Te doping effect on the structure and ionic conductivity of LiTa2PO8 solid electrolyte

LiTa₂PO₈ (LTPO) is a new solid-state electrolyte material, which has high bulk ionic conductivity and low grain boundary ion conductivity. However, the conductivity of materials synthesized by conventional methods is much lower than the theoretically calculated values. In this work, large radius Te ion are doped at Ta (3)-site in order to enlarge the lattice parameters and increase Li content, which are beneficial for increasing ionic conductivity. The Te substitution changes the Ta surrounding environment, increases the binding capacity of Ta–O, and reduces the attraction of oxygen to lithium ions in the system. The prepared dense Li_1.04Ta_1.96Te_0.04PO₈ ceramic electrolyte exhibits a low activation energy of 0.193 eV and four times higher ion conductivity (4.5 × 10^?4 S cm^?1) than undoped samples. Moreover, Li_1.04Ta_1.96Te_0.04PO₈ shows a stable cycling performance in the symmetric Li/Li cells and the Li/CPE/Li_1.04Ta_1.96Te_0.04PO₈/LiFePO₄ batteries with the separation of a thin PEO membrane.     

Achieving enhanced densification and superior ionic conductivity of garnet electrolytes via a co-doping strategy coupled with pressureless sintering

Lithium garnet oxides with 6.5 mol Li, such as Li_6.5La₃Zr_1.5(Ta/Nb)_0.5O₁₂, typically crystallise in cubic structure and exhibit excellent room-temperature ionic conductivity close to 1 mS cm^?1. However, it is challenging to densify garnet oxides. In this work, we investigated how the co-doping of tantalum (Ta) and niobium (Nb) affects the densification of pressureless sintered garnet electrolytes with compositions of Li_6.5La₃Zr_1.5Ta_(0.5?x)Nb_xO₁₂, where x = 0–0.5. The highest densification (94.5% of relative density) was achieved in Li_6.5La₃Zr_1.5Ta_0.1Nb_0.4O₁₂ (TN-LLZO) when it was sintered at 1150 °C for 6 h. This TN-LLZO garnet electrolyte delivers an ionic conductivity of 1.04 × 10^?3 S cm^?1 (at 22 °C) with a low activation energy of 0.41 eV. Our findings demonstrate that the content of dopants (Ta and Nb) plays a critical role in enhancing the sintering performance of garnet ceramics at ambient pressure.     

Lithium ion conductivity in the solid electrolytes (Li0.25La0.25)1−xM0.5xNbO3 (M=Sr,Ba, Ca,x=0.125) with perovskite-type structure

Perovskite-type structured solid electrolytes with the general formula (Li_0.25La_0.25)_1−xM_0.5xNbO₃ (M=Sr, Ba, Ca, x=0.125) have been prepared by solid-state reaction. Their crystal structure and ionic conductivity were examined by means of X-ray diffraction analysis (XRD), scanning electron microscope (SEM), and alternating current (AC) impedance technique. All sintered compounds are isostructural with the parent compound Li_0.5La_0.5Nb₂O₆. Some impurity phase is detected at the grain boundary in the Ba- and Ca-substituted compounds. The substitution of partial Li⁺ by alkaline earth metal ions has responsibility for the cell volume expansion as determined by the XRD data. The densification is accelerated, with the overall porosity and grain boundary minimized as Sr²⁺ ions are doped. Among the investigated compounds, the perovskite (Li_0.25La_0.25)_0.875Sr_0.0625NbO₃ shows a remarkable ionic conductivity of 1.02×10⁻⁵ S/cm at room temperature (20 °C) and the lowest activation energy of 0.34 eV in comparison with 0.38 eV and 0.44 eV for the corresponding Ba- and Ca-doped samples, respectively. It is identified that the enhancement of ionic conductivity is attributed to a reduction in activation energy for ionic conduction which is related to an increase in the cell volume.     

