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Nanoscale Research Letters · 2020 ·Vol. 15 ·期 1 ·1-10 · IF 3.578

Improved Cycling Stability of LiCoO2 at 4.5 V via Surface Modification of Electrodes with Conductive Amorphous LLTO Thin Film

Song Shipai,Peng Xiang,Huang Kai,Zhang Hao,Wu Fang,Xiang Yong,Zhang Xiaokun

The stability issue of LiCoO 2 cycled at high voltages is one of the burning questions for the development of lithium ion batteries with high energy density and long cycling life. Although it is effective to improve the cycling performance of LiCoO 2 via coating individual LiCoO 2 particles with another metal oxides or fluorides, the rate capacity is generally compromised because the typical coating materials are poor conductors. Herein, amorphous Li 0.33 La 0.56 TiO 3 , one of the most successful solid electrolytes, was directly deposited on the surface of made-up LiCoO 2 electrodes through magnetron sputtering. Not only the inherent conductive network in the made-up LiCoO 2 electrodes was retained, but also the Li + transport in bulk and across the cathode-electrolyte interface was enhanced. In addition, the surface chemical analysis of the cycled LiCoO 2 electrodes suggests that most of the stability issues can be addressed via the deposition of amorphous Li 0.33 La 0.56 TiO 3 . With an optimized deposition time, the LiCoO 2 electrodes modified by Li 0.33 La 0.56 TiO 3 performed a steady reversible capacity of 150 mAh/g at 0.2 C with the cutoff voltage from 2.75 to 4.5 V vs . Li + /Li and an 84.6% capacity gain at 5 C comparing with the pristine one.

研究领域: 材料科学 · 电化学
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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

Biomimetic PVDF/LLTO composite polymer electrolyte enables excellent interface contact and enhanced ionic conductivity

Boyu Li,Qingmei Su,Lintao Yu,Wuyou Liu,Shijia Dong,Shukai Ding,Miao Zhang,Gaohui Du,Bingshe Xu

Composite polymer electrolyte (CPE) with enhanced ionic conductivity, excellent flexibility and strong strength are urgently required for all-solid-state lithium metal batteries (LMBs). Inspired by the dragonfly wings that are super-lightweight and ultrathin but have excellent stability when subject to bending and twisting during flapping, we have constructed Li 0.35 La 0.55 TiO 3 (LLTO) nanowires-filled polyvinylidene fluoride (PVDF). In our design, the PVDF is used to construct the ultrathin membrane, the 1D LLTO nanowires are acted as the veins to give rise to a high mechanical strength of 10 Mpa. The special design creates cellular surface of PVDF/LLTO-CPE, which guarantees the excellent flexibility as well as a good interface contact between CPE and Li anode. When evaluated as electrolyte for LiFePO 4 |Li battery, the PVDF/LLTO-CPEs can suppress Li dendrites growth, and thus presents an excellent cycling stability of 140 mAh g −1 after 200 cycles. Moreover, the flexible LiFePO 4 |PVDF/LLTO-CPE|Li 4 Ti 5 O 12 pouch cell delivers a satisfactory rate performance and cycle stability under folding and bending states. The excellent performances are attributed to the unique cellular structure and super mechanical strength of biomimetic PVDF/LLTO-CPE. All results show the PVDF/LLTO-CPE is a promising solid-state electrolyte for flexible electronic devices.

研究领域: 材料科学 · 能源存储 · 仿生学
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International Journal of Minerals Metallurgy and Materials · 2021 ·Vol. 28 ·期 2 ·305-316 · IF 2.232

Coupling effect of the conductivities of Li ions and electrons by introducing LLTO@C fibers in the LiNi0.8Co0.15Al0.05O2 cathode

