Ionic conduction, colossal permittivity and dielectric relaxation behavior of solid electrolyte Li3La2/3-TiO3 ceramics

Yu, Kun; Tian, Ye; Gu, Rui; Jin, Li; Ma, Ruiping; Sun, Hongchen; Xu, Youlong; Wang, Chao; Wei, Xiaoyong

doi:10.1016/j.jeurceramsoc.2018.05.023

Cited by 52 publications

(23 citation statements)

References 37 publications

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“… The relatively high σ b of 1.65 × 10 −3 S/cm in this work could be due to the pure cubic structure and low porosity. By comparison, the grain‐boundary conductivity in literatures is very dispersed, and distributes from 6 × 10 −6 S/cm to 9.2 × 10 −4 S/cm Similar with the bulk σ b , σ gb was also influenced by composition, phase purity and porosity. However, σ gb was obviously affected by the grain size .…”

Section: Resultsmentioning

confidence: 89%

“…The bulk conductivity of similar compositions in the Li 3 x La 2/3‐ x TiO 3 systems was usually reported in the range of 1‐1.4 × 10 −3 S/cm, which was influenced by composition, phase purity and porosity. By optimizing sintering temperature, holding time and quenching process, a bulk conductivity as high as 1.8 × 10 −3 S/cm was also reported for Li 0.33 La 0.557 TiO 3.…”

Section: Resultsmentioning

confidence: 99%

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Electrochemical and mechanical stability of Li_xLa_0.557TiO_3‐δ perovskite electrolyte at various voltages

Yan

Cheng

et al. 2018

J Am Ceram Soc

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Perovskite LixLa0.557TiO3 electrolytes in all‐solid‐state lithium batteries are operated under a voltage gradient, which potentially induces the electrochemical and mechanical instability. To simulate the properties of LixLa0.557TiO3 (LLTO) under application relevant conditions, samples are charged (or discharged) to 0.2 V, 3.2 V, 4.0 V, and 4.5 V, respectively. The Li ion conductivity is 9.55 × 10−5 S/cm at 3.2 V and decreases obviously to 2.54 × 10−5 S/cm as the voltage increases to 4.5 V, whereas the value of the LLTO‐0.2 V is between that of LLTO‐3.2 V and LLTO‐4.0 V. In terms of mechanical behavior, elastic modulus (E), hardness (H), and fracture toughness (KIC) of LLTO operated at different voltages are also tested using depth‐sensitive indentation. The results can be used in the designing, monitoring and also improving of the battery cells.

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Section: Resultsmentioning

confidence: 89%

Section: Resultsmentioning

confidence: 99%

Electrochemical and mechanical stability of Li_xLa_0.557TiO_3‐δ perovskite electrolyte at various voltages

Yan

Cheng

et al. 2018

J Am Ceram Soc

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“…In recent years, various organic materials, as well as inorganic materials, have been studied as solid electrolytes for reversible lithium cells [1][2][3][4]. Among them, La 2/3-x Li 3x TiO 3 (LLTO) exhibits one of the highest bulk lithium ion conductivity, exceeding 1Á10 -3 S cm -1 at room temperature (RT) [5][6][7][8][9][10][11]. Taking into account its low electronic conductivity [6,12], simple synthesis and good sinterability [5,9,[13][14][15], as well as decent stability in air and at high redox potentials [13,16], LLTO can be considered as a promising solid electrolyte material for solid-state lithium batteries.…”

Section: Graphic Abstract Introductionmentioning

confidence: 99%

Mitigation of grain boundary resistance in La2/3-xLi3xTiO3 perovskite as an electrolyte for solid-state Li-ion batteries

