Advanced Materials Interfaces
·
2020
·Vol. 7
·期 20
·2000830
·
IF 4.948
Sajid Hussain Siyal,Muhammad Sufyan Javed,Ashique Hussain Jatoi,Jin-Le Lan,Yunhua Yu,Muhammad Saleem,Xiaoping Yang
Lithium–metal batteries (LiMBs) are promising energy storage devices due to the high capacity and minimum negative electrochemical potential. Nevertheless, their concrete applications remain disturbed by unbalanced electrolyte–electrode interfaces, limited electrochemical window, and high risk. Herein, a novel strategy to obtain dual ceramic-based electrolytes that possesses a great potential in energy storages and higher level of energy densities in LiMBs. Dual-ceramic (lithium aluminum titanium phosphate -lithium lanthanum titanium oxide (LATP-LLTO)) gel polymer electrolyte (DCGPE) film developed via the curable system aims to prepare flexible Li + interpenetrating network film to integrate the two ceramic structures with polyethylene oxide (PEO) to yield the free-standing electrolytes film for better battery safety and desired interfacial stability. The DCGPEs films present a satisfactory electrochemical performance, including good ionic conductivity, large transference number, and wide electrochemical stability window at room temperature. Most importantly, the fundamental function of LATP and LLTO is to support building a stable solid-electrolyte-interphase and limits the growth of dendrites. Thus, prepared dual ceramic-based electrolytes effectively render to inhibit lithium dendrite growth in a symmetrical cell Li//PEO + 10% LATP + 15% LLTO//Li test during charge/discharge at a current density of 2 and 0.25 mA cm −2 above 2400 h without short-circuiting occurrence at room temperature. Besides, the battery assembled of LiFePO 4 /PEO + 10% LATP + 20% LLTO/Li exhibits superior cyclic stability with high Coulombic efficiency. This study recommends that the binary network structures of Li-ion conductor help to design a prime solution of promising electrolyte for high-performance LiMBs applications.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Yong Liu,Chong Liu,Ting Zhao,Weijie Kou,Quanxian Hua,Wenhao Ren,Wenjia Wu
Inorganic superionic conductors hold great promise for all-solid-state lithium batteries because of their superior ionic conductivity. However, their application as electrolytes is limited by the trade-off between ion conduction and stability. Here, a thin composite solid electrolyte, vermiculite-Li 0.33 La 0.557 TiO 3 /poly(ethylene oxide) (Vr-LLTO/PEO), is prepared by in-situ co-sintering an interconnected Vr-LLTO framework and then impregnating PEO. Within this electrolyte, the continuous LLTO on Vr nanosheet surface acts as efficient pathways for vertical Li + transfer with reduced grain boundary resistance. Together with the thin thickness (35 μm), Vr-LLTO/PEO electrolyte attains the ionic conductivity as high as 1.04 × 10 −4 S cm −1 at 25 °C, over three times that of LLTO pellet and surpassing that of most reported ceramic electrolytes. Furthermore, the disordered stacked Vr nanosheets in framework are covalently linked by LLTO, together with the flexible PEO matrix, achieving highly enhanced structural stability with compressive strength of 319 MPa. In this manner, the trade-off between ion conduction and stability is overcome, which allows the assembled LiFePO 4 /Li cell achieving satisfactory cycling performances: an initial discharge capacity of 150.3 mAh g − 1 at 1 C and capacity decay of only 0.08% per cycle after 200 cycles. This study may inspire insights into the subtle design of conductive and stable electrolytes for high-performance devices.
