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Fluorine Substitution at the O-Site Imparts Enhanced Chemical Stability for Garnet-Structured Electrolytes
ACS Energy Letters ( IF 22.0 ) Pub Date : 2022-11-17 , DOI: 10.1021/acsenergylett.2c02329
Jingyu Shi, Ge Sun, Liping Li, Yuanhua Xia, Fei Du, Xiaojuan Liu, Hongwei Hou, Xiangyan Hou, Beining Zheng, Xiaofeng Wu, Keke Huang, Shouhua Feng

Garnet-based superionic conductors hold great promise in next-generation lithium-ion batteries (LIBs) because of their favorable ionic conductivity and unique stability against Li-metal anodes; however, they still face the challenge of air stability for mass production/practical application. Herein, we identify their structural features and tailor the functional elements to enhance the chemical stability via synergistic control of doping and non-stoichiometry. The optimal composition of Li6.25Ga0.2La3Zr2O11.85F0.15 (LGLZO-0.15F) garnet exhibits great air durability without noticeable impurity accumulation, even during continuous air exposure for 60 days, owing to the high affinity of the fluorine dopant for lithium occupying the octahedral site. Meanwhile, LGLZO-0.15F possesses an appreciable Li-ion conductivity of 8.4 × 10–4 S cm–1 with an activation energy of 0.29 eV. Benefiting from these properties, hybrid and all-solid-state lithium batteries constructed with LGLZO-0.15F electrolytes demonstrate low overpotential, high Coulombic efficiency, and stable cycling performance.

中文翻译:

O 位点的氟取代提高了石榴石结构电解质的化学稳定性

基于石榴石的超离子导体在下一代锂离子电池 (LIB) 中具有广阔的应用前景,因为它们具有良好的离子导电性和对锂金属阳极的独特稳定性;然而,它们仍然面临大规模生产/实际应用的空气稳定性挑战。在此,我们确定了它们的结构特征并定制功能元素,以通过掺杂和非化学计量的协同控制来增强化学稳定性。Li 6.25 Ga 0.2 La 3 Zr 2 O 11.85 F 0.15的最佳组成(LGLZO-0.15F) 石榴石具有出色的空气耐久性,即使连续暴露在空气中 60 天也没有明显的杂质积累,这是由于氟掺杂剂对占据八面体位点的锂具有高亲和力。同时,LGLZO-0.15F 具有 8.4 × 10 –4 S cm –1的可观锂离子电导率和 0.29 eV 的活化能。受益于这些特性,使用 LGLZO-0.15F 电解质构建的混合和全固态锂电池表现出低过电位、高库仑效率和稳定的循环性能。
更新日期:2022-11-17
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