Li0.625Al0.125H0.25Cl0.75O0.25Superionic Conductor with Disordered Rock-Salt Structure

Qian Zhang; William Arnold; Zachary D. Hood; Yang Li; Rachel Dewees; Miaofang Chi; Zhiwen Chen; Yan Chen; Hui Wang

doi:10.1021/acsaem.1c01011

Li_0.625Al_0.125H_0.25Cl_0.75O_0.25Superionic Conductor with Disordered Rock-Salt Structure

Qian Zhang, William Arnold, Zachary D. Hood, Yang Li, Rachel Dewees, Miaofang Chi, Zhiwen Chen, Yan Chen, Hui Wang

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

Solid-state Li-ion conductors are of broad interest in electrochemical energy storage, especially in solid-state Li batteries that serve as a promising alternative for the next-generation safe and high-energy-density batteries. Exploring solid-state superionic conductors is significant for the development of solid-state Li batteries with high performance. Herein, we report a disordered rock-salt (A1B1)-structured solid electrolyte (Li0.625Al0.125H0.25)(Cl0.75O0.25) (abbr. LAHCO) that was synthesized using Li2OHCl and LiAlCl4 as precursors. Neutron diffraction reveals that Li, Al, and H atoms occupy the A sites and O and Cl atoms occupy the B sites in the A1B1 structure for pure LAHCO. The LAHCO compound with excess LiAlCl4 shows the highest Li+ ionic conductivity of â 10-4 S cm-1 at room temperature due to the disordering induced by configurational entropy as well as the entropy of mixing. Moreover, LAHCO-LiAlCl4 solid electrolyte exhibits a stable polarization voltage under a current density of 5-50 μA cm-2 in Li symmetric cells. This work not only explicates the importance of Li-ion conductors with a rock-salt structure but also contributes toward the development of solid-state Li-ion conductors for broad applications.

Original language	English
Pages (from-to)	7674-7680
Number of pages	7
Journal	ACS Applied Energy Materials
Volume	4
Issue number	8
DOIs	https://doi.org/10.1021/acsaem.1c01011
State	Published - Aug 23 2021

Funding

The authors thank the support from the Conn Center for Renewable Energy Research and EVPRI Internal Grant of University of Louisville. The neutron diffraction work used resources at the Spallation Neutron Source (SNS), a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory (ORNL). M.C. is supported by the Center for Nanophase Materials Sciences (CNMS) at ORNL, and the user facility in CNMS at ORNL is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. Z.D.H. thanks the Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy under Contract No. DE-AC02-06CH11357.

Keywords

Li metal
disordered
ionic conductivity
rock-salt structure
solid electrolyte

Access to Document

10.1021/acsaem.1c01011

Cite this

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title = "Li0.625Al0.125H0.25Cl0.75O0.25Superionic Conductor with Disordered Rock-Salt Structure",

abstract = "Solid-state Li-ion conductors are of broad interest in electrochemical energy storage, especially in solid-state Li batteries that serve as a promising alternative for the next-generation safe and high-energy-density batteries. Exploring solid-state superionic conductors is significant for the development of solid-state Li batteries with high performance. Herein, we report a disordered rock-salt (A1B1)-structured solid electrolyte (Li0.625Al0.125H0.25)(Cl0.75O0.25) (abbr. LAHCO) that was synthesized using Li2OHCl and LiAlCl4 as precursors. Neutron diffraction reveals that Li, Al, and H atoms occupy the A sites and O and Cl atoms occupy the B sites in the A1B1 structure for pure LAHCO. The LAHCO compound with excess LiAlCl4 shows the highest Li+ ionic conductivity of {\^a} 10-4 S cm-1 at room temperature due to the disordering induced by configurational entropy as well as the entropy of mixing. Moreover, LAHCO-LiAlCl4 solid electrolyte exhibits a stable polarization voltage under a current density of 5-50 μA cm-2 in Li symmetric cells. This work not only explicates the importance of Li-ion conductors with a rock-salt structure but also contributes toward the development of solid-state Li-ion conductors for broad applications.",

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author = "Qian Zhang and William Arnold and Hood, {Zachary D.} and Yang Li and Rachel Dewees and Miaofang Chi and Zhiwen Chen and Yan Chen and Hui Wang",

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AU - Zhang, Qian

AU - Arnold, William

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AU - Li, Yang

AU - Dewees, Rachel

AU - Chi, Miaofang

AU - Chen, Zhiwen

AU - Chen, Yan

AU - Wang, Hui

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