JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2025
·
IF 3.8
Run Yu,Yongjin Chen,Chengyu Li,Shaojun Wang,Pengcheng Li,Ruihan Tang,Cong Gao,Chuanlong Lin,Xiang Gao
The garnet-type oxide Li 7 La 3 Zr 2 O 12 solid-state electrolytes (SSEs) are considered as a reliable option in all-solid-state lithium batteries (ASSLBs) due to its excellent properties. However, it still faces challenges such as limited ionic conductivity and low air stability. In this work, Ga 3+ and Ta 5+ co-doped samples Li 7−3 x − y Ga x La 3 Zr 2− y Ta y O 12 (Ga x Ta y -LLZO) synthesized via the solid-state method are demonstrated to stabilize the cubic phase, regulate the concentration of Li vacancies in LLZO, and improving the Li + transport channels. As a result, the Ga0.1Ta0.3-LLZO sample achieves a high conductivity of ∼1 mS cm −1 . Furthermore, we discovered that in addition to the previously reported effects of decreasing grain boundary density and the inert LiGaO 2 secondary phase at grain boundaries, the synergistic effect of introducing multiple dopant ions, which enhances lattice stability, is also a key factor contributing to improved air stability. Our findings demonstrate that co-doping strategy with Ga 3+ /Ta 5+ is an effective method for simultaneously enhancing conductivity and air stability of LLZO, laying solid foundation for the application of SSEs in ASSLBs.
研究领域:
材料科学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2024
·
IF 18.9
Liu Xing-kun,Zhou Yi-xuan,Mi Fang-hui,Ma Xue-lu,Chun-wen Sun
Zirconium-based halide solid electrolyte, Li 2 ZrCl 6 , with low raw-material cost and high oxidative stability is a promising candidate for next-generation energy storage devices. However, the low ionic conductivity hinders its practical applicability. Herein, we report a new zirconium-based superionic conductor based on high-valence Ta 5+ doping strategy. The optimized Li 1.7 Zr 0.7 Ta 0.3 Cl 6 (LZTC) exhibits excellent ionic conductivity of 1.42 mS cm -1 at 25°C. Moreover, it can be further increased up to 1.68 mS cm -1 with a low activation energy of 0.28 eV by slightly tuning Li + concentration. In addition, LZTC possesses a big compact density of 2.67 g cm -3 under 250 MPa and is compatible with 4V-class cathodes. Density function theory (DFT) and bond valence site energy (BVSE) calculations reveal Ta 5+ substitution significantly reduces the migration energy barrier of lithium ions due to the distortions and defects of local structural environment. The assembled all-solid-state batteries with Li 1.7 Zr 0.7 Ta 0.3 Cl 6 as electrolyte and scNCM811 as cathode show excellent cycling performance for 600 cycles at 1C with a high-capacity retention of 85.7%.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Hanwei Zhang,Xiaoyun Zhang,Tianyi Zeng,Aichun Dou,Panpan Zhang,Mingru Su,Yu Zhou,Yunjian Liu
The application of Ni-rich ternary cathode materials is restricted by the irreversible phase transition and interfacial side reactions during long-term cycling. Herein, a LiTaO 3 coating and Ta 5+ doping strategy are simultaneously achieved by a simple solid-phase synthesis. The surface side-reaction and undesired phase transition of LiNi 0.8 Co 0.15 Al 0.05 O 2 (NCA) are effectively restrained by this approach, which utilizes residual lithium to afford the coating. The NCA-LTO 3 (The modified NCA with a LiTaO 3 coating content of 3 wt%) delivers a high reversible capacity of 168.04 at 5 C (140.56 mAh g −1 for NCA), revealing the enhanced rate capability. More importantly, the cycling life could be greatly maintained after 200 cycles with a significant capacity retention of 94.1% (61.2% for NCA) at 1 C. Mechanism analysis indicates that such improvement is ascribed to the coating of conductor LiTaO 3 and doping Ta 5+ greatly promoting the Li-ion diffusion and stabilizing the interface of NCA. The study proposes a highly convenient strategy for interfacial optimization of cathode materials toward assisting the large-scale production of high-performance NCA.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态化学
·
电池技术
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Lei Gao,Zhigang Zhang,Zheyuan Zhang,Yongrui Luo,Bolong Hong,Longbang Di,Haijin Ni,Jinlong Zhu,Ruqiang Zou,Enyue Zhao,Songbai Han
The halide solid-state electrolyte (SSE) Li 2 ZrCl 6 has emerged as a promising candidate for all-solid-state batteries (ASSBs) due to the abundance of Zr in the Earth's crust and its low cost. However, its relatively low ionic conductivity prevents it from meeting the essential performance threshold (> 1 mS cm −1 ) required for application in ASSBs. In this work, a novel strategy is presented to enhance ionic conductivity by incorporating high-valence Ta 5+ into the Li 2 ZrCl 6 framework, resulting in a series of Li-deficient Li 2– x Ta x Zr 1– x Cl 6 (LTZC, 0 ≤ x ≤ 0.4) SSEs. Remarkably, the LTZC ( x = 0.275) achieves a high ionic conductivity of 1.43 mS cm −1 at 30 °C, surpassing that of Li-rich Li 2 ZrCl 6 -based SSEs (e.g., Li 2+2 x Zr 1– x Mg x Cl 6 ). Neutron powder diffraction reveals a pronounced rearrangement of Li + ions upon Ta 5+ doping, and bond-valence site energy calculations indicate that this rearrangement enhances Li + transport within the lattice. Furthermore, ASSBs incorporating LTZC SSE with LiCoO 2 or LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode and Li-In anode exhibit excellent cycling performance. This work underscores the effectiveness of structural regulation in developing Li-deficient halide SSEs as a viable strategy for enhancing their electrochemical performance.
研究领域:
材料科学
·
电化学
·
储能
·
固态离子学
✓ 已验证
产品关联
DOI
高影响因子