Mesoscopic Framework Enables Facile Ionic Transport in Solid Electrolytes for Li Batteries

Ma Cheng; Cheng Yongqiang; Chen Kai; Li Juchuan; Sumpter Bobby G.; Nan Ce-Wen; More Karren L.; Dudney Nancy J.; Chi Miaofang

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Mesoscopic Framework Enables Facile Ionic Transport in Solid Electrolytes for Li Batteries

机译：介术框架使得能够在Li电池的固体电解质中进行体内离子传输

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Li-ion-conducting solid electrolytes can simultaneously overcome two grand challenges for Li-ion batteries: the severe safety concerns that limit the large-scale application and the poor electrolyte stability that forbids the use of high-voltage cathodes. Nevertheless, the ionic conductivity of solid electrolytes is typically low, compromising the battery performances. Precisely determining the ionic transport mechanism(s) is a prerequisite for the rational design of highly conductive solid electrolytes. For decades, the research on this subject has primarily focused on the atomic and microscopic scales, where the main features of interest are unit cells and microstructures, respectively. Here, it is shown that the largely overlooked mesoscopic scale lying between these extremes could be the key to fast ionic conduction. In a prototype system, (Li0.33La0.56)TiO3, a mesoscopic framework is revealed for the first time by state-of-the-art scanning transmission electron microscopy. Corroborated by theoretical calculations and impedance measurements, it is demonstrated that such a unique configuration maximizes the number of percolation directions and thus most effectively improves the ionic conductivity. This discovery reconciles the long-standing structure-property inconsistency in (Li0.33La0.56)TiO3 and also identifies mesoscopic ordering as a promising general strategy for optimizing Li+ conduction.

机译：锂离子导电固体电解质可以同时克服锂离子电池的两个大挑战：限制大规模应用的严重安全问题和禁止使用高压阴极的差的电解质稳定性。然而，固体电解质的离子电导率通常为低，损害电池性能。精确地确定离子传输机制是高导电固体电解质的合理设计的先决条件。几十年来，对该受试者的研究主要集中在原子和微观尺度上，其中感兴趣的主要特征是单位细胞和微观结构。这里，示出了躺在这些极端之间的主要忽略的介面尺度可以是快速离子传导的关键。在原型系统中，通过最先进的扫描透射电子显微镜首次揭示介面镜片框架。通过理论计算和阻抗测量得到证实，证明这种独特的配置最大化了渗透方向的数量，因此最有效地提高了离子电导率。该发现与（LI0.33LA0.56）TiO3相符，并调整了长期的结构性质不一致，并且还将介观序列识别为优化Li +传导的有希望的一般策略。

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《Advanced energy materials》 |2016年第11期|1600053.1-1600053.7|共7页
作者
Ma Cheng; Cheng Yongqiang; Chen Kai; Li Juchuan; Sumpter Bobby G.; Nan Ce-Wen; More Karren L.; Dudney Nancy J.; Chi Miaofang;
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Oak Ridge Natl Lab Ctr Nanophase Mat Sci Oak Ridge TN 37831 USA;

Oak Ridge Natl Lab Chem & Engn Mat Div Oak Ridge TN 37831 USA;

Tsinghua Univ State Key Lab New Ceram & Fine Proc Sch Mat Sci & Engn Beijing 100084 Peoples R China;

Oak Ridge Natl Lab Mat Sci & Technol Div Oak Ridge TN 37831 USA;

Oak Ridge Natl Lab Ctr Nanophase Mat Sci Oak Ridge TN 37831 USA|Oak Ridge Natl Lab Comp Sci & Math Div Oak Ridge TN 37831 USA;

Tsinghua Univ State Key Lab New Ceram & Fine Proc Sch Mat Sci & Engn Beijing 100084 Peoples R China;

Oak Ridge Natl Lab Ctr Nanophase Mat Sci Oak Ridge TN 37831 USA;

Oak Ridge Natl Lab Mat Sci & Technol Div Oak Ridge TN 37831 USA;

Oak Ridge Natl Lab Ctr Nanophase Mat Sci Oak Ridge TN 37831 USA;

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1. Behind the Candelabra: A Facile Flame Vapor Deposition Method for Interfacial Engineering of Garnet Electrolyte To Enable Ultralong Cycling Solid-State Li-FeF3 Conversion Batteries [J] . Zhang Yang, Meng Junwei, Chen Keyi, ACS applied materials & interfaces . 2020,第30期

机译：烛台后面：石榴石电解质界面工程的容易火焰气相沉积方法，以实现超循环固态Li-Fef3转换电池
2. Correlating Macro and Atomic Structure with Elastic Properties and Ionic Transport of Glassy Li_2S-P_2S_5 (LPS) Solid Electrolyte for Solid-State Li Metal Batteries [J] . Garcia-Mendez Regina, Smith Jeffrey G., Neuefeind Joerg C., Advanced energy materials . 2020,第19期

机译：具有弹性性能的宏观和原子结构，玻璃Li_2S-P_2S_5（LPS）固体电解质的弹性性能和离子传输
3. Superior All-Solid-State Batteries Enabled by a Gas-Phase-Synthesized Sulfide Electrolyte with Ultrahigh Moisture Stability and Ionic Conductivity [J] . Lu Pushun, Liu Lilu, Wang Shuo, Advanced Materials . 2021,第32期

机译：通过具有超高湿度稳定性和离子电导率的气相合成的硫化物电解液使能上级全固态电池
4. Room Temperature to 150°C Lithium Metal Batteries Enabled By a "Molecular Ionic Composite" Solid Electrolyte [C] . Deyang Yu, Xiaona Pan, Curt J. Zanelotti, Pacific Rim Meeting on Electrochemical and Solid-State Science . 2020

机译：通过“分子离子复合”固体电解质使得室温至150°C锂金属电池。
5. ION TRANSPORT IN POLYMERIC SOLID ELECTROLYTES: PART I. AN INVESTIGATION OF NEW POLYMERIC SOLID ELECTROLYTES BASED ON POLY(ALKYLENE SULFIDES) AND POLY(1,3-DIOXOLANE). PART II. POTENTIOSTATIC POLARIZATION CELL MEASUREMENTS OF IONIC TRANSFERENCE NUMBERS [D] . CLANCY, SHAUN FRANCIS 1985

机译：聚合物固体电解质中的离子迁移：第一部分。基于聚（亚烷基硫）和聚（1,3-二氧戊环）的新型聚合物固体电解质的研究。第二部分离子传递数的恒电位极化细胞测量
6. High-Performance Solid Composite Polymer Electrolyte for all Solid-State Lithium Battery Through Facile Microstructure Regulation [O] . Jingjing Yang, Xun Wang, Gai Zhang, 1970

机译：适用于全固态锂电池的高性能固态复合聚合物电解质，通过容易的微结构调节
7. Solid‐State Batteries: Correlating Macro and Atomic Structure with Elastic Properties and Ionic Transport of Glassy Li 2 S‐P 2 S 5 (LPS) Solid Electrolyte for Solid‐State Li Metal Batteries (Adv. Energy Mater. 19/2020) [O] . Regina Garcia‐Mendez, Jeffrey G. Smith, Joerg C. Neuefeind, 2020

机译：固态电池：将宏观和原子结构与玻璃Li 2 S-P 2 S 5（LPS）固体电解质的弹性性能和离子传输进行相关性，用于固态Li金属电池（ADV。能源母体。19/2020）

Mesoscopic Framework Enables Facile Ionic Transport in Solid Electrolytes for Li Batteries

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