Mechanochemical Synthesis: A Tool to Tune Cation Site Disorder and Ionic Transport Properties of Li3MCl6(M = Y, Er) Superionic Conductors
The lithium-conducting, rare-earth halides, Li₃MX₆ (M = Y, Er; X = Cl, Br), have garnered significantly rising interest recently, as they have been reported to have oxidative stability and high ionic conductivities. However, while a multitude of materials exhibit a superionic conductivity close to 1...
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| Format: | Article |
| Language: | English |
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Wiley
2020
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| Online Access: | https://hdl.handle.net/1721.1/128746 |
| _version_ | 1811090941733240832 |
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| author | Schlem, Roman Muy, Sokseiha Prinz, Nils Banik, Ananya Shao-Horn, Yang Zobel, Mirijam Zeier, Wolfgang G. |
| author2 | Massachusetts Institute of Technology. Department of Materials Science and Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Materials Science and Engineering Schlem, Roman Muy, Sokseiha Prinz, Nils Banik, Ananya Shao-Horn, Yang Zobel, Mirijam Zeier, Wolfgang G. |
| author_sort | Schlem, Roman |
| collection | MIT |
| description | The lithium-conducting, rare-earth halides, Li₃MX₆ (M = Y, Er; X = Cl, Br), have garnered significantly rising interest recently, as they have been reported to have oxidative stability and high ionic conductivities. However, while a multitude of materials exhibit a superionic conductivity close to 1 mS cm⁻¹, the exact design strategies to further improve the ionic transport properties have not been established yet. Here, the influence of the employed synthesis method of mechanochemical milling, compared to subsequent crystallization routines as well as classic solid-state syntheses on the structure and resulting transport behavior of Li₃ErCl₆ and Li₃YCl₆ are explored. Using a combination of X-ray diffraction, pair distribution function analysis, density functional theory, and impedance spectroscopy, insights into the average and local structural features that influence the underlying transport are provided. The existence of a cation defect within the structure in which Er/Y are disordered to a new position strongly benefits the transport properties. A synthetically tuned, increasing degree of this disordering leads to a decreasing activation energy and increasing ionic conductivity. This work sheds light on the possible synthesis strategies and helps to systematically understand and further improve the properties of this class of materials. |
| first_indexed | 2024-09-23T14:54:22Z |
| format | Article |
| id | mit-1721.1/128746 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T14:54:22Z |
| publishDate | 2020 |
| publisher | Wiley |
| record_format | dspace |
| spelling | mit-1721.1/1287462022-10-01T23:17:10Z Mechanochemical Synthesis: A Tool to Tune Cation Site Disorder and Ionic Transport Properties of Li3MCl6(M = Y, Er) Superionic Conductors Schlem, Roman Muy, Sokseiha Prinz, Nils Banik, Ananya Shao-Horn, Yang Zobel, Mirijam Zeier, Wolfgang G. Massachusetts Institute of Technology. Department of Materials Science and Engineering Massachusetts Institute of Technology. Research Laboratory of Electronics The lithium-conducting, rare-earth halides, Li₃MX₆ (M = Y, Er; X = Cl, Br), have garnered significantly rising interest recently, as they have been reported to have oxidative stability and high ionic conductivities. However, while a multitude of materials exhibit a superionic conductivity close to 1 mS cm⁻¹, the exact design strategies to further improve the ionic transport properties have not been established yet. Here, the influence of the employed synthesis method of mechanochemical milling, compared to subsequent crystallization routines as well as classic solid-state syntheses on the structure and resulting transport behavior of Li₃ErCl₆ and Li₃YCl₆ are explored. Using a combination of X-ray diffraction, pair distribution function analysis, density functional theory, and impedance spectroscopy, insights into the average and local structural features that influence the underlying transport are provided. The existence of a cation defect within the structure in which Er/Y are disordered to a new position strongly benefits the transport properties. A synthetically tuned, increasing degree of this disordering leads to a decreasing activation energy and increasing ionic conductivity. This work sheds light on the possible synthesis strategies and helps to systematically understand and further improve the properties of this class of materials. 2020-12-08T22:28:12Z 2020-12-08T22:28:12Z 2020-02 2019-12 2020-08-07T13:34:05Z Article http://purl.org/eprint/type/JournalArticle 1614-6832 1614-6840 https://hdl.handle.net/1721.1/128746 Schlem, Roman et al. "Mechanochemical Synthesis: A Tool to Tune Cation Site Disorder and Ionic Transport Properties of Li3MCl6(M = Y, Er) Superionic Conductors." Advanced Energy Materials 10, 6 (February 2020): 1903719 © 2019 The Authors en http://dx.doi.org/10.1002/aenm.201903719 Advanced Energy Materials Creative Commons Attribution 4.0 International license https://creativecommons.org/licenses/by/4.0/ application/pdf Wiley Wiley |
| spellingShingle | Schlem, Roman Muy, Sokseiha Prinz, Nils Banik, Ananya Shao-Horn, Yang Zobel, Mirijam Zeier, Wolfgang G. Mechanochemical Synthesis: A Tool to Tune Cation Site Disorder and Ionic Transport Properties of Li3MCl6(M = Y, Er) Superionic Conductors |
| title | Mechanochemical Synthesis: A Tool to Tune Cation Site Disorder and Ionic Transport Properties of Li3MCl6(M = Y, Er) Superionic Conductors |
| title_full | Mechanochemical Synthesis: A Tool to Tune Cation Site Disorder and Ionic Transport Properties of Li3MCl6(M = Y, Er) Superionic Conductors |
| title_fullStr | Mechanochemical Synthesis: A Tool to Tune Cation Site Disorder and Ionic Transport Properties of Li3MCl6(M = Y, Er) Superionic Conductors |
| title_full_unstemmed | Mechanochemical Synthesis: A Tool to Tune Cation Site Disorder and Ionic Transport Properties of Li3MCl6(M = Y, Er) Superionic Conductors |
| title_short | Mechanochemical Synthesis: A Tool to Tune Cation Site Disorder and Ionic Transport Properties of Li3MCl6(M = Y, Er) Superionic Conductors |
| title_sort | mechanochemical synthesis a tool to tune cation site disorder and ionic transport properties of li3mcl6 m y er superionic conductors |
| url | https://hdl.handle.net/1721.1/128746 |
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