Li ion conduction of perovskite Li0.375Sr0.4375Ti0.25Ta0.75O3 and related compounds

In this work, perovskite-structured Li_0.375Sr_0.4375M_0.25N_0.75O₃ (M=Ti, Sn, N=Nb, Ta) solid electrolytes were synthesized by conventional solid state reaction method. Phase compositions, fractured morphologies and conductivities of these compounds were investigated by X-ray diffraction, scanning electron microscope and AC-impedance spectroscopy, respectively. X-ray diffraction analysis confirms that all of Li_0.375Sr_0.4375M_0.25N_0.75O₃ (M=Ti, Sn, N=Nb, Ta) ceramics present perovskite structure. Pure Li_0.375Sr_0.4375Ti_0.25Ta_0.75O₃ and Li_0.375Sr_0.4375Sn_0.25Ta_0.75O₃ perovskite ceramics were obtained. But impurities were detected in Li_0.375Sr_0.4375Ti_0.25Nb_0.75O₃ and Li_0.375Sr_0.4375Sn_0.25Nb_0.75O₃. Among all investigated compounds, Li_0.375Sr_0.4375Ti_0.25Ta_0.75O₃ shows the highest total ionic conductivity of 2.60 × 10^?4 S cm^?1 at room temperature and the lowest activation energy of 0.347 eV. Conductivities of Li_0.375Sr_0.4375Sn_0.25Ta_0.75O₃ and Li_0.375Sr_0.4375Sn_0.25Nb_0.75O₃ were 4.4 × 10^?5 S cm^?1 and 1.82 × 10^?6 S cm^?1, respectively. Their conductivities were much lower than Li_0.375Sr_0.4375Ti_0.25Ta_0.75O₃ and Li_0.375Sr_0.4375Ti_0.25Nb_0.75O₃.     

A novel promotion strategy for microstructure and electrical performance of garnet electrolytes via Li4GeO4 additive

Cubic Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (c-LLZTO) electrolyte is one of the most promising solid electrolytes. However, it is rather difficult to promote its electrical performance while reducing process parameters. Therefore, Li₄GeO₄ is applied as the additive in liquid sintering of LLZTO ceramics in this study. The LLZTO@Li₄GeO₄/Li₂O composite electrolyte sintered at 1180 °C for 3 h performs a significantly promoted microstructure and electrical performance, the ionic conductivity of which reaches 5.77 × 10⁻⁴ S cm⁻¹ at 25 °C. The Li₄GeO₄/Li₂O eutectic phase contributed prominently, in which the high concentration of Li⁺ seaming the LLZTO grains tightly. Meanwhile, Li⁺ conduction in the consecutive conductive pathways constructed by [GeO₄] groups among the grains was greatly stimulated. With the modification of the grain boundary, an improved garnet electrolytes/Li anode interface performance is produced. The Li/Au|LLZTO@Li₄GeO₄/Li₂O|Au/Li symmetrical cell is able to cycle stably for more than 500 h at the current density of 0.1 mA cm⁻² at room temperature.     

Partial nitridation of Li4SiO4 and ionic conductivity of Li4.1SiO3.9N0.1

The Li content and anion lattice of Li₄SiO₄ were modified to improve ionic conductivity. Li₂CO₃ and Si₃N₄ were mixed in a ratio of Li/Si?=?4.5 and heated in NH₃ at 820?°C, which resulted in the formation of the oxynitride, Li_4.1SiO_3.9N_0.1. Powder X-ray diffraction analyses revealed Li_4.1SiO_3.9N_0.1 and Li₄SiO₄ to be isostructural with a subtle variation in the lattice constants. Diffuse-reflectance absorption spectroscopy, however, showed a significant decrease in the band gap, from 5.6?eV in Li₄SiO₄ to 4.8?eV in Li_4.1SiO_3.9N_0.1. X-ray photoelectron spectra of the Li 1s and Si 2p levels revealed enhanced lattice covalency in Li_4.1SiO_3.9N_0.1 compared to the oxide phase. The ionic conductivity of Li₄SiO₄ and Li_4.1SiO_3.9N_0.1 were measured by ac impedance spectroscopy over the temperature range 100–400?°C. Non-linear fitting analysis of the equivalent circuit revealed that the ionic conductivity of Li_4.1SiO_3.9N_0.1 was approximately one order of magnitude higher than that of Li₄SiO₄.     

