Identifying Migration Channels and Bottlenecks in Monoclinic NASICON‐Type Solid Electrolytes with Hierarchical Ion‐Transport Algorithms. (7th September 2021)

• Record Type: Journal Article
• Authors: Zou, Zheyi; Ma, Nan; Wang, Aiping; Ran, Yunbing; Song, Tao; He, Bing; Ye, Anjiang; Mi, Penghui; Zhang, Liwen; Zhou, Hang; Jiao, Yao; Liu, Jinping; Wang, Da; Li, Yajie; Avdeev, Maxim; Shi, Siqi
• Is Part Of: Advanced functional materials. Volume 31:Number 49(2021)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2021-09-07
• Subjects: ab initio molecular dynamics -- bond‐valence energy landscape -- geometric analysis -- migration channels -- solid electrolytes; Materials -- Periodicals; Chemical vapor deposition -- Periodicals; 620.11
• DOI: 10.1002/adfm.202107747
• Languages: English
• ISSNs: 1616-301X

Abstract

Abstract: Monoclinic natrium superionic conductors (NASICON; Na3 Zr2 Si2 PO12 ) are well‐known Na‐ion solid electrolytes which have been studied for 40 years. However, due to the low symmetry of the crystal structure, identifying the migration channels of monoclinic NASICON accurately still remains unsolved. Here, a cross‐verified study of Na + diffusion pathways in monoclinic NASICON by integrating geometric analysis of channels and bottlenecks, bond‐valence energy landscapes analysis, and ab initio molecular dynamics simulations is presented. The diffusion limiting bottlenecks, the anisotropy of conductivity, and the time and temperature dependence of Na + distribution over the channels are characterized and strategies for improving both bulk and total conductivity of monoclinic NASICON‐type solid electrolytes are proposed. This set of hierarchical ion‐transport algorithms not only shows the efficiency and practicality in revealing the ion transport behavior in monoclinic NASICON‐type materials but also provides guidelines for optimizing their conductive properties that can be readily extended to other solid electrolytes. Abstract : Na + diffusion pathways in monoclinic natrium superionic conductors (NASICON) are identified by integrating geometric analysis, bond‐valence energy landscapes analysis, and ab initio molecular dynamics simulations. This set of hierarchical algorithms not only shows efficiency and practicality in revealing the ion transport in monoclinic NASICON, but also provides guidelines for optimizing their conductive properties that can be extended to other fast ion conductors.