{"title":"Unveiling the Structure and Diffusion Kinetics at the Composite Electrolyte Interface in Solid-State Batteries","authors":"Xueyan Zhang, Shichao Cheng, Chuankai Fu, Geping Yin, Pengjian Zuo, Liguang Wang, Hua Huo","doi":"10.1002/aenm.202401802","DOIUrl":null,"url":null,"abstract":"<p>The “interface” between polymer and oxide within the polymer-oxide composite electrolytes is widely acknowledged as a crucial factor influencing ionic conduction. However, a fundamental understanding of the precise composition and/or micro-structure, and the ionic conduction mechanism at the complex interface has remained elusive, primarily due to a dearth of compelling experimental evidence. In this study, the intricate correlation between morphology and composition in composite electrolytes is discerned by leveraging advanced 1D and 2D exchange nuclear magnetic resonance spectroscopy (1D and 2D EXSY NMR) techniques. Notably, this research represents the inaugural elucidation of the microstructure of the interface. The findings underscore the pivotal role of the preparation conditions for polymer-oxide composite electrolytes, particularly the solvent selection, in determining the formation of the interface structure. Direct insights into the lithium-deficient surface of Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> (LLZTO) are provided and elucidate the timescales of Li-ion exchange processes among various components. Furthermore, a comprehensive investigation into the roles of individual components within the composite electrolyte on the Li-ion conduction mechanism is conducted through the <sup>6</sup>Li→<sup>7</sup>Li isotope tracer technique as a function of current density.</p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":24.4000,"publicationDate":"2024-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Energy Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401802","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The “interface” between polymer and oxide within the polymer-oxide composite electrolytes is widely acknowledged as a crucial factor influencing ionic conduction. However, a fundamental understanding of the precise composition and/or micro-structure, and the ionic conduction mechanism at the complex interface has remained elusive, primarily due to a dearth of compelling experimental evidence. In this study, the intricate correlation between morphology and composition in composite electrolytes is discerned by leveraging advanced 1D and 2D exchange nuclear magnetic resonance spectroscopy (1D and 2D EXSY NMR) techniques. Notably, this research represents the inaugural elucidation of the microstructure of the interface. The findings underscore the pivotal role of the preparation conditions for polymer-oxide composite electrolytes, particularly the solvent selection, in determining the formation of the interface structure. Direct insights into the lithium-deficient surface of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) are provided and elucidate the timescales of Li-ion exchange processes among various components. Furthermore, a comprehensive investigation into the roles of individual components within the composite electrolyte on the Li-ion conduction mechanism is conducted through the 6Li→7Li isotope tracer technique as a function of current density.
期刊介绍:
Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small.
With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics.
The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.