Small
·
2026
·
IF 11.8
Bokang Liu,Shiyu Cao,Zhengyu Fu,Yawen Wu,Youfa Wang,Fei Chen
Solid-state electrolytes (SSEs) are regarded as promising candidates for high-energy-density lithium metal batteries (LMBs), but their practical application is severely hindered by lithium dendrite growth. Currently, numerous self-healing electrolytes are reported to suppress lithium dendrite growth. However, the self-healing functions reported so far are limited to repairing mechanical damage in the electrolyte membrane caused by lithium dendrite penetration; they cannot repair the lithium dendrites themselves. To address this, we utilize the hydrogen‑bond network formed by UPy‑UPy self‑assembly to design and prepare the composite electrolyte PEG‑UPy@LLZO. This electrolyte not only possesses the ability to self‑heal mechanical damage but also, for the first time, achieves active in‑situ self‑repair of lithium dendrites through the synergistic effect between the polymer and the ceramic filler. Experiments show that after a short‑circuit failure induced by lithium dendrites, the battery's charge‑-discharge function can be restored simply by letting it rest, without any external intervention. The Li symmetric cell exhibits stable cycling for over 1000 h at 0.2 mA cm −2 and 60°C. Furthermore, the LiFePO 4 (LFP) full cell maintains 75.36% capacity retention after 1000 cycles at 1C. This material-based active healing strategy provides a viable pathway to overcome the dendrite challenge in LMBs.
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DOI
PubMed
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Chenghao Zhao,Wei Wei,Zhiyi Li,Zhijun Liu
Composite solid electrolytes (CSEs) are promising alternatives to liquid electrolytes in lithium-ion batteries (LIBs). CSEs offer superior electrochemical stability, safety, and mechanical integrity. Herein, a flexible CSE film comprising aluminium-doped Li 6.28 La 3 Zr 2 Al 0.24 O 12 (LLZO – Al) and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF – HFP) is successfully fabricated via an optimised sol-gel synthesis and solution casting method. The LLZO – Al filler, with high cubic-phase purity, effectively reduces the crystallinity of the PVDF – HFP matrix, creating continuous Li + transport pathways. The optimised composite membrane containing 15 wt% LLZO – Al (CE15%) exhibits a high room-temperature ionic conductivity of 6.1 × 10 –4 S cm –1 and a broad electrochemical stability window up to 4.8 V vs. Li/Li + . Additionally, it demonstrates excellent mechanical flexibility (elongation at break: 162%) and enhanced thermal resistance. The Li/CE15%/Li symmetric cell maintains stable cycling for over 2000 h at 0.1 mA cm –2 , confirming outstanding interfacial stability. Furthermore, the LFP/CE15%/Li full cell delivers an initial discharge capacity of 166.1 mAh g –1 at 0.1 C and retains 86% of its capacity after 300 cycles. These results highlight the great potential of LLZO–Al/PVDF–HFP/LiTFSI composite electrolytes for high-performance solid-state Li-ion batteries.
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产品关联
DOI
高影响因子
Journal of Energy Storage
·
2023
·
IF 9.4
Yanan Teng,Huan Liu,Qi Wang,Yan He,YongChang Hua,Chunping Li,Jie Bai
Garnet type Li 7 La 3 Zr 2 O 12 solid electrolyte exhibits excellent thermal stability and high ionic conductivity, which is an ideal solid electrolyte. However, it is found that the cubic phase is a high conductivity phase and the synthesis condition is harsh. Therefore, low temperature synthesis and partial element substitution are expected to prepare cubic phase LLZO. In this paper, the LLZO cubic phase structure is stabilized by electrospinning technology and high-priced cation substitution strategy, and the transportation efficiency of lithium ions is improved. The experimental results show that LLZO NFs inorganic filler with stable cubic phase structure is obtained when the molar amount of In 3+ is 0.2. The In 3+ with large ion radius replaces the Li + inside the crystal, effectively increases the lithium vacancy concentration, and increases the Li + transport path inside the crystal, and successfully doubles the ionic conductivity of the composite solid electrolyte at 60 °C (9.39 × 10 −4 S/cm). The lithium ions migration number and electrochemical window were increased to 0.19 and 5.2 V respectively. With excellent cycle performance (60 °C), it can cycle 2000 cycles at a high rate of 0.5 C charge and discharge, and the Coulomb efficiency has been close to 100 %. Li|PL-LILZO NFs (0.2)|LFP all-solid-state lithium batteries can light small bulbs at room temperature and have practical application prospects. Therefore, in the composite electrolyte, the increase of the lithium ions pathway inside the active inorganic filler crystal will also improve the comprehensive performance of the composite electrolyte for preparation.
