrolyte and organic polymer electrolyte are recognized as promising candidates to realize high-performance solid state Li metal battery. Although the ionic conductivity of CSEs is limited, the usage of a plasticizer can make a great difference. Due to the high conductivity and extraordinary resistance to electrochemical oxidation, succinonitrile (SN) is widely used as a plasticizer in CSEs. However, the influence of the compatibility between SN and conductive oxide ceramics is underrated. In this work, we solve the catalytic decomposition effect of Li7La3Zr2O12 (LLZO) toward SN by silane coupling agent coating. Due to good affinity and chemical bonding toward the organic phase, the coating layer can promote the Li+ exchange rate through the heterogeneous interface between the organic/inorganic phase and improve the ionic conductivity of CSEs. Besides, surficial carbonyl groups of LLZO introduced by a coating can regulate the Li+ coordination structure and accelerate the ion transport. Our design realizes a high conductivity of 5.9 × 10–4 S cm–1 at 30 °C and enables the cyclability of Li symmetric cell over 480 h at 0.1 mA cm–2. Besides, the full cell with LiFePO4 (LFP) as the cathode delivers a capacity of 137.6 mAh g–1 with a capacity retention of 96.1% after 150 cycles. Our work demonstrates the regulation effect of interfacial structure on the electrochemical performance of SN-based CSEs, which contributes to realizing a practical solid state Li metal battery.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2025
·
IF 3.8
Run Yu,Yongjin Chen,Chengyu Li,Shaojun Wang,Pengcheng Li,Ruihan Tang,Cong Gao,Chuanlong Lin,Xiang Gao
The garnet-type oxide Li 7 La 3 Zr 2 O 12 solid-state electrolytes (SSEs) are considered as a reliable option in all-solid-state lithium batteries (ASSLBs) due to its excellent properties. However, it still faces challenges such as limited ionic conductivity and low air stability. In this work, Ga 3+ and Ta 5+ co-doped samples Li 7−3 x − y Ga x La 3 Zr 2− y Ta y O 12 (Ga x Ta y -LLZO) synthesized via the solid-state method are demonstrated to stabilize the cubic phase, regulate the concentration of Li vacancies in LLZO, and improving the Li + transport channels. As a result, the Ga0.1Ta0.3-LLZO sample achieves a high conductivity of ∼1 mS cm −1 . Furthermore, we discovered that in addition to the previously reported effects of decreasing grain boundary density and the inert LiGaO 2 secondary phase at grain boundaries, the synergistic effect of introducing multiple dopant ions, which enhances lattice stability, is also a key factor contributing to improved air stability. Our findings demonstrate that co-doping strategy with Ga 3+ /Ta 5+ is an effective method for simultaneously enhancing conductivity and air stability of LLZO, laying solid foundation for the application of SSEs in ASSLBs.
研究领域:
材料科学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Bing Cheng,Peng Du,Jin Xiao,Xiaowen Zhan,Lingyun Zhu
Utilizing aluminum-doped nano LLZO (Li6.28La3Zr2Al0.24O12) as the ceramic filler, we synthesized and optimized LLZO/PVDF/LiClO4 composite polymer electrolytes (CPEs) to achieve high ionic conductivity and good interfacial stability with metallic lithium. The research examines how the PVDF grade and the mass ratio of PVDF to LiClO4 affect the ionic conductivity, lithium metal compatibility, and overall performance of CPEs. The CPE using Kynar PVDF 741 and a PVDF-to-LiClO4 mass ratio of 2:1 emerged as superior, displaying a high ionic conductivity at room temperature (0.12 mS/cm), the lowest activation energy (0.247 eV), an extensive electrochemical stability window (approximately 4.9 V), and robust mechanical strength. In tests with lithium metal symmetric cells, the membrane facilitated over 1000 h of stable cycling at 0.1 mA cm–2 and 0.1 mAh cm–2. Furthermore, when integrated into full solid-state lithium–metal batteries with LiFePO4 cathodes, it sustained more than 80% capacity retention across 500 charge/discharge cycles at a rate of 0.5 C with constantly high Coulombic efficiencies above 99.8%, underscoring its exceptional durability and efficiency. This research provides a practical framework and benchmarks for developing LLZO/PVDF-based CPEs with high ionic conductivity and enhanced stability against lithium metals.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
DOI
高影响因子
APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2021
·Vol. 128
·期 1
·1-12
·
IF 2.584
Liang Xinghua,Li Suo,Yang Guanhua,Wu Xi,Huang Dongxue,Ning Yujue,Luo JianGuo,Fang Zhijie