Wang Hao-yang,Cheng Xue,Li Xiao-feng,Pan Ji-min,Hu Jun-hua

To probe the coupling effect of the electron and Li ion conductivities in Ni-rich layered materials (LiNi 0.8 Co 0.15 Al 0.05 O 2 , NCA), lithium lanthanum titanate (LLTO) nanofiber and carbon-coated LLTO fiber (LLTO@C) materials were introduced to polyvinylidene difluoride in a cathode. The enhancement of the conductivity was indicated by the suppressed impedance and polarization. At 1 and 5 C, the cathodes with coupling conductive paths had a more stable cycling performance. The coupling mechanism was analyzed based on the chemical state and structure evolution of NCA after cycling for 200 cycles at 5 C. In the pristine cathode, the propagation of lattice damaged regions, which consist of high-density edge-dislocation walls, destroyed the bulk integrity of NCA. In addition, the formation of a rock-salt phase on the surface of NCA caused a capacity loss. In contrast, in the LLTO@C modified cathode, although the formation of dislocation-driven atomic lattice broken regions and cation mixing occurred, they were limited to a scale of several atoms, which retarded the generation of the rock-salt phase and resulted in a pre-eminent capacity retention. Only NiO phase “pitting” occurred. A mechanism based on the synergistic transport of Li ions and electrons was proposed.

研究领域: 材料科学 · 电化学 · 能源存储技术
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Crystals · 2025 ·Vol. 15 ·期 8 ·707 · IF 2.4

Lithium Lanthanum Titanate (LLTO) Solid Electrolyte with High Ionic Conductivity and Excellent Mechanical Properties Prepared by Aerodynamic Levitation Rapid Solidification

Yidong Hu,Fan Yang,Jianguo Li,Qiaodan Hu

Lithium lanthanum titanate (LLTO) is a promising solid electrolyte for all-solid-state lithium-ion batteries (ASSLIBs), and its total conductivity is dramatically influenced by the ceramic microstructure. Here we report a novel aerodynamic levitation rapid solidification method to prepare dense LLTO ceramics with a dendrite-like microstructure, which can be hardly obtained by conventional sintering. At optimal nominal lithium content and cooling rate, the solidified LLTO ceramic achieved a high total conductivity of 2.5 × 10−4S·cm−1at room temperature, along with excellent mechanical properties such as a high Young’s modulus of 240 GPa and a high hardness of 16.7 GPa. Results from this work suggest that aerodynamic levitation rapid solidification is an effective processing method to manipulate the microstructure of LLTO ceramics to minimize the GBs’ contribution to the total conductivity, which may be expanded to prepare other oxide-type lithium electrolytes.

CAS / MDL: 13463-67-7 554-13-2
研究领域: 材料科学 · 固体离子学 · 储能技术 · 陶瓷制备
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MATERIALS RESEARCH BULLETIN · 2025 · IF 5.7

Enhanced ionic conductivity and improved electrochemical performance of hybrid Li0.33La0.56TiO3

Xiaojuan Lu,Jialin Yang,Ke Huang,Songtao Liu

Template-regulated Li 0.33 La 0.56 TiO 3 (LLTO) powders are synthesized using CTAB via a hydrothermal method. The hybird LLTO is obtained by mixing the template-regulated LLTO powders with Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) powders and non-templated LLTO powders. In the non-templated LLTO, small round grains develop, while large grains with a high aspect ratio tend to form in the template-regulated LLTO. The total conductivity of the hybrid LLTO increases, reaching 1.28×10 −4 S cm −1 . The presence of specific mesopores and the bridging effect among grains create an optimal balance between the mobility and density of lithium ions, therefore contributing to the increase of the conductivity. The hybrid LLTO demonstrates improved higher fracture toughness, indicating a greater cycling tolerance. It also exhibits superior initial capacity and a slower degradation rate. These results present a novel approach to prepare lithium-ion conductors with enhanced performance.

