Tailoring of the Anti-Perovskite Solid Electrolytes at the Grain-Scale

Marm Dixit; Nitin Muralidharan; Anuj Bisht; Charl J. Jafta; Christopher T. Nelson; Ruhul Amin; Rachid Essehli; Mahalingam Balasubramanian; Ilias Belharouak

doi:10.1021/acsenergylett.3c00265

Tailoring of the Anti-Perovskite Solid Electrolytes at the Grain-Scale

Marm Dixit, Nitin Muralidharan, Anuj Bisht, Charl J. Jafta, Christopher T. Nelson, Ruhul Amin, Rachid Essehli, Mahalingam Balasubramanian, Ilias Belharouak

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13 Scopus citations

Abstract

The development of thin, dense, defect-free solid electrolyte films is key for achieving practical and commercially viable solid-state batteries. Herein, we showcase a facile processing pathway for antiperovskite (Li₂OHCl) solid electrolyte materials that can yield films/pellets with very high densities (∼100%) and higher conductivities compared with conventional uniaxially pressed pellets. We have also achieved close to 50% improvement in the critical current density of the material and an improved lithiophilicity due to the surface nitrogen enrichment of the processed pellets. Distribution of relaxation time analysis supports the contributions from “faster” transport mechanisms for the antiperovskite films/pellets developed using the new protocol. Overall, the results highlight the feasibility of our new processing pathway for engineering antiperovskite solid electrolytes at the grain scale as a highly desirable approach for practical all-solid-state batteries.

Original language	English
Pages (from-to)	2356-2364
Number of pages	9
Journal	ACS Energy Letters
Volume	8
Issue number	5
DOIs	https://doi.org/10.1021/acsenergylett.3c00265
State	Published - May 12 2023

Funding

This research at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under contract DE-AC05-00OR22725, was sponsored by the Laboratory Directed Research and Development (LDRD) Program at Oak Ridge National Laboratory and the Energy Efficiency and Renewable Energy (EERE) Vehicle Technologies Office (VTO). M.D. was also supported by the Alvin M. Weinberg Fellowship at the Oak Ridge National Laboratory. The TEM was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. This research also used resources of the Advanced Photon Source, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357. The authors would like to thank Pavel Shevchenko and Francesco de Carlo for their help with the tomography experiments.

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abstract = "The development of thin, dense, defect-free solid electrolyte films is key for achieving practical and commercially viable solid-state batteries. Herein, we showcase a facile processing pathway for antiperovskite (Li2OHCl) solid electrolyte materials that can yield films/pellets with very high densities (∼100\%) and higher conductivities compared with conventional uniaxially pressed pellets. We have also achieved close to 50\% improvement in the critical current density of the material and an improved lithiophilicity due to the surface nitrogen enrichment of the processed pellets. Distribution of relaxation time analysis supports the contributions from “faster” transport mechanisms for the antiperovskite films/pellets developed using the new protocol. Overall, the results highlight the feasibility of our new processing pathway for engineering antiperovskite solid electrolytes at the grain scale as a highly desirable approach for practical all-solid-state batteries.",

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AU - Jafta, Charl J.

AU - Nelson, Christopher T.

AU - Amin, Ruhul

AU - Essehli, Rachid

AU - Balasubramanian, Mahalingam

AU - Belharouak, Ilias

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AB - The development of thin, dense, defect-free solid electrolyte films is key for achieving practical and commercially viable solid-state batteries. Herein, we showcase a facile processing pathway for antiperovskite (Li2OHCl) solid electrolyte materials that can yield films/pellets with very high densities (∼100%) and higher conductivities compared with conventional uniaxially pressed pellets. We have also achieved close to 50% improvement in the critical current density of the material and an improved lithiophilicity due to the surface nitrogen enrichment of the processed pellets. Distribution of relaxation time analysis supports the contributions from “faster” transport mechanisms for the antiperovskite films/pellets developed using the new protocol. Overall, the results highlight the feasibility of our new processing pathway for engineering antiperovskite solid electrolytes at the grain scale as a highly desirable approach for practical all-solid-state batteries.

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Tailoring of the Anti-Perovskite Solid Electrolytes at the Grain-Scale

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