Optimization of Lithium Content and Sintering Aid for Maximized Li+ Conductivity and Density in Ta‐Doped Li7La3Zr2O12

Ta‐doped cubic phase Li₇La₃Zr₂O₁₂ (LLZ) lithium garnet received considerable attention in recent times as prospective electrolyte for all‐solid‐state lithium battery. Although the conductivity has been improved by stabilizing the cubic phase with the Ta⁵⁺ doping for Zr⁴⁺ in LLZ, the density of the pellet was found to be relatively poor with large amount of pores. In addition to the high Li⁺ conductivity, density is also an essential parameter for the successful application of LLZ as solid electrolyte membrane in all‐solid‐state lithium battery. Systematic investigations carried out through this work indicated that the optimal Li concentration of 6.4 (i.e., Li_6.4La₃Zr_1.4Ta_0.6O₁₂) is required to obtain phase pure, relatively dense and high Li⁺ conductive cubic phase in Li_7?xLa₃Zr_2?xTa_xO₁₂ solid solutions. Effort has been also made in this work to enhance the density and Li⁺ conductivity of Li_6.4La₃Zr_1.4Ta_0.6O₁₂ further through the Li₄SiO₄ addition. A maximized room‐temperature (33°C) total (bulk + grain boundary) Li⁺ conductivity of 3.7 × 10^?4 S/cm and maximized relative density of 94% was observed for Li_6.4La₃Zr_1.4Ta_0.6O₁₂ added with 1 wt% of Li₄SiO₄.     

Dopant effect on Li+ ion transport in NASICON-type solid electrolyte: Insights from molecular dynamics simulations and experiments

The performance of sodium superionic conductor (NASICON)-type LiZr₂(PO₄)₃ (LZP) solid electrolytes for Li-ion batteries is dependent on their ion transportation properties. Therefore, to achieve high stability, ionic conductivity, and good compatibility with Li, the LZP solid electrolyte has chosen and doped with Al to improve aforesaid properties. Also, the effect of the dopant on various parameters has been investigated via MD simulations and experimentally. In this study, molecular dynamics (MD) simulations were used to investigate the effect of Al doping on the ion transport properties of Li_1+xAl_xZr_2?x(PO₄)₃ (LAZP, x = 0.0–1.0) solid electrolytes. A facile solid-state reaction was used to synthesize both pristine and Al-doped solid electrolytes and to estimate the effect of doping on the ionic conductivity and ion diffusion in LZP. Computational and experimental results provided strong evidence of improved ion conductivity and diffusion in LZP owing to the presence of the Al dopant. Furthermore, the computational results agreed well with the experimental results, thereby validating the computational model. A maximum ionic conductivity of σ_Li = 2.77 × 10^?5 S cm ^?1 (for x = 0.2) was obtained. Enhanced ionic conductivity was observed with Al dopants owing to the creation of interstitial Li ions through a reduction in grain boundary resistance. However, a further increase in the amount of dopant reduced the ionic conductivity of LZP owing to Li-ion trapping at the most stable and metastable sites around the Al insertions. Doped LZP solid electrolytes are suitable for use in energy storage devices because of their enhanced ionic conductivity compared to that of pristine LZP.     

