Elucidating the mobility of H+ and Li+ ions in (Li6.25-: XHxAl0.25)La3Zr2O12 via correlative neutron and electron spectroscopy

Xiaoming Liu, Yan Chen, Zachary D. Hood, Cheng Ma, Seungho Yu, Asma Sharafi, Hui Wang, Ke An, Jeff Sakamoto, Donald J. Siegel, Yongqiang Cheng, Niina H. Jalarvo, Miaofang Chi

Research output: Contribution to journalArticlepeer-review

56 Scopus citations

Abstract

A major challenge toward realizing high-performance aqueous lithium batteries (ALBs) is the utilization of a metallic lithium anode. However, an ideal solid electrolyte that can protect metallic lithium from reacting with aqueous solutions while still maintaining a high lithium ion conduction is not currently available. One obstacle is the lack of a reliable experimental tool to differentiate the conduction behaviour of H+ and Li+ ions in a solid electrolyte. Here, by correlating neutron and electron spectroscopy, we quantitatively reveal the mobility and lattice occupancy of the two ions individually in protonated cubic Li6.25Al0.25La3Zr2O12 (LLZO). Our results not only highlight LLZO as a potential effective separation layer for ALBs but also present a robust method to quantify the mobility of individual mobile ions in solid-state ion conductors.

Original languageEnglish
Pages (from-to)945-951
Number of pages7
JournalEnergy and Environmental Science
Volume12
Issue number3
DOIs
StatePublished - Mar 2019

Funding

Research sponsored by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division (X. L., M. C.). Research conducted at ORNL’s Center for Nanophase Materials Sciences (CNMS) (C. M., M. C.) and the Spallation Neutron Source (SNS) (Y. C., K. A., N. H. J., Y. C.), both of which are U.S. DOE Office of Science User Facilities. H. W. thanks the support by the EVPRI Internal Grant and Conn Center for Renewable Energy Res. at U. Louisville. Z. D. H. acknowledges support from the NSF Graduate Research Fellowship (DGE-1650044). J. S., S. S., and D. S. thanks the support by the U.S. DOE, Office of Energy Efficiency and Renewable Energy (Award DE-EE00006821). S. Y. thanks support by the Kwanjeong Educational Foundation. Research sponsored by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division (X. L., M. C.). Research conducted at ORNL's Center for Nanophase Materials Sciences (CNMS) (C. M., M. C.) and the Spallation Neutron Source (SNS) (Y. C., K. A., N. H. J., Y. C.), both of which are U.S. DOE Office of Science User Facilities. H. W. thanks the support by the EVPRI Internal Grant and Conn Center for Renewable Energy Res. at U. Louisville. Z. D. H. acknowledges support from the NSF Graduate Research Fellowship (DGE-1650044). J. S., S. S., and D. S. thanks the support by the U.S. DOE, Office of Energy Efficiency and Renewable Energy (Award DE-EE00006821). S. Y. thanks support by the Kwanjeong Educational Foundation.

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