Nanomaterials
·
2022
·Vol. 12
·期 19
·3390
·
IF 5.719
Xinghua Liang,Yujuan Ning,Linxiao Lan,Guanhua Yang,Minghua Li,Shufang Tang,Jianling Huang
The stability and wide temperature performance range of solid electrolytes are the keys to the development of high-energy density all-solid-state lithium-ion batteries. In this work, a PVDF-HFP-LiClO4-Li6.4La3Zr1.4Ta0.6O12(LLZTO) composite solid electrolyte was prepared using the solution pouring method. The PVDF-HFP-LiClO4-LLZTO composite solid electrolyte shows excellent electrochemical performance in the temperature range of 30 to 60 °C. By assembling this electrolyte into the battery, the LiFePO4/PVDF-HFP-LiClO4-LLZTO/Li battery shows outstanding electrochemical performance in the temperature range of 30 to 60 °C. The ionic conductivity of the composite electrolyte membrane at 30 °C and 60 °C is 5.5 × 10−5S cm−1and 1.0 × 10−5S cm−1, respectively. At a current density of 0.2 C, the LiFePO4/PVDF-HFP-LiClO4-LLZTO/Li battery shows a high initial specific discharge capacity of 133.3 and 167.2 mAh g−1at 30 °C and 60 °C, respectively. After 50 cycles, the reversible electrochemical capacity of the battery is 121.5 and 154.6 mAh g−1at 30 °C and 60 °C; the corresponding capacity retention rates are 91.2% and 92.5%, respectively. Therefore, this work provides an effective strategy for the design and preparation of solid-state lithium-ion batteries.Keywords:lithium-ion battery;solid-state electrolyte;composite;electrochemical performance
研究领域:
材料科学
·
电化学
·
电池技术
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DOI
PubMed
高影响因子
Ceramics-Switzerland
·
2025
·Vol. 8
·期 4
·132
·
IF 2
Chengjian Li,Frank Kern,Lianmeng Liu,Christopher Parr,Andreas Börger,Chunfeng Liu
Garnet-type Li7La3Zr2O12(LLZO) is a solid electrolyte candidate for ASSLBs, owing to its wide electrochemical window and intrinsic safety. Yet phase-pure LLZO remains difficult because secondary phases form, and the transition towards the tetragonal phase, aliovalent doping, mitigates these issues. Still, the phase formation pathway is not fully understood. Here, we present comparative in situ and ex situ studies of Nb- and Ta-doped LLZO (LLZNO and LLZTO) that were synthesized by a solid-state reaction. In situ/ex situ XRD reveals that the lithium precursor dictates the reaction path: differing decomposition temperatures of the lithium precursor define reaction windows that control cubic-phase purity and particle morphology. In air, limited Li diffusion favors oxycarbonates and pyrochlore, necessitating 950–1050 °C to achieve phase-pure cubic LLZO. Under N2, faster Li availability and diffusion enable uniform nucleation and a route to cubic LLZO without detectable secondary phases. These findings demonstrate the coupled effects of temperature, precursor, dopant, and atmosphere, guiding process optimization and scalable production.
