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.
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
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.
研究领域:
材料科学
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电化学
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储能技术
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固态电池
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聚合物纳米复合材料
✓ 已验证
DOI
高影响因子
RARE METALS
·
2023
·Vol. 43
·期 2
·692-701
·
IF 8.8
Lv Ying-Tong,Zhang Teng-Fei,Hu Zhao-Tong,Xia Guang-Lin,Huang Ze-Ya,Liu Zhen-Hua,Que Li-Hua,Yuan Cai-Ting,Guo Fang-Qin,Ichikawa Takayuki,Yu Xue-Bin
Garnet-type solid-state batteries (SSBs) are considered to be one of the most promising candidates to realize next-generation lithium metal batteries with high energy density and safety. However, the dendrite-induced short-circuit and the poor interfacial contact impeded the practical application. Herein, interface engineering to achieve low interfacial resistance without high temperature calcination was developed, which Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) was simply coated with complex hydride (Li 4 (BH 4 ) 3 I (3L1L)) in various mass ratios n (Li 4 (BH 4 ) 3 I)-(100− n )LLZTO (10 ≤ n ≤ 40). The interfacial conductivity increases by more than three orders of magnitude from 8.29 × 10 −6 S·cm −1 to 1.10 × 10 −2 S·cm −1 . Symmetric Li cells exhibit a high critical current density (CCD) of 4.0 mA·cm −2 and an excellent cycling stability for 200 h at 4.0 mA·cm −2 . SSBs with polymeric sulfur-polyacrylonitrile (SPAN) cathode achieve a high discharge capacity of 1149 mAh·g −1 with a capacity retention of 91% after 100 cycles (0.2 C). This attempt guides a simple yet efficient strategy for obtaining a stable Li/LLZTO interface, which would promote the development of solid-state batteries. Graphical abstract
研究领域:
材料科学
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电化学
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电池技术
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
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2022
·
IF 13.599
Xi Wang,Yong Wang,Yiyu Wu,Yunmiao Fan,Yang Tian
Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) solid garnet-type electrolyte has been widely reported due to its outstanding safety and electrochemical stability. However, the inherent rigidity and brittleness of LLZTO lead to poor contact with anode/cathode and the operation failure of full cells. Herein, the dual-interlayers are constructed as the fast interfacial ion-migration channel by using Ti 3 C 2 T x (MXene, T x is –O, –OH, –F) with trace ionic liquid (IL), which promote the intimate contact between LLZTO and anode/cathode and suppress Li-dendrites growth. Notably, IL can wet the cathode to promote intimate interface contact and be decomposed into some inorganic compounds (such as Li 3 N, LiF, and Li 2 S x ), resulting in reduced interfacial resistance and fast Li-ion transportation. Consequently, in the prepared Li-symmetric cell, the interfacial resistance on the anode side plunges to 33.1 Ω cm −2 , and stably maintains over 1000 h without short circuit at 0.05 mA cm −2 . The full cell of Li|LiFePO 4 delivers a high initial capacity of 158.52 mA h g −1 and outstanding retention of 90.18% after 100 cycles at 60 °C and 0.2 C. Our work provides an efficient strategy to design dual-interlayers between LLZTO and anode/cathode for the interfacial modification to enhance the performance of solid garnet batteries.
研究领域:
材料科学
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电化学
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固态电池
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界面工程
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能源材料
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 20
·2112113
·
IF 19.924
Zhonghui Gao,Yang Bai,Haoyu Fu,Jiayi Yang,Thimo Ferber,Junrun Feng,Wolfram Jaegermann,Yunhui Huang
Garnet-type Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTaO) is considered a promising solid-state electrolyte (SSE) for all-solid-state batteries (SSBs), but LLZTaO/Li interfacial issues limit their power density. The key question of whether LLZTaO does or does not form an interphase layer before and at the initial stage of electrochemical cycling remains debatable. An XPS interface approach, electrochemical cycling, and an electrochemically coupled phase field model to study the dynamic changes of interfacial resistance during cycling are utilized, and it is found that the generation rate of the interphase via electrochemical reaction processes at the LLZTaO/Li interface depends on the applied current density. For a Li/LLZTaO/Li cell, the impedance and overpotential increase gradually at the initial stage of electrochemical cycling at a current density of 0.1 mA cm –2 due to the formation of a passivating reaction zone (interphase) at LLZTaO/Li interface, which can protect the LLZTaO from being continuously reacted. With increasing the current density to 0.5 mA cm –2 , the electrochemical reaction is suppressed and tied to uneven Li ion transport across the LLZTaO/Li interface on plating, leading to a short circuit of the cell. Understanding how interface dynamic transformations influence electrochemical degradation is helpful to stabilize these interfaces in SSBs.
