Elucidating the mobility of H+ and Li+ ions in (Li6.25−xHxAl0.25)La3Zr2O12via 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

doi:10.1039/C8EE02981D

Elucidating the mobility of H⁺ and Li⁺ ions in (Li_6.25−xH_xAl_0.25)La₃Zr₂O₁₂via correlative neutron and electron spectroscopy†‡

Xiaoming Liu,

§^a Yan Chen,

§^b Zachary D. Hood,

^ac Cheng Ma,^d Seungho Yu,

^e Asma Sharafi,^e Hui Wang,^f Ke An,

^b Jeff Sakamoto,^e Donald J. Siegel,

^eg Yongqiang Cheng,*^b Niina H. Jalarvo

*^bh and Miaofang Chi

*^a

Author affiliations

* Corresponding authors

^a Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
E-mail: chim@ornl.gov

^b Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
E-mail: jalarvonh@ornl.gov, chengy@ornl.gov

^c Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA

^d School of Chemistry and Materials Science, University of Science and Technology of China (USTC), Hefei, Anhui 230026, China

^e Mechanical Engineering, University of Michigan, Ann Arbor, MI 48109, USA

^f Mechanical Engineering, Conn Center for Renewable Energy Research, University of Louisville, Louisville, KY, USA

^g Department of Materials Science and Engineering, University of Michigan, Ann Arbor, MI 48109, USA

^h JCNS-1, Forschungszentrum Jülich, D-52425 Jülich, Germany

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 Li_6.25Al_0.25La₃Zr₂O₁₂ (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.

Energy & Environmental Science

Elucidating the mobility of H⁺ and Li⁺ ions in (Li_6.25−xH_xAl_0.25)La₃Zr₂O₁₂via correlative neutron and electron spectroscopy†‡

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Elucidating the mobility of H⁺ and Li⁺ ions in (Li_6.25−xH_xAl_0.25)La₃Zr₂O₁₂via correlative neutron and electron spectroscopy

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