All-solid-state lithium batteries are considered to be the most promising electrochemical energy storage equipment due to their high safety, high energy density, and simple structure. However, the preparation of solid electrolytes with high lithium-ion conductivity and superior electrode–electrolyte interface contact is the development needs. In this study, the electronic structures of garnet-type Li 7 La 3 Zr 2 O 12 (LLZO) and Sb-doped LLZO electrolytes were investigated using the first-principles method based on density functional theory (DFT). Theoretical calculations have confirmed that elemental doping facilitates the migration of lithium ions in solid-state electrolytes at the micro-atomic level. Based on the theoretical calculations and analysis results, Li 6.7 La 3 Zr 1.7 Sb 0.3 O 12 (LLZSbO) with high ionic conductivity was synthesized by the conventional solid-state method. To reduce the interfacial impedance between electrolyte and electrode, the composite solid electrolytes (CSEs) containing LLZSbO active fillers were prepared by the solution casting method. The prepared CSEs exhibits a high ionic conductivity of 0.97 × 10 –4 S cm −1 at 30 °C and a stable electrochemical window of 5.3 V as well as the lithium-ion transference number up to 0.37. The all-solid-state battery using the CSEs prepared with 20 wt% LLZSbO has excellent rate performance and cycle stability. The initial discharge specific capacity can reach 148.4 mAh g −1 when the rate is 0.1 C. The capacity can cover 138.8 mAh g −1 after 100 cycles at 0.2 C with a capacity retention rate of 97.5%.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Xiaoyu Yang,Yanxia Liu,Dezhao Li,Jiayu Dong,Fengtao Chai,Baoyu Yang,Muhao Liu,Shuang Wang
PEO based solid electrolyte has high crystallinity, which seriously hinder the transport of lithium ions at room temperature, resulting in low ionic conductivity. In this paper, a high performance composite solid electrolyte membrane with LLZO@ZiF-67 as an inorganic filler and PEO as matrix was synthesized. The LLZO@ZiF-67 inorganic filler, which covered by in-situ synthesis of ZiF-67 layer on surface of LLZO, show a large specific surface area and a polyhedral structure. The introduction of LLZO@ZiF-67 effectively reduce the crystallinity of PEO, providing a continuous channel for the transport of lithium ions, which result in a ionic conductivity as high as 1 . 09 × 1 0 − 4 S cm −1 at room temperature of the composite electrolyte PLZ-20. Furthermore, the electrochemical stability and interface compatibility to lithium metal are improved. The lithium stripping/plating process at 0.1 mA cm −2 can maintain stable for more than 600 h without short circuit. In addition, the initial discharge capacity of the full battery (Li / PLZ-20 / LFP) can reach up to 141.1 mA h g −1 with retention of 91.45% after 100 cycles, which provide possibility for the application of high performance solid state battery.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Yuexin Shen,Xingyue Sun,Chenglin Zhang,Genxiang Zhu
In this work, we innovatively used the electrospinning method to prepare templates, which were then used in the template method to prepare Li 6.4 La 3 Zr 2 Al 0.2 O 12 (LLZO). By combining the advantages of electrospinning and template methods, we greatly expanded the source of template materials for the template method. Different template materials combined with electrospinning can obtain LLZO with different structures and performance. At the same time, we innovatively combined PVDF-based solid electrolyte with high concentration of LiTFSI with 3D LLZO framework. Using the complex formed by N-methyl pyrrolidone (NMP) and lithium ion (Li + ) as a charge carrier, unique lithium ion migration channels formed by high-concentration LiTFSI, and the joint effect of high-content LLZO, we obtained a composite solid electrolyte with excellent performance. It has high mechanical strength (1.4 MPa) and high Young's modulus (6.4 MPa), which effectively inhibits the growth of lithium dendrites. In addition, the composite solid electrolyte exhibits excellent ion conductivity at room temperature (2.07 ×10 −4 S cm −1 ), and a lithium symmetric battery can operate stably for at least 1000 h at 50 ℃. After 100 cycles at a current density of 0.5 C at 50 ℃, the remaining specific capacity of LiFePO 4 | 3D LLZO·CSE | Li was 141.9 mAh g −1 , and the capacity retention rate was 96.4%. Our research results show that this low-cost LLZO template manufacturing method, combined with the excellent performance of the obtained composite solid electrolyte, has great potential in energy storage direction.
