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Engineering Solution-Processed Non-Crystalline Solid Electrolytes for Li Metal Batteries

[Image: see text] Non-crystalline Li-ion solid electrolytes (SEs), such as lithium phosphorus oxynitride, can uniquely enable high-rate solid-state battery operation over thousands of cycles in thin film form. However, they are typically produced by expensive and low throughput vacuum deposition, li...

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Autores principales: Vadhva, Pooja, Gill, Thomas E., Cruddos, Joshua H., Said, Samia, Siniscalchi, Marco, Narayanan, Sudarshan, Pasta, Mauro, Miller, Thomas S., Rettie, Alexander J. E.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9933431/
https://www.ncbi.nlm.nih.gov/pubmed/36818586
http://dx.doi.org/10.1021/acs.chemmater.2c03071
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author Vadhva, Pooja
Gill, Thomas E.
Cruddos, Joshua H.
Said, Samia
Siniscalchi, Marco
Narayanan, Sudarshan
Pasta, Mauro
Miller, Thomas S.
Rettie, Alexander J. E.
author_facet Vadhva, Pooja
Gill, Thomas E.
Cruddos, Joshua H.
Said, Samia
Siniscalchi, Marco
Narayanan, Sudarshan
Pasta, Mauro
Miller, Thomas S.
Rettie, Alexander J. E.
author_sort Vadhva, Pooja
collection PubMed
description [Image: see text] Non-crystalline Li-ion solid electrolytes (SEs), such as lithium phosphorus oxynitride, can uniquely enable high-rate solid-state battery operation over thousands of cycles in thin film form. However, they are typically produced by expensive and low throughput vacuum deposition, limiting their wide application and study. Here, we report non-crystalline SEs of composition Li–Al–P–O (LAPO) with ionic conductivities > 10(–7) S cm(–1) at room temperature made by spin coating from aqueous solutions and subsequent annealing in air. Homogenous, dense, flat layers can be synthesized with submicrometer thickness at temperatures as low as 230 °C. Control of the composition is shown to significantly affect the ionic conductivity, with increased Li and decreased P content being optimal, while higher annealing temperatures result in decreased ionic conductivity. Activation energy analysis reveals a Li-ion hopping barrier of ≈0.4 eV. Additionally, these SEs exhibit low room temperature electronic conductivity (< 10(–11) S cm(–1)) and a moderate Young’s modulus of ≈54 GPa, which may be beneficial in preventing Li dendrite formation. In contact with Li metal, LAPO is found to form a stable but high impedance passivation layer comprised of Al metal, Li–P, and Li–O species. These findings should be of value when engineering non-crystalline SEs for Li-metal batteries with high energy and power densities.
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spelling pubmed-99334312023-02-17 Engineering Solution-Processed Non-Crystalline Solid Electrolytes for Li Metal Batteries Vadhva, Pooja Gill, Thomas E. Cruddos, Joshua H. Said, Samia Siniscalchi, Marco Narayanan, Sudarshan Pasta, Mauro Miller, Thomas S. Rettie, Alexander J. E. Chem Mater [Image: see text] Non-crystalline Li-ion solid electrolytes (SEs), such as lithium phosphorus oxynitride, can uniquely enable high-rate solid-state battery operation over thousands of cycles in thin film form. However, they are typically produced by expensive and low throughput vacuum deposition, limiting their wide application and study. Here, we report non-crystalline SEs of composition Li–Al–P–O (LAPO) with ionic conductivities > 10(–7) S cm(–1) at room temperature made by spin coating from aqueous solutions and subsequent annealing in air. Homogenous, dense, flat layers can be synthesized with submicrometer thickness at temperatures as low as 230 °C. Control of the composition is shown to significantly affect the ionic conductivity, with increased Li and decreased P content being optimal, while higher annealing temperatures result in decreased ionic conductivity. Activation energy analysis reveals a Li-ion hopping barrier of ≈0.4 eV. Additionally, these SEs exhibit low room temperature electronic conductivity (< 10(–11) S cm(–1)) and a moderate Young’s modulus of ≈54 GPa, which may be beneficial in preventing Li dendrite formation. In contact with Li metal, LAPO is found to form a stable but high impedance passivation layer comprised of Al metal, Li–P, and Li–O species. These findings should be of value when engineering non-crystalline SEs for Li-metal batteries with high energy and power densities. American Chemical Society 2023-01-18 /pmc/articles/PMC9933431/ /pubmed/36818586 http://dx.doi.org/10.1021/acs.chemmater.2c03071 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Vadhva, Pooja
Gill, Thomas E.
Cruddos, Joshua H.
Said, Samia
Siniscalchi, Marco
Narayanan, Sudarshan
Pasta, Mauro
Miller, Thomas S.
Rettie, Alexander J. E.
Engineering Solution-Processed Non-Crystalline Solid Electrolytes for Li Metal Batteries
title Engineering Solution-Processed Non-Crystalline Solid Electrolytes for Li Metal Batteries
title_full Engineering Solution-Processed Non-Crystalline Solid Electrolytes for Li Metal Batteries
title_fullStr Engineering Solution-Processed Non-Crystalline Solid Electrolytes for Li Metal Batteries
title_full_unstemmed Engineering Solution-Processed Non-Crystalline Solid Electrolytes for Li Metal Batteries
title_short Engineering Solution-Processed Non-Crystalline Solid Electrolytes for Li Metal Batteries
title_sort engineering solution-processed non-crystalline solid electrolytes for li metal batteries
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9933431/
https://www.ncbi.nlm.nih.gov/pubmed/36818586
http://dx.doi.org/10.1021/acs.chemmater.2c03071
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