研究领域:
材料科学
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能源技术
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 12.5
Boyu Li,Jiajing Liu,Huan Wang,Huanhuan Ren,Yanlei Shen,Ziyao Zhang,Yuman Zhou,Weitao Zhou,Jianxin He
Lithium–sulfur batteries (LSBs) suffer from sluggish sulfur redox kinetics and severe polysulfide shuttle, especially under lean-electrolyte conditions. Here, we report a cobalt-doped lithium lanthanum titanate (LLTO) perovskite that constructs ion/electron co-conductive catalytic interfaces to promote rapid sulfur reduction. Co doping induces oxygen vacancies and lattice distortion, thereby enhancing electronic conductivity, local density of states, and catalytic activity. These structural regulations endow LLTO with strong polysulfide adsorption and fast conversion capability. As a result, LSBs with LLTO-Co-modified separators exhibit excellent electrochemical performance, delivering high specific capacity, superior rate capability, and long-term cycling stability. Even at a high sulfur loading of 9 mg·cm −2 and a low electrolyte/sulfur ratio (E/S = 4 μL·mg −1 ), an areal capacity of 10.1 mAh·cm −2 is achieved and maintained at 7.2 mAh·cm −2 after 30 cycles. This work demonstrates a robust strategy of tailoring ion/electron co-conductive catalytic interfaces via lattice engineering, offering new insights for the design of high-performance LSBs.
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Zhaoze Fan,Jiayuan Xiang,Qiong Yu,Xianzhang Wu,Min Li,Xiuli Wang,Xinhui Xia,Jiangping Tu
Sulfide-based all-solid-state lithium batteries (ASSLBs) assembled with Ni-rich layered cathodes are currently promising candidates for achieving high-energy-density and high-safety energy storage systems. However, the interfacial challenges between sulfide electrolyte and Ni-rich layered cathode, such as space charge layer, side reaction, and poor physical contact, greatly limit the practicality of all-solid-state batteries. In this work, an optimal crystalline Li0.35La0.55TiO3 (LLTO) surface coating with a thickness of roughly 6 nm and a high Li ion conductivity of 0.3 mS cm–1 was adopted to enhance the structural stability of the single-crystal LiNi0.6Co0.2Mn0.2O2 (S-NCM622) cathode in ASSLBs. Furthermore, due to the high ionic conductivity and chemical stability of the LLTO coating layer, the interfacial problems, involving interfacial reaction and a space charge layer, in sulfide-based all-solid-state batteries have been effectively solved. As a result, the assembled ASSLBs with the S-NCM622@LLTO cathode exhibit high initial capacity (179.7 mAh g–1) at 0.05 C and excellent cycling performance with 84.5% capacity retention after 100 cycles at 0.1 C at room temperature. This work proposes an effective strategy to enhance the performance of Ni-rich layered cathodes for next-generation high-energy-density sulfide-based lithium batteries.
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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锂电池
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Boyu Li,Huan Wang,Weitao Zhou,Fan Liu,Jianxin He,Gaohui Du,Qingmei Su
Solid-state lithium (Li) metal batteries (LMBs) are promising owing to enhanced safety and high energy density . However, the issues of Li dendrite growth and large electrolyte-electrode interfacial resistance still hinder their practical applications in LMBs. Here, a Li anode-electrolyte structure integration has been developed using in-situ chemical reactions between the polyvinylidene fluoride/Li 3x La 2/3−x TiO 3 /N-methyl pyrrolidone (PVDF/LLTO/NMP) solution and the Li metal interphase. After gradually coating the PVDF/LLTO/NMP solution onto Li metal, NMP as catalyst, inducing PVDF reacted with Li spontaneously to form lithium fluorine (LiF), and the accompanying Ti 4+ ions (in LLTO) are reduced to Ti 3+ ions to form a LLTO ionic/electronic conductor (Li x LLTO). After NMP evaporation, an ionic/electronic conductor protective layer of LiF/Li x LLTO is created between the PVDF/LLTO electrolytes and Li metal. When applying the integrated solid-state Li batteries (ISSLBs), the protective layer can reduce interfacial resistance and the formation of Li dendrites by regulating the even Li deposition redistributing the Li-ion transport. As a result, the as-assembled LiNi 0.8 Co 0.1 Mn 0.1 O 2 /ISSLBs achieves an initial capacity of 181 mA h g −1 and retains 83% capacity after 200 cycles at 0.5 C. This design can be an effective strategy to tailor the properties of Li-metal anodes for achieving dendrite-free LMBs with high performance and high safety.
