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Isomeric Li–La–Zr–O Amorphous–Crystalline Composite Thin-Film Electrolytes for All-Solid-State Lithium Batteries
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2021-08-01 , DOI: 10.1021/acsaem.1c01710 Shidong Song 1, 2 , Yongqiang Xu 1 , Yanli Ruan 1 , Hong Wang 3 , Dequan Zhang 1 , Joykumar Thokchom 4 , Donghai Mei 5
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2021-08-01 , DOI: 10.1021/acsaem.1c01710 Shidong Song 1, 2 , Yongqiang Xu 1 , Yanli Ruan 1 , Hong Wang 3 , Dequan Zhang 1 , Joykumar Thokchom 4 , Donghai Mei 5
Affiliation
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Amorphous Li–La–Zr–O (LLZO) solid-state electrolyte thin films are promising alternatives to the well-established lithium phosphorus oxynitride (LiPON) electrolyte for all-solid-state lithium batteries due to their potentially higher Li-ion conductivity and stability. Herein, the enhancement methodology in the ionic conductivity of amorphous LLZO-based thin films is investigated. By doping with Ta, the conductivity of the amorphous LLZO film at 30 °C (3.9 × 10–7 S cm–1) can be enhanced by up to an order of magnitude (2.6 × 10–6 S cm–1), ascribed to tuning Li conduction in local near-order LLZO nanodomains. On that basis, an isomeric Li–La–Zr–Ta–O (LLZTO) amorphous–crystalline composite thin film is prepared via incorporating cubic LLZTO particles into the amorphous LLZTO matrix. The composite film with 10 wt % cubic LLZTO filler can further achieve an ionic conductivity of 0.8 × 10–5 S cm–1 at 30 °C, which is comparable to the best values obtained for the state-of-art LLZO-based thin films. Li transport through the well-connected cubic LLZTO filler network and along the interfaces between the crystallites and the amorphous matrix in the LLZTO composite thin film may offer fast and long-range Li-conduction pathways, which supplement the ionic conduction in the amorphous matrix with short-range-ordered and long-range-disordered structures.
中文翻译：
用于全固态锂电池的异构 Li-La-Zr-O 非晶-结晶复合薄膜电解质
无定形 Li-La-Zr-O（LLZO）固态电解质薄膜是用于全固态锂电池的成熟锂磷氧氮化物（LiPON）电解质的有前途的替代品，因为它们具有更高的锂离子电导率和稳定性。在此，研究了非晶 LLZO 基薄膜离子电导率的增强方法。通过掺杂 Ta，非晶 LLZO 薄膜在 30 °C (3.9 × 10 –7 S cm –1 )的电导率可以提高一个数量级 (2.6 × 10 –6 S cm –1)，归因于在局部近阶 LLZO 纳米域中调节锂传导。在此基础上，通过将立方 LLZTO 颗粒掺入非晶 LLZTO 基体中，制备了异构 Li-La-Zr-Ta-O (LLZTO) 非晶-晶体复合薄膜。含有 10 wt% 立方 LLZTO 填料的复合膜可以进一步实现 0.8 × 10 –5 S cm –1的离子电导率在 30 °C 时，这与最先进的基于 LLZO 的薄膜获得的最佳值相当。通过连接良好的立方 LLZTO 填料网络以及沿 LLZTO 复合薄膜中微晶和非晶基体之间的界面的锂传输可以提供快速和长程的锂传导途径，补充非晶基体中的离子传导短程有序和长程无序结构。
更新日期：2021-08-23
中文翻译：
用于全固态锂电池的异构 Li-La-Zr-O 非晶-结晶复合薄膜电解质
无定形 Li-La-Zr-O（LLZO）固态电解质薄膜是用于全固态锂电池的成熟锂磷氧氮化物（LiPON）电解质的有前途的替代品，因为它们具有更高的锂离子电导率和稳定性。在此，研究了非晶 LLZO 基薄膜离子电导率的增强方法。通过掺杂 Ta，非晶 LLZO 薄膜在 30 °C (3.9 × 10 –7 S cm –1 )的电导率可以提高一个数量级 (2.6 × 10 –6 S cm –1)，归因于在局部近阶 LLZO 纳米域中调节锂传导。在此基础上，通过将立方 LLZTO 颗粒掺入非晶 LLZTO 基体中，制备了异构 Li-La-Zr-Ta-O (LLZTO) 非晶-晶体复合薄膜。含有 10 wt% 立方 LLZTO 填料的复合膜可以进一步实现 0.8 × 10 –5 S cm –1的离子电导率在 30 °C 时，这与最先进的基于 LLZO 的薄膜获得的最佳值相当。通过连接良好的立方 LLZTO 填料网络以及沿 LLZTO 复合薄膜中微晶和非晶基体之间的界面的锂传输可以提供快速和长程的锂传导途径，补充非晶基体中的离子传导短程有序和长程无序结构。
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