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
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 27
·16425-16436
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IF 10.733
Zeya Huang,Wanying Pang,Peng Liang,Zhehui Jin,Nicholas Grundish,Yutao Li,Chang-An Wang
A garnet-type solid-state electrolyte Li6.4La3Zr1.4Ta0.6O12 (LLZTO) was modified using dopamine to improve the wettability of LLZTO with PEO, allowing 80 wt% LLZTO to be uniformly dispersed in 20 wt% PEO/LiTFSI polymer electrolyte. Transmission electron microscopy and Fourier transform infrared spectroscopy confirmed a 4–5 nm thick polydopamine (PDA) layer coating on LLZTO nanoparticles. The composite LLZTO@PDA/PEO electrolyte was synthesized using a solvent casting method. The composite electrolyte has good compatibility and adhesion with both positive and negative electrodes of Li-ion batteries owing to the superior wetting capability of dopamine. This property allows for improved interfacial contact at the electrode/solid electrolyte interface which can decrease the overall resistance of the battery. With dopamine modification, the conductivity of the composite electrolyte at 30 °C increased from 6.3 × 10−5 S cm−1 to 1.1 × 10−4 S cm−1, and the interfacial resistance between the composite electrolyte and a metallic lithium anode decreased from 308 Ω cm2 to 65 Ω cm2 at 50 °C. The composite electrolyte also demonstrated improved thermal stability.
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
Energy Material Advances
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2022
·
IF 0
Qingya Guo,Fanglin Xu,Lin Shen,Shungui Deng,Zhiyan Wang,Mengqi Li,Xiayin Yao
The doped garnet-type solid electrolytes are attracting great interest due to high ionic conductivity and excellent electrochemical stability against Li metal. However, the thick electrolyte layer and rigid nature as well as poor interfacial contact are huge obstacles for its application in all-solid-state lithium batteries. Herein, an ultrathin flexible Li6.4La3Zr1.4Ta0.6O12- (LLZTO-) based solid electrolyte with 90 wt% LLZTO content is realized through solvent-free procedure. The resultant 20 μm-thick LLZTO-based film exhibits ultrahigh ionic conductance of 41.21 mS at 30°C, excellent oxidation stability of 4.6 V, superior thermal stability and nonflammability. Moreover, the corresponding Li||Li symmetric cell can stable cycle for more than 2000 h with low overpotential at 0.1 mA cm-2 under 60°C. The assembled Li||LiFePO4 pouch cell with integrated electrolyte/cathode interface exhibits excellent rate performances and cycle performances with a capacity retention of 71.4% from 153 mAh g-1 to 109.2 mAh g-1 at 0.1 C over 500 cycles under 60°C. This work provides a promising strategy towards realizing ultrathin flexible solid electrolyte for high-performance all-solid-state lithium batteries.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Zhiang Li,Shuai Liu,Hao Xu,Fan Ding,Weimin Wang,Kaikai Song,Ting Liu,Lina Hu
Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) is widely used in polyethylene oxide (PEO) based solid electrolytes preparation due to its high ionic conductivity, electrochemical stability towards lithium and excellent mechanical properties. However, agglomeration of LLZTO and the inert interfacial layer for Li + transport between LLZTO and PEO limit its application. Herein, we systematically study the effect of different contents of 1-methyl-1-propylpiperidinium bis(trifluoromethylsulfonyl)imide (denoted as PP13-TFSI) ionic liquid on PEO/LLZTO composite solid electrolytes (CSEs). PP13-TFSI, which provides a new pathway for Li + transport and promotes the uniform dispersion of LLZTO. By adjusting the proportion of PP13-TFSI reasonably, the agglomeration of LLZTO is weakened, the crystallinity of PEO is reduced, and the growth of lithium dendrites is also inhibited. Therefore, the CSEs with high ionic conductivity (2.03 × 10 −4 S cm −1 , 30 ℃) enhanced by PP13-TFSI. Li||Li symmetric batteries exhibit stable cycling up to 6000 h at 60 °C, and can cycle stably for up to 3000 h at 28 °C. LiFePO 4 ||Li full batteries exhibit high-capacity retention rate (≈ 90.5 %) after 500 cycles at 1 C. This work not only systematically study the effects of different contents of PP13-TFSI on CSEs, but also provide a simple composite solid electrolyte strategy.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
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2022
·
IF 7.336
Huirong Liu,Wei Feng,Mingliang Zhao,Jianling Li
The development of all-solid-state batteries has become an inevitable trend as safety is increasingly valued. Naturally, solid-state electrolytes(SSEs) have attracted extensive attention. The composite of superionic conductors and polymer is considered to be a material that can achieve both high energy density and safety. Nevertheless, the compatibility between the polymer and superionic conductors is poor due to the large differences in structure and electrochemistry, resulting in a high interfacial transport energy barrier of the cation. In this work, a functional Li x -CeO 2 (LCO) layer is synthesized on the surface of the superionic conductor. While broadening the cation transport path at the interface, the anion of lithium salt is successfully anchored and the concentration of lithium-ion is increased. In addition, the structural compatibility and adhesion between polymer and superionic conductors are improve. Compared with the pristine electrolyte, the ionic conductivity and the lithium-ion transference number (t Li+ ) of LLZTO@2%LCO are as high as 2.325 × 10 −3 S cm −1 (pristine sample is only 7.109 × 10 −5 S cm −1 ) and 0.44 (pristine sample is only 0.27)respectively. At 2C, the discharge specific capacity of LiFePO 4 (LFP)|LLZTO@2%LCO-CSE|Li can reach 134.8mAh g −1 . The outstanding performance of the composite electrolyte is attributed to the interface functionalized Li x -CeO 2 compound coating. Therefore, polymer/ceramic interface engineering to promote the interaction between the two components should be one of the directions of future research.