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2023
·
IF 5.7
Guoqiang Zhao,Changwei Luo,Qingsong Hua
This paper elucidates the mechanism of BN as sintering additive and the enhancement for LLZO performance. The introduction of the sintering additive boron nitride (BN) to Li 6.25 Ga 0.25 La 3 Zr 2 O 12 (LGLZO) can effectively eliminate the insulating phase Li 2 CO 3 and form the liquid phase Li 3 BO 3 along the grain boundaries, which significantly enhances the relative density (from 72.4% to 92.9%), ionic conductivity (from 1.3 × 10 − 5 to 6.7 × 10 − 4 S cm − 1 ), mechanical strength (from 1.36 to 5.36 GPa) and air stability (anti-Li 2 CO 3 ) of the electrolyte. Density functional theory (DFT) results reveal that the formation of Li 3 BO 3 contributes to the improvement of the interfacial lithiophilicity, and the interface resistance is reduced from 1219 to 32 Ω cm −2 . The critical current density (CCD) is enhanced from 0.1 to 0.7 mA cm −2 , and the cells can be stably cycled for more than 1000 h at a current density of 0.2 mA cm −2 with a low overpotential at room temperature.
研究领域:
材料科学
·
电化学
·
能源存储
·
固体离子学
·
无机非金属材料
✓ 已验证
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Fei Chen,Yiluo Zhang,Qing Hu,Shiyu Cao,Shangbin Song,Xinqi Lu,Qiang Shen
Traditional liquid lithium-sulfur batteries have two key problems: poor safety and shuttle effect . These two challenges can be overcome by using solid-state electrolytes. But poor ionic and electronic conductivity due to solid/solid contact between the electrode and the electrolyte for all-solid-state lithium-sulfur batteries (ASSLSBs). Here, we have synthesized Li 6.4 Ga 0.2 La 3 Zr 2 O 12 (LLZO) conductive ceramics with high ionic conductivity . LLZO is used as the lithium-ion conductor and multi-walled carbon nanotubes (MWCNt) are used as the electronic conductor to form S/MWCNt/LLZO by the thermal diffusion method, resulting in an e − /S/Li + conductive network. The prepared S/MWCNt/LLZO composite material, composite solid electrolyte, and lithium metal are assembled into ASSLSBs. After 50 cycles, the high capacity of 825 mAh·g −1 is maintained with 72.62% capacity retention at 0.2C and 45 °C. The higher capacity indicates the success of forming a conductive network that can improve the electrochemical performance of ASSLSBs. At 0.2C, the capacity of the S/MWCNt/LLZO composite cathode remains at 873 mAh·g −1 after 60 cycles when the operating temperature is increased to 60 °C, indicating good cycle performance.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2023
·Vol. 27
·期 9
·2499-2507
·
IF 2.5
Wu Jiani,Lu Yan,Wu Huacheng,Luo Qian,Bai Zhe,Li Jun
All solid-state lithium batteries have been widely used in mobile communications and electric vehicles due to their high energy density, wide operating voltage, and long cycle life. However, solid-state electrolytes have shortcomings such as insufficient stability and low conductivity. In this study, the sol–gel method prepared the solid electrolyte Li 6.25 Al 0.25 La 3 Zr 2 Ti 0.25 O 12 co-doped with Al and Ti. The influence of Al and Ti on the structure and conductivity of Li 7 La 3 Zr 2 O 12 was investigated by X-ray diffraction, impedance spectroscopy, scanning electron microscopy, and inductively coupled plasma spectrometer (ICP). With optimal additions of Al and optimal additions of Ti, Li 6.25 Al 0.25 La 3 Zr 1.75 Ti 0.25 O 12 electrolyte calcined at 900 °C for only 6 h showed an ionic conductivity of 1.51 × 10 −4 S/cm at room temperature. Li/Li 6.25 Al 0.25 La 3 Zr 1.75 Ti 0.25 O 12 /LiFePO 4 all solid-state battery was assembled. The initial charge and discharge capacity of the lithium-ion phosphate positive electrode at 10 μA/cm 2 was 165.1 mAh/g and 130.1 mAh/g at room temperature. The initial coulomb efficiency was 78.9%. After 100 cycles, the discharge capacity was 149.1 mAh/g, and the capacity retention rate was 99.8% at room temperature.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Haoshan Xu,Shuhong Huang,Jiaqi Qian,Siming Liu,Ling Li,Xiaohui Zhao,Wenming Zhang
Herein, Li 7 La 3 Zr 2 O 12 (LLZO) ceramic nano-networks were introduced by electrostatic spinning into the polyethylene oxide (PEO)/thermoplastic polyurethane (TPU)/LiTFSI matrix (PTL) to constitute novel composite solid electrolytes due to the synergy between the nano-networks and the electrolyte matrix. By adjusting the LLZO nanonetwork with different weight ratios (5 wt%, 10 wt%, and 15 wt%) relative to the total weight of the PEO/TPU/LiTFSI/LLZO (PTLL) composite electrolyte, the electrochemical behavior of the gel electrolyte was optimized. When filled with a 10 wt% Li 7 La 3 Zr 2 O 12 nano-network, the PTLL has a maximum ionic conductivity of 1.33 × 10 −3 S cm −1 at 60 °C and an electrochemical stability window of 5.6 V. Furthermore, the LiFePO 4 /PTLL/Li battery presents an initial specific discharge capacity of 170 mA h g −1 at 0.1 C. After 100 cycles, it demonstrated superior cycle durability at 0.5 C at 60 °C, representing 96.1 % of the initial capacity. These results indicate that the PTLL electrolyte is a promising candidate for advanced solid state lithium batteries .