研究领域:
材料科学
·
能源科学
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2024
·Vol. 35
·期 9
·1-13
·
IF 2.8
Gong Zonggui,Wang Nanlan,Guo Haoxuan,Zhu Peishu,Wang Qijing,Yu Hang,Zhang Yu,Gao Min,Zheng Xinghua
Due to the increasingly urgent safety and energy density concerns of lithium-ion batteries, more and more attention has been attracted by the Li 7 La 3 Zr 2 O 12 (LLZO)-based solid electrolytes with high ion conductivity and chemical stability against Li-metal. However, to prepare the high-quality LLZO ceramic electrolyte with high-ion conductivity and density, there is still a big challenge of the serious “Li-loss” and the abnormal grain growth during the long-time high-temperature sintering process. A novel covered sintering method is put forward to prepare the high-quality Mo-doped LLZO (LLZMO) ceramic electrolyte. The sintering strategy effectively suppresses the Li-loss to obtain the LLZMO dense ceramics with cubic garnet phase and tight grain boundaries. The LLZMO ceramics sintered at lower temperature of 1050 °C for 2 h via the novel covered sintering exhibit high density ( ρ r = 92.3%) and high-ionic conductivity of 6.08 × 10 –4 S cm −1 at 25 °C, which are close to those of LLZO-based ceramics prepared by hot pressing sintering, ultrafast high-temperature sintering (UHS). The novel covered sintering provides an energy-saving, low-cost and high-efficient strategy to prepare the high-quality LLZO-based ceramics electrolyte.
研究领域:
材料科学
·
固态电解质研究
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DOI
高影响因子
Journal of Materials Chemistry A
·
2014
·Vol. 2
·期 33
·13277-13282
·
IF 0
Ru-Jun Chen,Mian Huang,Wen-Ze Huang,Yang Shen,Yuan-Hua Lin,Ce-Wen Nan
Li–La–Zr–O thin films were successfully fabricated using a sol–gel spin coating method, and the effects of altering the annealing temperature and the number of layers of the films on electrolyte conductivity were studied. Using X-ray diffraction, scanning electron microscopy and X-ray photoelectron spectroscopy, the characteristics of these films were investigated as a function of annealing temperature and the numbers of layers of the film. With these methods, an amorphous structure and a smooth surface on the films were revealed. The thin film's ionic conductivity was investigated by impedance analysis. The results show that the ionic conductivity of the films decreases with an increase of the annealing temperature, from 1.67 × 10−6 S cm−1 for 600 °C annealing to 8.53 × 10−7 S cm−1 for 800 °C annealing. The influence of film thickness on conductivity was investigated and the conductivity followed an inverse u-shaped curve with increasing film thickness. We propose that Li–La–Zr–O thin films may be promising solid electrolytes for solid-state lithium-ion batteries.
研究领域:
材料科学
·
能源存储技术
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产品关联
DOI
Nanoscale
·
2021
·Vol. 13
·期 16
·7822-7830
·
IF 7.79
Yuwan Dong,Panzhe Su,Guanjie He,Huiling Zhao,Ying Bai
With high theoretical capacity and tap density, LiCoO2 (LCO) cathode has been extensively utilized in lithium-ion batteries (LIBs) for energy storage devices. However, the bottleneck of structural and interfacial instabilities upon cycling severely restricts its practical application at high cut-off voltage. From another perspective, the compatibility between the electrode and electrolyte is highly valued in the development of all-solid-state batteries. Herein, we construct a compatible interface between Li7La3Zr2O12 (LLZO) and LCO through a facile surface modification strategy, which significantly improves the cycling stability of LCO at a high cut-off voltage of 4.5 V. Characterization results demonstrate that the LCO@1.0 LLZO sample delivers a desirable capacity retention of 76.8% even after 1000 cycles at 3.0–4.5 V with the current density of 1 C (1 C = 274 mA g−1). Further investigation indicates that the LLZO modification layer could protect the LCO electrode through effectively alleviating the side reactions, which not only facilitates the Li+ transportation at the interface but also mitigates the bulk structure degradation. Moreover, it is also established that a small amount of La and Zr ions could gradiently migrate into the surface lattice of LCO to generate a thin layer of the surface solid solution Li–Co–La–Zr–O. Thus formed pinning region between surface modified LLZO and LCO cathode could contribute both to their mechanical compatibility and Li+ kinetics behavior upon repeated cycling. This work not only provides a strategy in broadening the operation potential and extracting higher capacity of LCO but also sheds light on constructing compatible interfaces in LIBs, especially for all-solid-state energy storage and conversion devices.
