Ga3+和Ta5+共掺杂Li7La3Zr2O12 （LLZO）对离子电导率和空气稳定性的协同改性

IF 3.8 3区材料科学 Q1 MATERIALS SCIENCE, CERAMICS

Journal of the American Ceramic Society Pub Date : 2025-04-16 DOI:10.1111/jace.20576

Run Yu, Yongjin Chen, Chengyu Li, Shaojun Wang, Pengcheng Li, Ruihan Tang, Cong Gao, Chuanlong Lin, Xiang Gao

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引用次数: 0

摘要

石榴石型氧化物Li7La3Zr2O12固态电解质（ses）由于其优异的性能被认为是全固态锂电池（asslb）的可靠选择。然而，它仍然面临着诸如有限的离子电导率和低空气稳定性等挑战。通过固相法合成的Ga3+和Ta5+共掺杂样品Li7−3x−yGaxLa3Zr2−yTayO12 (gaxtayi -LLZO)，可以稳定立方相，调节LLZO中Li空位的浓度，改善Li+的输运通道。结果，Ga0.1Ta0.3-LLZO样品获得了~ 1 mS cm−1的高电导率。此外，我们发现除了先前报道的晶界密度降低和晶界惰性LiGaO2二次相的影响外，引入多种掺杂离子的协同效应，增强了晶格稳定性，也是提高空气稳定性的关键因素。研究结果表明，Ga3+/Ta5+共掺杂策略是同时提高LLZO电导率和空气稳定性的有效方法，为sss在asslb中的应用奠定了坚实的基础。

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The synergetic modification on ionic conductivity and air stability of Ga3+ and Ta5+ co-doped Li7La3Zr2O12 (LLZO)

The garnet-type oxide Li₇La₃Zr₂O₁₂ 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, Ga³⁺ and Ta⁵⁺ co-doped samples Li₇₋₃_x₋_yGa_xLa₃Zr₂₋_yTa_yO₁₂ (GaxTay-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 LiGaO₂ 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 Ga³⁺/Ta⁵⁺ is an effective method for simultaneously enhancing conductivity and air stability of LLZO, laying solid foundation for the application of SSEs in ASSLBs.

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来源期刊

Journal of the American Ceramic Society 工程技术-材料科学：硅酸盐

CiteScore

7.50

自引率

7.70%

发文量

590

审稿时长

2.1 months

期刊介绍： The Journal of the American Ceramic Society contains records of original research that provide insight into or describe the science of ceramic and glass materials and composites based on ceramics and glasses. These papers include reports on discovery, characterization, and analysis of new inorganic, non-metallic materials; synthesis methods; phase relationships; processing approaches; microstructure-property relationships; and functionalities. Of great interest are works that support understanding founded on fundamental principles using experimental, theoretical, or computational methods or combinations of those approaches. All the published papers must be of enduring value and relevant to the science of ceramics and glasses or composites based on those materials. Papers on fundamental ceramic and glass science are welcome including those in the following areas: Enabling materials for grand challenges[...] Materials design, selection, synthesis and processing methods[...] Characterization of compositions, structures, defects, and properties along with new methods [...] Mechanisms, Theory, Modeling, and Simulation[...] JACerS accepts submissions of full-length Articles reporting original research, in-depth Feature Articles, Reviews of the state-of-the-art with compelling analysis, and Rapid Communications which are short papers with sufficient novelty or impact to justify swift publication.