CAS / MDL: 57-09-0
研究领域: 材料科学 · 电化学
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JOURNAL OF NON-CRYSTALLINE SOLIDS · 2026 · IF 3.6

Synergistic enhancement of borophosphate glasses - halides in Li+ ionic conductivity of LLTO

Beibei Pan,Yuanhao Ma,Jiawei Zhao,Caiyan Chen,Shuaishuai Liu,Yang Shen,Qiuju Zheng,Yuebo Hu

Li 0.5 La 0.5 TiO 3 (LLTO) is a promising solid-state electrolyte material due to its excellent chemical stability, wide electrochemical window, and relatively high ionic conductivity. This work aims to further improve the ionic conductivity of LLTO via modification with borophosphate glasses containing lithium halides. The underlying rationale is that the unique mixed network structure of borophosphate glass can provide additional pathways for lithium ion (Li + ) transport. Furthermore, the incorporation of halogenated borosilicate glass (especially LiI) is expected not only to supply extra Li + , but also to improve the solid electrolyte interface by filling the voids among LLTO pellets, thus enhancing the overall electrochemical performance. The results demonstrate that the sample with 2 wt.% Li 2 O-B 2 O 3 -P 2 O 5 -LiI (LBPI) glass achieves a favorable room temperature ionic conductivity of 1.03 × 10 –3 S·cm –1 , which is approximately double that of the pristine LLTO. Our findings confirm the synergistic modification effect of borophosphate glass and lithium halides in improving Li + transport and present a strategic approach for developing advanced solid-state electrolytes with satisfactory electrochemical performance.

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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2026 ·Vol. 37 ·期 22 ·1766 · IF 3.2

Polydopamine-mediated interface regulation and performance optimization of LLTO/PVDF-HFP composite solid electrolyte

Wang Dingqin,Fei Zihao,Zheng Deyi

Perovskite-structured Li 0.33 La 0.56 TiO 3 (LLTO) ceramic fillers are widely used for their low cost and environmental friendliness, yet their poor uniform dispersion in polymer matrices and inadequate interfacial compatibility between phases still limit performance. This study fabricated PDA@LLTO/PVDF-HFP composite electrolytes via solution casting, by modifying LLTO with a biodegradable polydopamine (PDA) coating. Dopamine undergoes oxidative self-polymerization on LLTO surfaces to form a PDA layer, whose excellent adhesion ensures firm binding to the LLTO surfaces, reducing filler surface energy and promoting uniform dispersion. Meanwhile, PDA’s phenolic hydroxyl and amino groups interact with PVDF-HFP’s fluorine and carbonyl groups via hydrogen bonding, electrostatic interactions, and physical entanglement, forming a strong interface. PDA reduces interfacial gaps and defects by acting as a “molecular bridge” to improve adhesion between the two phases. Results show the 2.4 wt%-PDA@LLTO/PVDF-HFP composite exhibits well-balanced electrochemical performance: an ionic conductivity of 2.37 × 10 −4 S cm −1 at 25 °C, an interfacial impedance reduced from 367 to 167 Ω, a lithium-ion migration number of 0.81, and an electrochemical stability window expanded to 4.88 V, The critical current density reaches 2.297 mA/cm 2 . The assembled solid-state full batteries deliver an initial discharge capacity of 168.59 mAh/g at 0.5 C, retaining 148.80 mAh/g (88.3% capacity retention) after 180 cycles, with Coulombic efficiency stabilized at 99.6% and significantly improved thermal stability. This work provides new insights for developing high-performance all-solid-state electrolytes, which hold promising applications.

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ACS Omega · 2021 · IF 3.512

Solvent-Free Procedure to Prepare Ion Liquid-Immobilized Gel Polymer Electrolytes Containing Li0.33La0.56TiO3 with High Performance for Lithium-Ion Batteries