Lithium-metal potential in Li<Superscript>+</Superscript> containing ionic liquids

Impedance spectroscopy studies of the interface between lithium and ionic liquid (IL) showed the formation of a film (solid electrolyte interface, SEI), protecting metal from its further dissolution. Consequently, the potential of metallic lithium immersed in an electrolyte containing Li⁺ cations may be described as a Li|SEI|Li⁺ system, rather than simply Li/Li⁺. The potential of lithium-metal in a series of ionic liquids (and in a number of molecular liquids) containing Li⁺ cation (0.1 M) was measured versus the Ag|(Ag⁺ 0.01 M, cryptand 222 0.1 M, in acetonitrile) reference. The lithium-metal potential (E(Li|SEI|Li⁺)) was ca. −2.633 ± 0.017 V in ILs based on the [N(CF₃SO₂)₂ ^– ] anion, while −2.848 ± 0.043 V in ILs containing [BF₄ ^– ] anion (the difference is ca. 200 mV). In the case of ILs based on the triflate anion ([CF₃SO₃ ^– ]), the cation of ionic liquid also influences the E(Li|SEI|Li⁺) value: it was ca. −1.987 ± 0.075 V for imidazolium based cations and much lower (−2.855 V) for the pyrrolidinium based cation. In ionic liquid based on the imidazolium cation and hexafluorophosphate anion ([PF₆ ^– ]), the Li/SEI/Li⁺ potential was −2.245 V. The Li|SEI|Li⁺ potential measured in cyclic carbonates was −2.780 ± 0.069 V while in dimethylsulfoxide showed the lowest value of ca. −3.285 V. The measured potentials were also expressed versus the formal potential of the ferrocene/ferrocinium redox couple, obtained from cyclic voltammetry.     

Synthesis and thermoelectric performance of Li-doped NiO ceramics

Ni_1?xLi_xO (x = 0, 0.03, 0.06, 0.09) powders were prepared by sol–gel method combined with sintering procedure using Ni(CH₃COO)₂·4H₂O and citric acid as the raw materials and alcohol as solvent. The crystal structures of the samples were investigated by X-ray diffraction and Raman spectroscopy. The thermoelectric properties, such as the electrical conductivity, the Seebeck coefficient and the thermal conductivity were measured. The results showed that all the samples are p-type semiconductors. The electrical conductivity increases with the increase of the temperature, which indicates that the substitution of Li⁺ for Ni²⁺ can increase the concentrations and mobility of the carriers. The thermal conductivity decreases remarkably with the increase of the Li doping content, which indicates that Li doping can enhance the scattering of phonon. However, the Seebeck coefficient will decline with the increase of the Li doping content. As results of the increase of electrical conductivity and reduction of thermal conductivity, Li doping can increase the figure of merit (ZT) of NiO, the ZT value reach 0.049 at 770 K for Ni_1?xLi_xO with x = 0.06.     

Reactive flash sintering and electrical transport properties of high-entropy (MgCoNiCuZn)1-xLixO oxides

In this paper, high-entropy (MgCoNiCuZn)_1-xLi_xO oxides (x = 0, 0.1, 0.15, 0.2, and 0.3) were synthesized via reactive flash sintering (RFS), and the effect of RFS process on the microstructure and electrical property of the materials were studied. The Li-doped materials exhibited a mixed ionic–electronic transport behavior. The oxidation of Co²⁺ into Co³⁺ upon Li incorporation into the materials synthesized via the conventional solid-state reaction route was not evidenced in the flash sintered materials. Instead, the charge unbalance in the Li-doped materials synthesized via RFS was compensated by oxygen vacancies and holes in the valence band of the oxides, which were accounted for the ionic conduction and electronic conduction, respectively. The ionic conductivity increased upon increasing the Li concentration as more oxygen vacancies were formed. The attraction between defects with different charges (Li_M^/ and V_O^••), which formed defect complexes, led to a decrease in the mobility of the defects, thus resulting in a less pronounced increase in the ionic conductivity at high Li concentrations. The change in the charge compensation mechanism of the materials indicates that the microstructure of such kind of oxides could be altered through RFS, and thus the property may be manipulated.     