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Shenghan Li,Jiatang Wang,Feng Ji,Mingyin Wang,Zhenyuan Hu,Shikang Huo,Shuai Zhang,Hansong Cheng,Yunfeng Zhang
The interfacial compatibility between inorganic powder and polymeric matrix is one of the most important key factors for the applications of polymer ceramic composite electrolytes (PCCEs). In the present study, a surface modification strategy has been proposed by using three different terminating groups of silane coupling agents in the modification of the interfacial compatibility between LLZO and PEO in PEO/LLZO composite electrolyte. Experiments and density functional theory (DFT) calculations have been performed in studying the effect of different silane coupling agents on interfacial properties . Especially, the interface compatibility is found to be improved when using amino-terminated silane coupling agent KH550, which is due to hydrogen bond interactions between amino groups and PEO. In addition, the mechanical strength and conductivity are significantly increased by increasing the interaction energy and by decreasing the crystallinity , and the values of 1.39 MPa and 0.22 mS cm −1 at 30 °C are then successfully achieved. As a result, the solid-state LiFePO 4 |PCCE|Li battery demonstrates a high discharge specific capacity of 157 mAh g −1 at 60 °C and 1C. And it has a cycle capacity decay rate of only 0.034 % for 380 cycles. These results pave the way for future developments of high-performance PCCEs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Pengfei Pang,Yiran Bai,Hu Wang,Jiangchao Chen,Furong Zhang,Zhuoyan Yi,Yunyun Zhao,Kunpeng Jiang,Guisheng Zhu,Huarui Xu
The all-solid-state lithium batteries (ASSLBs) are widely acknowledged as the most promising candidate for energy storage devices due to their excellent safety features and high energy density. However, ASSLBs face significant challenges in terms of low ionic conductivity and the formation of lithium dendrites. Excitingly, composite solid-state electrolytes offer promising solutions to critical challenges. Here, we report a PEO-LiTFSI/LGLZTO organic-inorganic composite solid-state electrolytes (O-ICSEs). A high-performance Li 6.4 Ga 0.10 La 3 Zr 11.7 Ta 0.30 O 12 particles, co-doped with Ga and Ta, was incorporated into matrices of poly (ethylene oxide) (PEO) and lithium bis(trifluoro-methylsulfonyl)imide (LiTFSI) to establish a continuous pathway for the transportation of Li + . Additionally, the synergistic effect of Ga and Ta enhances the Li + transport capability within the LGLZTO particles. PEO-LiTFSI/LGLZTO O-ICSEs, which have fast ion transport channels, exhibit exceptional ionic conductivity (4.35 × 10 −4 S cm −1 at 60 °C) and possess a wide and stable electro- chemical window (5.5 V). The Li||PL(Ga 0.10 Ta 0.30 ) 25 ||Li cell demonstrates an outstanding cycle life exceeding 1000 h at a current density of 0.2 mAh cm −2 . The prominent electrochemical performance of PL(Ga 0.10 Ta 0.30 ) 25 O-ICSEs can primarily be attributed to their excellent electrode/electrolyte interfacial compatibility and effective suppression of Li dendrite growth. The proposed PL(Ga 0.10 Ta 0.30 ) 25 O-ICSEs offer a promising solution for designing highly efficient ASSLBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）