研究领域:
材料科学
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电化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Chong Liu,Junxiao Wang,Weijie Kou,Zhihao Yang,Pengfei Zhai,Yong Liu,Wenjia Wu,Jingtao Wang
All-solid-state lithium batteries, featuring high security and volume energy density, hold great potential as next-generation energy storage device. However, their development needs the fabrication of ionic conductive and structural stable solid electrolyte. Herein, Li 0.33 La 0.557 TiO 3 (LLTO) framework with interlocked porous structure is synthesized by sintering the gel permeated nylon. Then, poly(ethylene oxide) (PEO) is incorporated in the pores to produce PEO-LLTO framework solid electrolyte (PLLF electrolyte) with vertically bicontinuous phase. We demonstrate that LLTO framework fast transports Li + through the intrinsic vacancy; meanwhile the confined PEO with low crystallization displays fast Li + transfer ability, thus synergistically realizing efficient Li + conduction. This novel PLLF electrolyte exhibits a remarkable ionic conductivity of 2.04 × 10 −4 S cm −1 , which is ~72 times higher than that of traditional PEO-based electrolytes and superior to most reported solid electrolytes. Moreover, the interconnected networks endow PLLF electrolyte with excellent structural stability. Thus, the LiFePO 4 (LFP)/Li cell exhibits extraordinary cycling stability: the discharge capacity of 154.7 mAh g −1 at 1 C after 150 cycles with capacity decay of only 0.03% per cycle. Briefly, such a vertically bicontinuous phase structure maximizes the cooperation between the conduction function of ceramic framework and the stability of polymer, offering a promising approach for all-solid-state batteries.
研究领域:
材料科学
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能源存储技术
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产品关联
DOI
高影响因子
Materials
·
2026
·Vol. 19
·期 14
·3113
·
IF 3.7
Dingqin Wang,Zihao Fei,Deyi Zheng
Poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) polymer electrolytes suffer from low ionic strength and poor mechanical performance. Meanwhile, lithium lanthanum titanate (LLTO) fillers exhibit severe agglomeration and weak interfacial compatibility with the polymer matrix. To solve these problems, 3-glycidoxypropyltrimethoxysilane (KH560) at four different concentrations (1 wt%, 2 wt%, 3 wt%, 4 wt%) was loaded onto polydopamine-modified LLTO (PDA@LLTO). The modified materials were mixed with PVDF-HFP, and composite solid electrolytes were fabricated by the solution casting method. The epoxy groups in KH560 undergo ring-opening reactions with amino and hydroxyl moieties on PDA, while its trimethoxysilane groups crosslink with the polymer matrix, forming a robust “LLTO-PDA-KH560-polymer” interfacial structure. This dual modification markedly improves the dispersion of PDA@LLTO, strengthens interfacial adhesion, and enhances the mechanical and electrochemical properties of the composite electrolyte. All KH560 loadings suppress LLTO agglomeration, and the 3 wt% grafting ratio yields the optimal performance: a uniform and dense microstructure, a room-temperature ionic conductivity of 5.92 × 10 −4 S cm −1 , an electrochemical stability window extended to 4.88 V, and a tensile strength over 50% higher than the ungrafted sample. The modified electrolyte effectively inhibits lithium dendrite growth and enhances the cycling stability of solid-state batteries. This work demonstrates that KH560-PDA synergistic modification enables comprehensive performance optimization of composite electrolytes, offering a viable strategy for designing high-performance electrolytes for solid-state lithium-metal batteries.