Sintering analysis of garnet-type ceramic as oxide solid electrolytes for rapid Li+ migration

Metallic doping can stabilize cubic phase Li₇La₃Zr₂O₁₂ (LLZO) solid electrolyte for high conductivity, due to the enhanced vacancies and disordered Li-site. However, the understanding of metallic doping in the crystal lattice during the high-temperature sintering process is still not clear. In present study, a gradient series of Fe doped LLZO are formulated via solid-phase reaction, and then investigated through crystal analysis and morphological characterization. Pair distribution function essay implies that doped Fe³⁺ promotes random distribution of Li⁺ over the available sites in the located crystal. Additionally, the ceramic morphology confirms that the particles sizes in LLZO pellets suddenly grow above 1000 ℃, and Fe doping can obviously suppress Li loss above 600 ℃. As a result, the LLZF0.15 exhibits the relatively high ionic conductivity of 1.99 × 10^–5 S cm^–1 at 45 ℃.     

Effect of SnO–P2O5–MgO glass addition on the ionic conductivity of Li1.3Al0.3Ti1.7(PO4)3 solid electrolyte

NASICON-type structured compounds Li_1+xM_xTi_2-x(PO₄)₃ (M = Al, Fe, Y, etc.) have captured much attention due to their air stability, wide electrochemical window and high lithium ion conductivity. Especially, Li_1.3Al_0.3Ti_1.7(PO₄)₃ (LATP) is a potential solid electrolyte due to its high ionic conductivity. However, its actual density usually has a certain gap with the theoretical density, leading the poor ionic conductivity of LATP. Herein, LATP solid electrolyte with series of SnO–P₂O₅–MgO (SPM, 0.4 wt%, 0.7 wt%, 1.0 wt%, 1.3 wt%) glass addition was successfully synthesized to improve the density and ionic conductivity. The SPM addition change Al/Ti–O bond and P–O bond distances, leading to gradual shrinkage of octahedral AlO₆ and tetrahedral PO₄. The bulk conductivity of the samples increases gradually with SPM glass addition from 0.4 wt% to 1.3 wt%. Both SPM and the second-phase LiTiPO₅, caused by glass addition, are conducive to the improvement of compactness. The relative density of LATP samples increases first from 0 wt% to 0.7 wt%, and then decreases from 0.7 wt% to 1.3 wt% with SPM glass addition. The grain boundary conductivity also changes accordingly. Especially, the highest ionic conductivity of 2.45 × 10^?4 S cm^?1, and a relative density of 96.72% with a low activation energy of 0.34 eV is obtained in LATP with 0.7 wt% SPM. Increasing the density of LATP solid electrolyte is crucial to improve the ionic conductivity of electrolytes and SPM glass addition can promote the development of dense oxide ceramic electrolytes.     

Rapid preparation and performances of garnet electrolyte with sintering aids for solid-state Li–S battery

Lithium-sulfur (Li–S) batteries are attractive due to their high theoretical energy density. However, conventional Li–S batteries with liquid electrolytes undergo polysulfide shuttle-effect and lithium dendrite formation during charge/discharge process, leading to poor electrochemical performance and safety issues. Garnet type Li₇La₃Zr₂O₁₂ (LLZO) solid-state electrolyte (SSE) restricts the penetration of polysulfides and exhibits high ionic conductivity at room temperature (RT). Herein, Li_6.5La₃Zr_1.5Nb_0.5O₁₂ (LLZNO) ceramic electrolyte using Li₃PO₄ (LPO) as sintering aids (LLZNO-LPO) is prepared by the rapid sintering method and is applied to construct a shuttle-effect free solid-state Li–S battery. The SSE displays high conductive pure cubic-LLZO phase; during the rapid sintering, LPO melts and junctions the voids between the grains, thus improves Li⁺ conductivity. As a result, the LLZNO-LPO ceramic electrolyte with Li⁺ conductivity of 4.3 × 10^?4 S cm^?1 and high critical current density (CCD) of 1.2 mA cm^?2 is obtained at RT. The Li–S solid-state battery which utilizes LLZNO-LPO ceramic electrolyte can deliver an initial discharge capacity of 943 mA h·g^?1 and 602 mA h·g^?1 retention after 60 cycles. In the same time, the initial coulombic efficiency is as high as 99.5%, indicating that the SSE can effectively block the polysulfide shuttle towards the Li anode and fulfill a shuttle-free Li–S battery.     