研究领域:
材料科学
·
能源存储与转换
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Qiang Shen,Dongyu Jiang,Shiyu Cao,Xinqi Lu,Chong Mao,Xiaobing Dai,Fei Chen
High Li+ conductivity, good interfacial compatibility, and nano-scale particle size have always been essential conditions for selecting inorganic fillers in high-performance composite solid electrolytes. In this study, non-milled in situ LLZO fillers with nanosize was synthesized via the sol–gel method by rapid heating sintering, which resulted in more surface defects and fewer impurities in LLZO. Compared with milled LLZO fillers, these non-milled LLZO fillers with more surface defects and fewer impurities can effectively reduce the crystallinity of PEO and agglomeration in PEO, which can form composite electrolytes with high Li+ conductivity. Most importantly, the discharge capacity of the 7.5% non-milled LLZO–PEO-based LiFePO4/Li battery is about 135.5 mA h g–1 at 1C and 60 °C. After 100 cycles, the discharge specific capacity remains at 99%. It is worth noting that nano-sized non-milled LLZO will improve the discharge capacity of LiFePO4/Li batteries to 122.1 mA h g–1 at 0.2C and 30 °C.
研究领域:
材料科学
·
储能
·
固态电解质
·
锂离子电池
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DOI
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Jianan Zan,Wei Shan,Lu Guo,Kwun Nam Hui,Min Luo,Fuming Chen
The global transition to green energy has precipitated a surge in the demand for lithium resources. However, terrestrial lithium reserves are limited and unevenly distributed. While the ocean harbors abundant lithium, its ultralow concentration and the interference from high concentrations of background ions pose significant challenges for efficient extraction. This study introduces a strategy for lithium extraction from seawater, leveraging the synergistic effect of a flexible LLZO/PVDF-HFP composite membrane and a TEMPO redox couple. A cubic phase garnet-type Li6.5Ga0.25La2.75Ba0.25Zr2O12 (LLZO) solid electrolyte, prepared via a sol–gel method, was compounded with PVDF-HFP to create a flexible membrane with high lithium-ion selectivity. With integration into a redox flow device, the TEMPO redox couple drives the transmembrane migration of lithium ions. The effects of the applied voltage, TEMPO concentration, and operating time on the lithium extraction performance were systematically investigated. At an optimal constant voltage of 1.5 V, the lithium concentration in the enriched solution reached 20.6 times that of the initial seawater. The system demonstrated excellent selectivity with Li/Na, Li/Ca, and Li/Mg selectivity factors of 2309.3, 11164.2, and 3808.9, respectively. After 72 h of continuous lithium extraction, the Li+ concentration in the recovered solution reached 130.6 times that of the feed, with an average energy consumption as low as 34.1 Wh/g(Li). This research demonstrates a promising path for the development of low-cost, highly selective seawater lithium extraction technologies.
