Liquid-Like Li-Ion Conduction in Oxides Enabling Anomalously Stable Charge Transport across the Li/Electrolyte Interface in All-Solid-State Batteries

Bibliographische Detailangaben
Veröffentlicht in:	Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 40 vom: 26. Okt., Seite e2303730
1. Verfasser:	Wu, Jian-Fang (VerfasserIn)
Weitere Verfasser:	Zou, Zheyi, Pu, Bowei, Ladenstein, Lukas, Lin, Shen, Xie, Wenjing, Li, Shen, He, Bing, Fan, Yameng, Pang, Wei Kong, Wilkening, H Martin R, Guo, Xin, Xu, Chaohe, Zhang, Tao, Shi, Siqi, Liu, Jilei
Format:	Online-Aufsatz
Sprache:	English
Veröffentlicht:	2023
Zugriff auf das übergeordnete Werk:	Advanced materials (Deerfield Beach, Fla.)
Schlagworte:	Journal Article distorted polyhedra interfacial ionic transport liquid-like conduction oxide solid electrolytes

Beschreibung
Zusammenfassung:	© 2023 Wiley-VCH GmbH. The softness of sulfur sublattice and rotational PS4 tetrahedra in thiophosphates result in liquid-like ionic conduction, leading to enhanced ionic conductivities and stable electrode/thiophosphate interfacial ionic transport. However, the existence of liquid-like ionic conduction in rigid oxides remains unclear, and modifications are deemed necessary to achieve stable Li/oxide solid electrolyte interfacial charge transport. In this study, by combining the neutron diffraction survey, geometrical analysis, bond valence site energy analysis, and ab initio molecular dynamics simulation, 1D liquid-like Li-ion conduction is discovered in LiTa2 PO8 and its derivatives, wherein Li-ion migration channels are connected by four- or five-fold oxygen-coordinated interstitial sites. This conduction features a low activation energy (0.2 eV) and short mean residence time (<1 ps) of Li ions on the interstitial sites, originating from the Li-O polyhedral distortion and Li-ion correlation, which are controlled by doping strategies. The liquid-like conduction enables a high ionic conductivity (1.2 mS cm-1 at 30 °C), and a 700 h anomalously stable cycling under 0.2 mA cm-2 for Li/LiTa2 PO8 /Li cells without interfacial modifications. These findings provide principles for the future discovery and design of improved solid electrolytes that do not require modifications to the Li/solid electrolyte interface to achieve stable ionic transport
Beschreibung:	Date Revised 20.10.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE
ISSN:	1521-4095
DOI:	10.1002/adma.202303730