Wen Zheng,Wanying Bi,Yaobing Fang,Shuya Chang,Wenhui Yuan,Li Li

Based on the advantages of intrinsic safety, flexibility, and good interfacial contact with electrodes, a gel polymer electrolyte (GPE) is a promising electrolyte for lithium-ion batteries, compared with the conventional liquid electrolyte. However, the unstable electrochemical performance and the liquid state in a microscale limit the commercial application of GPE. Herein, we developed a novel gel polymer electrolyte for lithium-ion batteries by blending methyl methacrylate (MMA), N-butyl-N-methyl-piperidinium (Pyr14TFSI), and lithium salts in a solvent-free procedure, with SiO2 and Li0.33La0.56TiO3 (LLTO) additives. The prepared MMA-Pyr14TFSI-3 wt % LLTO electrolyte shows the best electrochemical performance and obtains a high ion conductivity of 4.51 × 10–3 S cm–1 at a temperature of 60 °C. Notably, the electrochemical window could be stable up to 5.0 V vs Li+/Li. Moreover, the batteries with the GPE also show excellent electrochemical performance. In the LiFePO4/MMA-Pyr14TFSI-3 wt % LLTO/Li cell, a high initial discharge capacity was achieved 150 mA h g–1 at 0.5C with a Coulombic efficiency over 99% and maintaining a good capacity retention of 90.7% after 100 cycles at 0.5C under 60 °C. In addition, the physical properties of the GPE have been investigated by scanning electron microscopy (SEM), X-ray diffraction (XRD) measurements, Fourier transform infrared (FTIR) spectroscopy, and thermogravimetry (TG).

研究领域: 材料科学 · 电化学
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Batteries-Basel · 2023 ·Vol. 9 ·期 5 ·270 · IF 4

Effectively Elevating Ceramic Fillers’ Dispersity in Gel Hybrid Electrolyte through Bridge–Linked Construction for High–Performance Lithium Metal Batteries

Minghua Chen,Wannian Liu,Ziyu Yue,Yang Wang,Yixin Wu,Yu Li,Zhen Chen

Gel polymer-ceramic hybrid electrolytes (GHEs) have emerged as desirable candidates for preparing high energy density and excellent practicability gel batteries. However, the agglomeration of ceramic particles in polymer matrix leads to a decrease in cycling stability and low mechanical properties of GHEs. Here, we present a feasible method for improving the dispersity of Li0.24La0.59TiO3(LLTO) nanorods in the polyvinylidenefluoride (PVDF)/poly(propylene carbonate) (PPC) co-blended matrix (K–LLTO/PVDF/PPC) by γ-(2,3-epoxypropoxy)propytrimethoxysilane (KH560) surface treatment. The as-prepared GHE with 10% K–LLTO filler (10% GHE) exhibits a high ionic conductivity (3.01 mS cm−1) and an appropriate lithium-ion transference number (0.55). The Li|10% GHE|Li symmetric cell shows an exceptional lithium stripping-plating lifetime of > 2000 h at 0.1 mA cm−2. The assembled LiFePO4(LFP)|10% GHE|Li full cells show satisfactory cycling stability in the 2.5–4.2 V electrochemical window by recovering 84% of the initial capacity at 2 C over 500 cycles. The uniformly dispersed K–LLTO within the polymer matrix is ascribed to the formation of a bridge-linked network via Si–O–Ti bonds between KH560 and LLTO, and plenty of hydrogen bonds within the polymer matrix. This modification method provides a feasible strategy for fabricating GHEs with good repeatability, which may easily adapt to the high requirements of commercial production.Keywords:LLTO nanorods;surface modification;dual polymer matrix;gel polymer-ceramic hybrid electrolyte

研究领域: 材料科学 · 电化学
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DALTON TRANSACTIONS · 2022 ·Vol. 51 ·期 18 ·7076-7083 · IF 4.569

Two-dimensional layered lithium lanthanum titanium oxide/graphene-like composites as electrodes for lithium-ion batteries

Bo Gu,Chenyang Zhan,Bing Heng Liu,Gang Wang,Qian Zhang,Ming Zhang,Zhongrong Shen

Perovskite-structured (ABO3) lithium lanthanum titanate (LixLa(2−x)/3TiO3, LLTO) is widely used in all solid state lithium ion batteries due to its high ionic conductivity. In this study, a two-dimensional LLTO nanosheet/graphene (LLTO/C) nanosheet composite has been designed as an electrode material for lithium-ion batteries (LIBs). LLTO/C not only exhibits the ionic conductivity properties of perovskite-type LLTO, but the graphene between the layers of LLTO nanosheets also endows the material with additional electronic conductivity. Moreover, LLTO@C-600 exhibits an excellent rate capability as the electrode for delithiation with a high specific capacity of 350 mA h g−1 at 20 mA g−1, and 70% of the specific capacity can be maintained at 1.0 A g−1 after 800 cycles. The excellent electrochemical performances can be attributed to the superior interficial capacitive Li+ storage capability.