et al. 2020

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In this work, we report that modification of the chemical composition of grain boundaries of La2/3-xLi3xTiO3 double perovskite, one of the most promising Li-ion conducting solid electrolytes, can be a convenient and versatile way of controlling the space charge potential, leading to a mitigated electrical resistance of the grain boundaries. Two groups of additives are investigated: lithium-enriching agents (Li3BO3, LiF) and 3d metal ions (Co2+, Cu2+), both expected to reduce the Schottky barrier. It is observed that Li-containing additives work effectively at a higher sintering temperature of 1250 °C. Regarding copper, it shows a much stronger positive impact at lower temperature, 1150 °C, while the addition of cobalt is always detrimental. Despite overall complex behavior, it is documented that the decreased space charge potential plays a more important role in the improvement of lithium conduction than the thickness of the grain boundaries. Among the proposed additives, modification of La2/3-xLi3xTiO3 by 2 mol.% Cu2+ results in the space charge potential reduction by 32 mV in relation to the reference sample, and the grain boundary specific conductivity increase by 80%, as measured at 30 °C. Introduced additive allows to obtain a similar effect on the conductivity as elevating the sintering temperature, which can facilitate manufacturing procedure. Graphic abstract

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“…The XRD patterns of all pellets are plotted in Figure 3 and match to a perovskite ABO 3 superstructure (tetragonal structure JCPDS #87-0935) ( Yu et al, 2018 ; Li et al, 2019 ). Figure 3A proves that the bulk structure of white LLTO remains unchanged after mixing G-LLTO and M-LLTO powder.…”

Section: Resultsmentioning

confidence: 93%

Engineered interfaces between perovskite La2/3xLi3xTiO3 electrolyte and Li metal for solid-state batteries

et al. 2022

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Perovskite La2/3xLi3xTiO3 (LLTO) materials are promising solid-state electrolytes for lithium metal batteries (LMBs) due to their intrinsic fire-resistance, high bulk ionic conductivity, and wide electrochemical window. However, their commercialization is hampered by high interfacial resistance, dendrite formation, and instability against Li metal. To address these challenges, we first prepared highly dense LLTO pellets with enhanced microstructure and high bulk ionic conductivity of 2.1×10−4 S cm−1 at room temperature. Then, the LLTO pellets were coated with three polymer-based interfacial layers, including pure (polyethylene oxide) (PEO), dry polymer electrolyte of PEO-LITFSI (lithium bis (trifluoromethanesulfonyl) imide) (PL), and gel PEO-LiTFSI-SN (succinonitrile) (PLS). It is found that each layer has impacted the interface differently; the soft PLS gel layer significantly reduced the total resistance of LLTO to a low value of 84.88 Ω cm−2. Interestingly, PLS layer has shown excellent ionic conductivity but performs inferior in symmetric Li cells. On the other hand, the PL layer significantly reduces lithium nucleation overpotential and shows a stable voltage profile after 20 cycles without any sign of Li dendrite formation. This work demonstrates that LLTO electrolytes with denser microstructure could reduce the interfacial resistance and when combined with polymeric interfaces show improved chemical stability against Li metal.

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Ionic conduction, colossal permittivity and dielectric relaxation behavior of solid electrolyte Li3La2/3-TiO3 ceramics

Cited by 52 publications

References 37 publications

Electrochemical and mechanical stability of Li_xLa_0.557TiO_3‐δ perovskite electrolyte at various voltages

Electrochemical and mechanical stability of Li_xLa_0.557TiO_3‐δ perovskite electrolyte at various voltages

Mitigation of grain boundary resistance in La2/3-xLi3xTiO3 perovskite as an electrolyte for solid-state Li-ion batteries

Engineered interfaces between perovskite La2/3xLi3xTiO3 electrolyte and Li metal for solid-state batteries

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Ionic conduction, colossal permittivity and dielectric relaxation behavior of solid electrolyte Li3La2/3-TiO3 ceramics

Cited by 52 publications

References 37 publications

Electrochemical and mechanical stability of LixLa0.557TiO3‐δ perovskite electrolyte at various voltages

Electrochemical and mechanical stability of LixLa0.557TiO3‐δ perovskite electrolyte at various voltages

Mitigation of grain boundary resistance in La2/3-xLi3xTiO3 perovskite as an electrolyte for solid-state Li-ion batteries

Engineered interfaces between perovskite La2/3xLi3xTiO3 electrolyte and Li metal for solid-state batteries

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Electrochemical and mechanical stability of Li_xLa_0.557TiO_3‐δ perovskite electrolyte at various voltages

Electrochemical and mechanical stability of Li_xLa_0.557TiO_3‐δ perovskite electrolyte at various voltages