Li15P4S16Cl3, a Lithium Chlorothiophosphate as a Solid-State Ionic Conductor

Zhantao Liu, Tatiana Zinkevich, Sylvio Indris, Xingfeng He, Jue Liu, Wenqian Xu, Jianming Bai, Shan Xiong, Yifei Mo, Hailong Chen

Research output: Contribution to journalArticlepeer-review

13 Scopus citations

Abstract

Tremendous efforts have been devoted to the design of solid Li+ electrolytes and the development of all-solid-state batteries. Compared with conventional Li-ion batteries, which use flammable liquid organic electrolytes, all-solid-state batteries show significant advantages in safety. In this work, a novel lithium chlorothiophosphate compound, Li15P4S16Cl3, is discovered. The crystal structure and electrochemical properties are investigated. Li15P4S16Cl3 can be synthesized as a pure phase via a facile solid-state reaction by heating a ball-milled mixture of Li2S, P2S5, and LiCl at 360 °C. The crystal structure of Li15P4S16Cl3 was refined against neutron and synchrotron powder X-ray diffraction data, revealing that it crystallizes in the space group I4̄ 3d. The Li+ transport in Li15P4S16Cl3 was also investigated by multiple solid-state NMR methods, including variableerature NMR line-shape analysis, NMR relaxometry, and pulsed-field-gradient NMR. Li15P4S16Cl3 shows good thermodynamic stability and can be synthesized at relatively low temperature. Although it exhibits a low ionic conductivity at room temperature, it can serve as a new motif crystal structure for the design and development of new solid-state electrolytes.

Original languageEnglish
Pages (from-to)226-234
Number of pages9
JournalInorganic Chemistry
Volume59
Issue number1
DOIs
StatePublished - Jan 6 2020

Funding

X.H. and Y.M. acknowledge support from the National Science Foundation under Award 1550423, the computational facilities from the University of Maryland supercomputing resources, the Maryland Advanced Research Computing Center, and the Extreme Science and Engineering Discovery Environment supported by the National Science Foundation under Award DMR150038. Z.L. and H.C. acknowledge financial support by the U.S. National Science Foundation under Grant CBET-1706723 and a new faculty startup fund of Georgia Institute of Technology. This research used resources of the Advanced Photon Source and National Synchrotron Light Source II, U.S. Department of Energy (DOE) Office of Science User Facilities operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357 and by Brookhaven National Laboratory under Contract No. DE-SC0012704.

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