JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2026
·Vol. 47
·期 2
·118837
·
IF 6.3
Chengjian Li,Abdullah Jabr,Christopher Parr,Andreas Börger,Chunfeng Liu,Raul Bermejo,Frank Kern
This work systematically investigates how lithium precursor and sintering strategy determine the processing–structure–property relationship of Nb-doped Li 7 La 3 Zr 2 O 12 (LLZNO) thin solid electrolytes. LLZNO thin electrolytes were fabricated by tape casting using a designed constrained-sintering methodology. A clear precursor-dependent evolution from powder characteristics to final microstructure and performance was identified. LiOH-derived powder showed more uniformly distributed particles with weaker agglomeration, enabling tighter packing and more homogeneous particle networks in the green tape. Consequently, the resulting thin electrolytes exhibited stable densification and similar ionic conductivities of 0.31–0.32 × 10 −3 S/cm at relative densities of ∼90–91%, regardless of sintering route. In contrast, Li 2 CO 3 -derived powder showed poorer particle contact and more heterogeneous packing, leading to non-uniform densification, lower ionic conductivities of 0.13–0.24 × 10 −3 S/cm at comparable densities, and greater sensitivity to the debinding–sintering routes. Overall, these findings provide insights into scalable fabrication of high-performance LLZO thin electrolytes.
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DOI
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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产品关联
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
Materials
·
2020
·Vol. 13
·期 3
·560
·
IF 3.057
Yan Ji,Cankai Zhou,Feng Lin,Bingjing Li,Feifan Yang,Huali Zhu,Junfei Duan,Zhaoyong Chen
The garnet Li7La3Zr2O12(LLZO) has been widely investigated because of its high conductivity, wide electrochemical window, and chemical stability with regards to lithium metal. However, the usual preparation process of LLZO requires high-temperature sintering for a long time and a lot of mother powder to compensate for lithium evaporation. In this study submicron Li6.6La3Zr1.6Nb0.4O12(LLZNO) powder―which has a stable cubic phase and high sintering activity―was prepared using the conventional solid-state reaction and the attrition milling process, and Li stoichiometric LLZNO ceramics were obtained by sintering this powder―which is difficult to control under high sintering temperatures and when sintered for a long time―at a relatively low temperature or for a short amount of time. The particle-size distribution, phase structure, microstructure, distribution of elements, total ionic conductivity, relative density, and activation energy of the submicron LLZNO powder and the LLZNO ceramics were tested and analyzed using laser diffraction particle-size analyzer (LD), X-Ray Diffraction (XRD), Scanning Electron Microscope (SEM), Electrochemical Impedance Spectroscopy (EIS), and the Archimedean method. The total ionic conductivity of samples sintered at 1200 °C for 30 min was 5.09 × 10−4S·cm−1, the activation energy was 0.311 eV, and the relative density was 87.3%. When the samples were sintered at 1150 °C for 60 min the total ionic conductivity was 3.49 × 10−4S·cm−1, the activation energy was 0.316 eV, and the relative density was 90.4%. At the same time, quasi-solid-state batteries were assembled with LiMn2O4as the positive electrode and submicron LLZNO powder as the solid-state electrolyte. After 50 cycles, the discharge specific capacity was 105.5 mAh/g and the columbic efficiency was above 95%.Keywords:solid-state electrolyte;submicron powder;garnet;lithium-ion conductivity;solid-state batteries
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）