研究领域:
材料科学
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电化学
·
储能技术
·
固体离子学
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2018
·
IF 6.945
Wenping Zha,Fei Chen,Dunjie Yang,Qiang Shen,Lianmeng Zhang
In this work, the scalable ceramic-polymer composite electrolytes composed of Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 , poly (ethylene oxide), lithium bis(trifluoromethane)sulfonimide, and solid plasticizer succinonitrile are prepared in the form of flexible membranes. The ionic transport properties, electrochemical stability, and interfacial behaviors against lithium electrode of this electrolyte are systematically investigated. Among these electrolytes, the sample containing 60 wt.% Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 and 10 wt.% succinonitrile presents a maximum conductivity of 1.22 × 10 −4 S cm -1 at 30 °C, and exhibits a broadened electrochemical stability window of 5.5 V vs. Li/Li + . Moreover, the ionic transference number of this electrolyte is improved to 0.41, and the interfacial compatibility against lithium electrode is excellent under both static and dynamic conditions. Excellent cycling and rate performance of the Li/LiFePO 4 cells are resulted from the enhanced ionic transport properties and improved interfacial contact between electrolyte and electrodes. The cell run at 0.5C delivers a discharge specific capacity of 151.1 mAh·g −1 after 200 cycles under 60 °C, and retains 98% of the maximum specific capacity. Notably, this cell also can be successfully charged and discharged at 45 °C and still delivers a discharge capacity of 124.1 mAh·g −1 after 70 cycles at 0.5 C.
研究领域:
材料科学
·
能源技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Ran Wei,Yue Zhang,Jiameng Yu,Xinshui Zhang,Yining Zhang,Tianyi Gao,Yi Yu,Jie Zhao,Wei Liu
Ta-doped Li6.4La3Zr1.4Ta0.6O12 (LLZTO) for solid-state lithium batteries demonstrates encouraging performance; however, they encounter issues with lithium dendrite formation that impede their widespread use. Herein, we design a LLZTO ceramic with an interlayer containing a mixed dense layer of Ag and LLZTO, prepared by one-step sintering. The Ag-rich interlayer in LLZTO can hinder the growth and the penetration of lithium dendrites though the reaction between Ag and lithium metal. Compared with the Ag-free counterpart, a higher critical current density of 0.6 mA cm–2, in addition to a longer life span under a current density of 0.2 mA cm–2, is achieved by adopting the interlayer in LLZTO. This research offers novel insights into the engineering of garnet-based solid electrolytes, tailored for the advancement of high-rate lithium metal batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Wei Weng,Bin Liu,Weiwei Lin,Fanyou Zeng,Rui Mei,Feng Yan,Xinghua Zheng
As a promising candidate for solid-state electrolytes, garnet solid electrolyte Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) with high ionic conductivity and excellent electrochemical performance has attracted more and more attention due to the increasingly urgent safety and energy density concerns of lithium-ion batteries. However, there is still a big challenge to prepare the high-quality LLZTO ceramic electrolyte with fine grains, high ion conductivity and high density because of the serious Li-loss, porous microstructure and the abnormal grain growth during the long-time high-temperature conventional sintering process. Herein, Fe 2 O 3 as a sintering aid has been introduced to prepare the high-quality LLZTO ceramic electrolyte by low temperature sintering, which is an effective strategy to obtain high density and inhibit Li-loss. The densification behavior, phase composition, microstructure and electrochemical performance have been systematically investigated for LLZTO ceramics with different amount of Fe 2 O 3 additive. High density (ρ r = 94.7 %), high ionic conductivity of 6.82 × 10 −4 S cm −1 and low electronic conductivity of 9.09 × 10 −9 S cm −1 at 25 °C are achieved for the LLZTO-5 mol% Fe 2 O 3 ceramics sintered at the lower temperature of 1075 °C for 3 h. Meantime, the garnet electrolyte exhibits excellent electrochemical performance. Li/LLZTO-5 mol% Fe 2 O 3 /Li symmetric cell exhibits good stability after cycling more than 800 h at a current density of 0.1 mA·cm −2 . The LiFePO 4 /LLZTO-5 mol% Fe 2 O 3 /Li full cell delivers an initial discharge capacity of 115.2 mAh·g⁻¹ and retains a good capacity of 88 % after 80 charge-discharge cycles at 0.2 C. This suggests that the introduction of Fe 2 O 3 as a sintering aid provides a promising strategy of energy-saving, low-cost and high-efficient to achieve high-quality LLZTO-based solid electrolytes for advanced energy storage systems.
✓ 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）