研究领域: 材料科学 · 能源存储技术
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ACS Applied Energy Materials · 2026 · IF 5.5

Interface-Stabilized LLTO/PVDF/PE Composite Separator Boosts High-Performance All-Solid-State Lithium Metal Batteries

Wenxin Shi,Qingmei Su,Xuan Li,Huayu Li,Siyu Wang,Weihao Shi,Liming Wang,Yinyin Song,Shan Yang,Gaohui Du,Miao Zhang,Wenqi Zhao,Bingshe Xu

The development of composite solid electrolytes with high ionic conductivity and superior interfacial stability is crucial for practical all-solid-state lithium metal batteries (ASSLMBs). Herein, a high-performance bilayer composite separator is designed by integrating Li0.33La0.557TiO3 (LLTO) nanofibers into a poly(vinylidene fluoride) (PVDF) matrix, which is coated onto a polyethylene (PE) substrate. The interconnected LLTO nanofibers construct three-dimensional continuous ion-conducting pathways and reduce the crystallinity of the polymer matrix, endowing the optimized separator (with 60 wt % LLTO) with a high ionic conductivity of 5.17 × 10–4 S cm–1, a large lithium-ion transference number (tLi+= 0.81), and a wide electrochemical stability window up to 4.87 V. The unique bilayer architecture, where the LLTO/PVDF layer facilitates rapid Li+ transport and the PE layer ensures interfacial compatibility, enables stable lithium plating/stripping over 500 h and yields a high critical current density of 2.9 mA cm–2. Furthermore, the robust mechanical properties of the separator ensure uniform lithium-ion flux and effectively resist lithium dendrite penetration. When applied in NCM811/Li metal battery, this modified solid-state electrolyte separator enabled remarkable cycling stability (89.8% capacity retention after 200 cycles at 5C) and exceptional rate performance (115.4 mAh g–1 at 5C). This work provides a feasible and effective strategy for designing composite separators toward high-energy-density and dendrite-free ASSLMBs.

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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Ion/Electron Co-Conductive Triple-Phase Interface Enabling Fast Redox Reaction Kinetics in Lithium–Sulfur Batteries

Huan Wang,Boyu Li,Yanlei Shen,Ziyao Zhang,Yinzhao Sun,Weitao Zhou,Shuaitong Liang,Weitao Li,Jianxin He

Lithium–sulfur batteries (LSBs) are promising next-generation energy storage systems because of their high energy densities and high theoretical specific capacities. However, most catalysts in the LSBs are based on carbon materials, which can only improve the conductivity and are unable to accelerate lithium-ion transport. Therefore, it would be worthwhile to develop a catalytic electrode exhibiting both ion and electron conductivity. Herein, a triple-phase interface using lithium lanthanum titanate/carbon (LLTO/C) nanofibers to construct ion/electron co-conductive materials was used to afford enhanced adsorption of lithium polysulfides (LiPSs), high conductivity, and fast ion transport in working LSBs. The triple-phase interface accelerates the kinetics of the soluble LiPSs and promotes uniform Li2S precipitation/dissolution. Additionally, the LLTO/C nanofibers decrease the reaction barrier of the LiPSs, significantly improving the conversion of LiPSs to Li2S and promoting rapid conversion. Specifically, the LLTO promotes ion transport owing to its high ionic conductivity, and the carbon enhances the conductivity to improve the utilization rate of sulfur. Therefore, the LSBs with LLTO/C functional separators deliver stable life cycles, high rates, and good electrocatalytic activities. This strategy is greatly important for designing ion/electron conductivity and interface engineering, providing novel insight for the development of the LSBs.

研究领域: 材料科学 · 能源存储技术
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