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SOLID STATE IONICS
·
2024
·
IF 3
Heng Pan,Lingcong Fan,Yongxi Zhang,Lei Zhang,Ying Shi,Jianjun Xie,Fang Lei
Garnet-type electrolytes are regarded as one of the most promising solid-state electrolytes (SSEs) for lithium-ion batteries due to their potential advantages in terms of energy density , electrochemical stability and safety. To achieve the maximum energy density, it is necessary to ensure that the electrolyte layer is as thin as possible. Nevertheless, thin sheet SSE is more challenging to sinter than pellet due to the greater lithium volatilization from the high surface/volume ratio. Garnet-type SSE (Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 , LLZTO) green tape was prepared by the tape-casting technique. The effects of supporter, sintering temperature and dwell time on the relative density, microstructure and ionic conductivity of thin sheet were investigated. A ceramic SSE sheet with a thickness of 173 μm, a relative density of 97.2 %, an ionic conductivity of 2.02 × 10 −4 S/cm at 25 °C and an activation energy of 0.25 eV, was achieved using a rapid pressureless sintering at 1250 °C for 25 min with a MgO supporter. This work offers insights into the practical production of LLZTO sheets.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Yuchen Cong,Jing Li,Haiping Su,Yazhuo Shang,Honglai Liu
Solid polymer electrolytes have emerged as one of the most promising solid electrolytes due to their excellent flexibility and interfacial contact. However, their practical applications are hindered by low ionic conductivity and Li dendrite growth. Herein, metal–organic framework (ZIF-67) modified Li6.4La3Zr1.4Ta0.6O12 (LLZTO) were used as nanofillers (LZ) for PEO-based composite solid polymer electrolytes (CSPE). The electrospinning method was applied to promote the uniform dispersion of LZ particles in the film that helps to construct continuous Li+ transport channels. In addition, the ZIF-67 interact with both ether oxygen in PEO and anion in Li salt and can release more free lithium ions, thereby significantly enhancing the ionic conductivity (1.39 × 10–4 S cm–1, RT) and the Li+ transference number (0.62). The Li/Li symmetric cell continuously cycled without short-circuiting for a long duration over 2000 h, proving the high interface stability of Li-solid electrolyte. The Li/CSPE-LZ/LiFePO4 full cell delivered an initial discharge capacity of 154.3 mA h g–1 at 1 C, with a capacity retention rate of 95.4% after 220 cycles, demonstrating the feasibility of this CSPE for high performance all-solid-state lithium metal batteries.
研究领域:
材料科学
·
电化学
·
能源存储
·
高分子化学
·
固态离子学
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高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 27
·16425-16436
·
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
·
电化学
·
能源存储
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高影响因子
Small
·
2023
·Vol. 19
·期 46
·2305326
·
IF 13.3
Shida Xue,Shiming Chen,Yanda Fu,Hengyao Zhu,Yuchen Ji,Yongli Song,Feng Pan,Luyi Yang
Composite solid electrolytes (CSEs) consisting of polyethylene oxide (PEO) matrix and active inorganic fillers have shown great potential for practical applications. However, mechanisms of how different active fillers enhance ion transport in CSEs still remain inconclusive. In this work, the component dependencies of ionic conductivity of PEO-based CSEs are investigated by comparing two widely investigated active fillers: NASICON-type (LATP) and garnet-type (LLZTO). In terms of ionic conductivity, the optimum ratios are strikingly different for LLZTO (10 wt%) and LATP (50 wt%). Through experimental and computational studies, it is demonstrated that the high affinity between LATP and PEO facilitates unhindered interfacial Li + transfer so that LATP functions as a bulk-active filler to provide additional inorganic ion pathways. By contrast, Li + transfer between LLZTO and PEO is found to be sluggish. Instead, LLZTO mainly improves ionic conductivity by dissociating lithium salt, making it a surface-active filler. Through categorizing active fillers based on their Li + conductive mechanisms, this work provides new understanding and guidelines for componential design and optimization of solid composite electrolytes.