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DOI
PubMed
高影响因子
DESALINATION
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2026
·
IF 9.9
Jilong Han,Ruyi Shi,Mochi Li,Huanzhang Lu,Yijian Zheng,Pengfei Li,Jisheng Li
Dense LLTO-Al 2 O 3 membrane (∼20 μm) for /Li + from high Mg 2+ /Li + brine. • Optimised LLTO (x = 0.11, 1250 °C/6 h): tetragonal, 3.26 × 10 3 S/cm. • La-poor/La-rich enables 2D Li + transport; Mg 2+ blocked by size. • Intergranular defects are main pathway for Mg 2+ co-permeation. • Selectivity 16.06, 99.61% Mg 2+ rejection (6 h); energy 23.21 kW·h (24 h). To solve the problem of lithium extraction from salt lake brine with a high magnesium‑lithium ratio, a composite ceramic membrane electrodialysis technology based on perovskite-type superionic conductor Li 3x La 2/3-x TiO 3 (LLTO) was proposed. LLTO powder was synthesised by the sol-gel method. The lithium doping amount (x = 0.11), sintering temperature (1250 °C) and time (6 h) were systematically optimised to obtain tetragonal LLTO with high ionic conductivity (3.26 × 10 −3 S/cm). Then, the LLTO-Al 2 O 3 composite film was prepared by a spin coating process (PVA content of 20%, LLTO solid content of 0.08 g/mL, spin coating 10 times) with porous alumina as the substrate. After calcination at 1275 °C for 6 h, a dense film with a thickness of about 20 μm was formed. Molecular dynamics simulations show that the two-dimensional selective transport of Li can be realised in the LLTO inner layer based on the La-poor / La-rich alternating structure, while Mg 2+ is hindered by the size effect. Intergranular defects are the main pathway leading to the co-permeation of Mg 2+ . The electrodialysis experiment showed that the membrane had good selectivity (selectivity coefficient 16.06) and Mg 2+ rejection rate (99.61%) for Li at the initial stage of operation (6 h), and the energy consumption was 23.21 kWh after 24 h of electrodialysis. This study provides a reference for membrane material design, preparation process and transmission mechanism for lithium extraction from high magnesium‑lithium ratio brine, and has potential application value.
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高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Fangyu Hao,Hao Zheng,Mingtai Hou,Hao Zhou,Lin Lin,Zeyi Jiang,Nien-Chu Lai
The development of all-solid-state lithium batteries (ASSLBs) currently faces challenges such as the need for electrolyte materials to possess high chemical stability, high ionic conductivity, and excellent compatibility with lithium (Li) metal anodes. Herein, a facile template-free sintering method for three-dimensional porous Li 0.5 La 0.5 TiO 3 (LLTO) framework is reported. By integrating these frameworks with a poly(ethylene oxide) (PEO) matrix, a new-type composite polymer electrolyte (CPE) is fabricated. In the CPE, the crystallinity and melting point of the PEO matrix are significantly reduced, which is beneficial for enhancing the Li + conductivity and transference number. Incorporating fluoroethylene carbonate (FEC) facilitates the formation of a robust SEI layer on the Li foil surface, significantly mitigating Li dendrite growth and interfacial degradation. The optimized CPE2F electrolyte enables stable Li||Li symmetric cell cycling for over 1000 h at 0.1 mA cm −2 and demonstrates superior full-cell performance: the LiFePO 4 ||Li configuration achieving a high specific capacity of 144.5 mAh g −1 at 0.5 C and 60 °C, retaining 94.5% capacity after 500 cycles. This work provides an efficient and scalable approach for producing solid electrolytes suitable for all-solid-state batteries.
研究领域:
材料科学
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电化学
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能源存储
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固体离子学
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电池技术
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 11
·9074-9079
·
IF 3.201
Zhixiong Hu,Jiali Sheng,Jiahui Chen,Guoqing Sheng,Yunming Li,Xian-Zhu Fu,Lei Wang,Rong Sun,Ching-Ping Wong
Ge-Doped Li0.33La0.56TiO3 (Ge-LLTO) perovskites are synthesized with various GeO2 contents by solid-state reactions as Li-ion conductive electrolytes for rechargeable all-solid-state Li batteries. After the addition of GeO2, the sinterability and Li ion conductivity are enhanced for the perovskite solid electrolyte. The Li0.43La0.56Ti0.95Ge0.05O3 electrolytes exhibit the highest sinterability and Li ion conductivity among the as-prepared Li0.33+2xLa0.56Ti1−xGexO3 electrolytes. The improvement of Li ion conductivity might be attributed to the improvement of the densification and structural integrity of the LLTO solid electrolyte. The lithium transference number (tLi+) of Ge-doped LLTO is close to 1. Moreover, the Ge-LLTO electrolytes are stable in the potential range of 0–10 V vs. Li/Li+.
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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固体离子学
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DOI
高影响因子
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