研究领域:
能源材料
·
电化学工程
·
可持续资源回收
·
膜技术
·
锂离子分离
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产品关联
DOI
PubMed
高影响因子
Cell Reports Physical Science
·
2023
·
IF 8.9
Chuan Shi,Jianjun Song,Yang Zhang,Xiuting Wang,Zhen Jiang,Tong Sun,Jinbao Zhao
Conductive filler-based solid polymer electrolytes are excellent candidates for the large-scale production of solid-state lithium-ion batteries. However, the transport and conduction mechanisms of lithium ions in such solid polymer electrolyte systems remain largely unrevealed. In this work, the results of in situ conductive atomic force microscopy demonstrate that lithium ions travel mainly through the Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZO) filler in polyethylene oxide (PEO)-based SPEs. The transport routes from LLZO into the polymer matrix can be greatly altered by adding succinonitrile (SCN). Combining experiment with ab initio simulations, we find that the adsorption affinity order for lithium ions is SCN > LLZO > PEO. Diffusion barriers are calculated for various composites, showing higher barriers for migration of lithium on the surface compared with in bulk. This work provides understanding of lithium affinity, diffusion barriers, and conductive mechanisms in solid polymer electrolytes, enhancing our understanding of mechanisms to guide future designs.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Materials Research Express
·
2020
·Vol. 7
·期 2
·025518
·
IF 1.929
Jiali Xue,Kuibao Zhang,Daimeng Chen,Jianjun Zeng,Baozhu Luo
Ta-doped Li7La3Zr2O12 (Ta-LLZO) solid electrolyte ceramics were synthesized by solid-state sintering, spark plasma sintering (SPS) and SPS plus heat-treatment (two-step method) using LiOH·H2O, La2O3, ZrO2 and Ta2O5 as the raw materials. The Ta-LLZO samples prepared from these three routes are all in cubic phase structure. However, the solid-state method results in Ta-LLZO samples with different particle sizes and porous morphology, while the samples prepared by SPS route contain fewer internal voids and smaller particle size. The two-step method not only retains the high compactness of SPS samples, but also the increment of grain size. The SEM results demonstrate that Ta-LLZO sintered by the two-step method shows optimal electrical properties. And the total ionic conductivity is 4.6 × 10−3 S cm−1 at 150 °C and the activation energy is calculated to be 0.38 eV.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2014
·
IF 5.211
Yanhua Zhang,Fei Chen,Rong Tu,Qiang Shen,Lianmeng Zhang
High performance lithium ion conducting Li 7 La 3 Zr 2 O 12 solid electrolytes are prepared for the first time by field assisted sintering technology (FAST). The effect of sintering temperature on the phase compositions , microstructure and Li ionic conductivity is systematically investigated. The results show that pure cubic phase LLZO can be obtained at a range of temperatures from 1100 to 1180 °C for no more than 10 min. For the sample sintered at 1150 °C, a maximum relative density of 99.8% with a total ionic conductivity as high as 5.7 × 10 −4 S cm −1 are obtained at room temperature . This value is the highest among the present research. Compared with the traditional preparation methods, the current FAST is very promising to obtain high performance LLZO for its advantages of very short sintering time , a single preparation step of reaction-densification processing, and relatively lower sintering temperature.
研究领域:
材料科学
·
能源科学
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DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Xiaohuan Meng,Haiping Liu,Liuyan Ji,Wenxiu Gao,Sifu Bi,Shanshan Fan,Chen Yang,Lixin Cao
As one of the main components of the cathode and electrolyte for Li thermal batteries (LTBs), conventional binders typically employ high thermal stability MgO to maintain LTBs structure stability, but MgO has the disadvantage of high resistance, which can result in a high resistance at the cathode-electrolyte interface. Thus, it is crucial to optimize the cathode-electrolyte interface for NiS 2 to achieve high performance LTBs. Herein, Li 7 La 3 Zr 2 O 12 (LLZO) with high thermal stability and excellent ionic conductivity was adopted in the cathode and electrolyte to replace the conventional binders, aiming to build a low resistance interface between the cathode and electrolyte, promoting the Li + transport kinetics. More importantly, LLZO also plays a vital role in reducing molten salt leakage and enhancing the stability of the cathode-electrolyte interface in LTBs, which contributed to increasing the discharge capacity of the NiS 2 cathode material. Consequently, LTB containing LLZO delivers a high discharge specific capacity of 635.1 mAh g −1 with a cut off voltage of 1.4 V at 100 mA cm −2 at 500 °C, retaining 72.8 % of the theoretical capacity of NiS 2 , which is 25.5 % higher than LTB with MgO. These findings indicate that optimizing the NiS 2 electrode and LLZO electrolyte interface would be an effective way to enhance the performance of LTBs.
研究领域:
材料科学
·
电化学
·
能源存储
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DOI
高影响因子
危险品化学品经营许可证（带存储）