研究领域:
材料科学
·
电化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Yanhua Zhang,Xinglong Gao,Yuhang Mei,Zijun Tang,Dawei Luo,Jiadong Deng
The instability of Ta-doped Li 7 La 3 Zr 2 O 12 (LLZTO) solid electrolytes with Li anode has severely restricted the development of all-solid-state lithium batteries. Herein, a simple interlayer of graphite is constructed at the Li/LLZTO interface with pencil, and the electrochemical stability of the battery has been significantly improved. Results show that the internal resistance of battery modified by 2B type graphite interlayer is reduced more than 2 orders of magnitude than that of the unmodified battery. And the battery has good cycling stability at current density of 0.1 mA cm −2 with polarization voltage< 0.01 V after 200 cycles. Besides, it also has excellent high-current discharge performance in the range of 0.1 mA cm −2 ∼ 0.6 mA cm −2 with polarization voltage close to 0 V. SEM showed that before galvanostatic charge-discharge (GCD) cycle, the morphology of the surface graphite is lamellar, while it is irregular granular shape and appeared at the grain boundary of LLZTO solid electrolyte after GCD cycle. Raman and XPS results shows that a LiC 6 compound is formed after GCD cycle, which locally form LiC 6 /LLZTO/LiC 6 microbatteries, where Li + can spontaneously diffuse in the in-situ lithiated graphite layer, thereby enhancing the electrochemical performance of the battery.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Open Ceramics
·
2025
·
IF 2.8
Chengjian Li,Frank Kern,Lianmeng Liu,Christopher Parr,Andreas Börger,Chunfeng Liu
Garnet-type Li₇La₃Zr₂O₁₂ (LLZO) is a promising solid electrolyte for all-solid-state batteries due to its high ionic conductivity and excellent thermal stability. However, production of high performance LLZO remains constrained by the reliance on high-purity reagents and complex synthesis routes. This study presents a cost-effective strategy to prepare high-performance Ta- and Nb-doped LLZO using commercially sourced raw materials via conventional solid-state reaction. Two lithium precursors, Li 2 CO 3 and LiOH·H₂O, were systematically compared to evaluate their impacts on formation and performances of LLZO. LiOH-derived powders showed higher phase purity and finer morphology, while Li 2 CO 3 -derived powders offered better processability. While the LLZNO-LOH sample achieved 94.4% relative density and 0.78 × 10⁻ 3 S/cm conductivity, LLZTO-LCO also reached 0.75 × 10⁻ 3 S/cm with a relative density of 94.1%. All sintered samples exhibited phase-pure cubic garnet structures. These findings demonstrate the industrial feasibility of LLZO production, paving the way for its practical deployment in next-generation solid-state batteries.
研究领域:
材料科学
·
电化学
·
固态化学
·
储能技术
·
陶瓷材料
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yunqi Gao,Chengliang Wang,Hairui Wang,Changhao Feng,Hongwei Pan,Zhenpeng Zhang,Jianjiang He,Qingfu Wang
Liquid electrolytes are prone to leaks and fires, which is exacerbated in Li metal batteries (LMBs) because of dendrite formation. Solid polymer electrolytes (SPEs) with their tunable mechanical properties and easy manufacturability, are increasingly becoming the preferred choice to address the interface issues in LMBs. However, their electrochemical instability against lithium-metal, mediocre conductivity and poorly interphases between Li and SPEs have prevented extensive application in LMBs. In this study, guided by theoretical calculations, an organic–inorganic composite solid-state polymer electrolyte (LPCU) based on Polyurethane (PU) and Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) was designed, and showed no lithium dendrite penetration after 500 h of cycling. The addition of LLZTO makes up for the deficiency of lithium ion coordination environment in PU matrix and improve electrochemical performances of LPCU electrolytes. Owing to the room-temperature ionic conductivity of 2.22 × 10 −4 S cm −1 , the transference number of 0.55 and the improved contact interface of Li-SPE, the optimized LPCU with a LLZTO content of 4% could achieve 150.0 mAh/g with 90% retention capacity after 150 cycles at 1C rate and 60 °C for Li||LiFePO 4 full batteries. This composite solid polymer electrolyte (LPCU) presents a powerful strategy for enabling the stable operation of LMBs.
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高影响因子
ACS Applied Energy Materials
·
2023
·
IF 6.4
Huihui Gan,Jiajun Sun,Ye Xia,Pengyuan Qiu,Liang Li,Wen Zhu
Functionalized separator is more competitive than commercial polyolefin separator for rechargeable lithium-ion batteries. In this work, we design the separator modified by a composite coating layer, which is composed of Li6.75La3Zr1.75Ta0.25O12 (LLZTO), poly(ethylene oxide) (PEO), poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP) and lithium bis(triuoromethanesulfonyl) imide (LiTFSI) (LLZTO-PEO/PVDF-HFP/LiTFSI, LLZTO-PPL). The LLZTO-PPL composite coating layer gives an impressive effect on dendrite inhibition of lithium metal. In comparison with commercial polyolefin separator, smaller overpotential value and better Coulombic efficiency are observed for the Li/LLZTO-PPL/Li symmetric cells and the Li/LLZTO-PPL/Cu asymmetric cells at various current densities of 0.2, 0.5, and 1 mA cm–2. Moreover, the LLZTO-PPL composite coating layer modified separator exhibits better high-rate capability and cycle performance for these cells assembled with different kinds of cathode materials (LiFePO4, LiCoO2, and LiNi0.8Co0.1Mn0.1O2) and their counterpart of a lithium metal anode. The functionalized composite coating layer modified separator may be a more attractive candidate material for commercial lithium-ion batteries.