Influence of sintering aids and excess Lithium on the conductivity of perovskite-type Li3/8Sr7/16Zr1/4Nb3/4O3 solid electrolyte

Perovskite-structured Li_3/8Sr_7/16Zr_1/4Nb_3/4O₃ solid-state Lithium-conductors were prepared by conventional solid-state reaction method. Influence of sintering aids (Al₂O₃, B₂O₃) and excess Lithium on structure and electrical properties of Li_3/8Sr_7/16Zr_1/4Nb_3/4O₃ (LSNZ) has been investigated. Their crystal structure and microstructure were characterized by X-ray diffraction analysis and scanning electron microscope, respectively. The conductivity and electronic conductivity were evaluated by AC-impedance spectra and potentiostatic polarization experiment. All sintered compounds are cubic perovskite structure. Optimal amount of excess Li₂CO₃ was chosen as 20 wt% because of the total conductivity of LSNZ-20% was as high as 1.6×10⁻⁵ S cm⁻¹ at 30 °C and 1.1×10⁻⁴ S cm⁻¹ at 100 °C, respectively. Electronic conductivity of LSNZ-20% is 2.93×10⁻⁸ S cm⁻¹, nearly 3 orders of magnitude lower than ionic conductivity. The density of solid electrolytes appears to be increased by the addition of sintering aids. The addition of B₂O₃ leads to a considerable increase of the total conductivity and the enhancement of conductivity is attributed to the decrease of grain-boundary resistance. Among these compounds, LSNZ-1 wt%B₂O₃ has lower activation energy of 0.34 eV and the highest conductivity of 1.98×10⁻⁵ S cm⁻¹ at 30 °C.     

Conductivity of zirconium oxide alloyed with lithium oxide

The solid-phase method is used to synthesize polycrystalline samples of zirconium dioxide stabilized with 10% Y₂O₃ (or content) and up to 3% Li₂O. It is found that the conductivity of the samples increases substantially when Li₂O is added and reaches its maximum value at 1.7% Li₂O. The conduction activation energy decreases from 0.85 eV in samples with no Li₂O added to 0.56 eV in samples containing 1.7% Li₂O. It is suggested that lithium ions in the ZrO₂ cubic lattice form two types of defects: substitution effects — Li _Zr ^3? and interstitial defects — Li _i ⁺ . The latter greatly increase the electrical conductivity of the samples.     

Crystal structure of cubic Li7-3xGaxLa3Zr2O12 with space group of I-43d

Cubic Li_7-3xGa_xLa₃Zr₂O₁₂ is a cubic phase with a space group of I-43d instead of Ia-3d. This structure is more conducive to the migration of lithium ions. However, the effect of Ga on the size and environment of lithium ion transport channels has not been researched. In this work, Li_7-3xGa_xLa₃Zr₂O₁₂ (x = 0–0.25) was formulated, and the crystal structure was obtained by neutron diffraction. The results indicated that the minimum channel size to control Li⁺ migration in LLZO was the bottleneck size between the Li2 and Li3 sites (bottleneck size 2), and compared with lanthanum ions, the zirconium ions were closer to lithium ions. As the Ga content increased, bottleneck size 2 levelled off, while the lithium concentration and the distance between skeleton ions and lithium ions decreased. As a result, the lithium ionic conductivity primarily increased and then decreased. When doping 0.2 pfu of Ga, LLZO exhibited the highest lithium ionic conductivity of 1.45 mS/cm at 25 °C due to the coordinated regulation of Li⁺ concentration, bottleneck size, and the distance between skeleton ions and lithium ions.     

