journal article·2023-10Open access

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

Jian‐Fang Wu, Zheyi Zou, Bowei Pu, Lukas Ladenstein, Shen Lin, Wenjing Xie, Shen Li, Bing He, Yameng Fan, Wei Kong Pang, H. Martin R. Wilkening, Xin Guo, Chaohe Xu, Tao Zhang, Siqi Shi, Jilei Liu

Advanced Materials· Volume 35· Issue 40

Abstract

Abstract 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 LiTa2PO8 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/LiTa2PO8/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.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced Battery Technologies Research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

College of Materials Science and Engineering Hunan Joint International Laboratory of Advanced Materials and Technology of Clean Energy Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology Hunan University Changsha 410082 P. R. China

School of Materials Science and Engineering Xiangtan University Xiangtan 411105 P. R. China

School of Materials Science and Engineering Materials Genome Institute Shanghai University Shanghai 200444 P. R. China

Institute of Chemistry and Technology of Materials Christian Doppler Laboratory for Lithium Batteries Graz University of Technology (NAWI Graz) Graz 8010 Austria

Institute for Superconducting & Electronic Materials University of Wollongong Wollongong New South Wales 2522 Australia

State Key Laboratory of Material Processing and Die & Mould Technology Laboratory of Solid State Ionics School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 P. R. China

College of Aerospace Engineering Chongqing University Chongqing 400044 P. R. China

State Key Lab of High Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences 1295 Dingxi Road Shanghai 200050 P. R. China

Funding

National Key Research and Development Program of China · National Natural Science Foundation of China · Natural Science Foundation of Chongqing · State Key Laboratory of Materials Processing and Die and Mould Technology · Huazhong University of Science and Technology · Australian Nuclear Science and Technology Organisation

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