研究领域:
材料科学
·
电化学
·
储能
·
电池技术
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DOI
高影响因子
Nano Research
·
2019
·Vol. 12
·期 10
·2543-2548
·
IF 8.515
Wang Rui,Zhang Xuejing,Cai Yichao,Nian Qingshun,Tao Zhanliang,Chen Jun
The rechargeable Li-CO 2 battery has been receiving significant attention owing to its merits of high energy density and the efficient utilization of CO 2 . However, the widely application is plagued by severe security risks, such as leakage, flammability and lithium dendrites growth due to the use of liquid organic electrolytes. Here, a composite solid state electrolyte consisting of polyethylene oxide (PEO) and 20 wt.% Li 7 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) was prepared and first introduced into Li-CO 2 battery to solve the problems. The composite solid state electrolyte exhibited high ionic conductivity (1.03 × 10 −1 S·cm −1 at 70 °C), wide electrochemical window (5 V vs. Li + /Li), good mechanical properties and excellent flexibility. Ultimately, the Li symmetric cell with PEO/LLZTO composite solid state electrolyte can operate 1,500 h at a current density of 0.1 mA·cm −2 . The assembled all-solid-state Li-CO 2 battery behaved a long cycle life of 70 cycles at a current density of 100 mA·g −1 with fixed capacity of 1,000 mAh·g −1 . Our work provides new perspective to develop rechargeable all-solid-state Li-CO 2 batteries.
研究领域:
材料科学
·
能源技术
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产品关联
DOI
高影响因子
ENERGY & FUELS
·
2026
·Vol. 40
·期 35
·19765-19777
·
IF 6
Yang Zhitao,Liu Yulei,Fu Xiuwen,Xu Weiheng,Liu Jinpeng
Poly(ethylene oxide) (PEO)-based solid polymer electrolytes
are
promising for solid-state lithium metal batteries because of their
favorable flexibility, processability, and lithium-salt solvation
capability. However, their practical application is still limited
by insufficient ion transport, a low lithium-ion transference number,
and poor lithium-metal interfacial stability. Herein, dual-lithium-salt-regulated
composite polymer electrolytes (DSCPEs) were constructed by incorporating
a LiTFSI/LiDFOB dual-salt system into a PEO–LLZTO composite
polymer electrolyte matrix to achieve a balance between ion transport
capability and lithium-metal interfacial stability. The optimized
DSCPE-2 (LiTFSI:LiDFOB = 3:2) delivers an ionic conductivity of 6.63
× 10 –4 S cm –1 , a lithium-ion
transference number of 0.69, and an electrochemical stability window
of up to 5.1 V. In addition, the Li|DSCPE-2|Li symmetric cell operates
stably for over 2000 h at 60 ° C under 0.1 mA cm –2 , with a critical current density of 1.05 mA cm –2 , indicating its enhanced compatibility with lithium metal. When
assembled with a LiFePO 4 cathode, the Li|DSCPE-2|LFP full
cell delivers an initial discharge capacity of 136.54 mAh g –1 and retains 123.41 mAh g –1 after 300 cycles at
0.5 C and 60 ° C, corresponding to a capacity retention of 90.38%.
Furthermore, the cell maintains a reversible capacity of approximately
115 mAh g –1 even at 5 C. This work provides an effective
strategy for regulating ion transport behavior and lithium–metal
interfacial stability in PEO-based composite polymer electrolytes.
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