Ceria (La3+, Sr2+)/Carbonates Nanocomposite Electrolytes with High Electrical Conductivity for Low‐Temperature SOFCs

A series of ceria‐based nanocomposites consisting of lanthanum and strontium codoped ceria with composition Ce_0.89La_0.07Sr_0.04O_1.925 (CL7S4) and eutectic mixture of carbonates Li₂CO₃‐Na₂CO₃ (LNCO) have been prepared by mixing nanosize powders of CL7S4 and LNCO. Samples have been characterized using differential thermal analysis, X‐ray diffraction, scanning electron microscopy combined with energy‐dispersive spectroscopy, thermal expansion, and impedance spectroscopy. A sharp increase in ionic conductivity is observed in all the composite specimens corresponding to superionic transition. Sample containing 35 wt% of carbonate shows the maximum conductivity (2.56 × 10^?1 S/cm at 500°C) with activation energy of conduction, E_a 0.23 eV.     

Synthesis,structure and electrochemical properties of Al doped high entropy perovskite Lix(LiLaCaSrBa)Ti1-xAlxO3

In this work, the Al doped high entropy perovskite Li_0.2La_0.2Ca_0.2Sr_0.2Ba_0.2TiO₃ ceramic is synthesized by using a solid state reaction method, and the effect of different doping amount on the crystal structures and conductivity are also studied. The result proves that doping leads to a positive influence on the conductivity of ceramic. The material of Li_0.1(LiLaCaSrBa)Ti_0.9Al_0.1O₃ (LLCSBTA-0.1) exhibits a high total conductivity with approximately 3.92 × 10^-7 S cm^-1 at 30 °C and an activation energy of 0.39 eV. The beneficial result can be ascribed to the increase of Li ⁺ concentration. The Li_0.2La_0.2Ca_0.2Sr_0.2Ba_0.2TiO₃ presents a pure cubic perovskite structure, but with partial tetragonal structure due to the addition of Al₂O₃. However, these high entropy perovskite ceramics showed porous structures which are unfavourable for lithium ion conduction. The electrochemical property of the Li_0.1(LiLaCaSrBa)Ti_0.9Al_0.1O₃ as electrode is investigated as well. The results show that the Li_0.1(LiLaCaSrBa)Ti_0.9Al_0.1O₃ electrode exhibits good cyclability and stability for the insert-extraction of lithium ions with the specific capacity of 58.6 mA h g^?1.     

Impacts of 3Li2O-2GeO2 melt on fabrication and electrical performance of novel LLZTO@Li4GeO4/Li2O composite electrolytes

Novel LLZTO@Li₄GeO₄/Li₂O composite electrolytes have been successfully produced through liquid sintering Li_6.4La₃Zr_1.4Ta_0.6O₁₂ via the 3Li₂O-2GeO₂ (LGO1.5) additive at 1140 °C for 3 h in air atmosphere. The Li-Ge-O additive performs a prominent role in fabricating compact connections among LLZTO grains and accelerating their densification procedure. Moreover, the additive acts as a bridge to promote Li⁺ transportation in the grain boundary domains. Consecutive Li⁺ conduction pathways are constructed inside the ceramics correspondingly. A considerably enhancement for the electrical performance of the garnet-type electrolytes is realized. The composite electrolyte with 2wt% LGO1.5 exhibits a high ionic conductivity of 5.57 × 10^?4 S·cm^?1 at 25 °C, the relative density of which reaches 95.8%. It is also capable of withstanding a high voltage up to 6 V (vs. Li/Li⁺) and a large critical current density of 0.65 mA·cm^?2.