Data-driven design of electrolyte additives supporting high-performance 5 V LiNi0.5Mn1.5O4 positive electrodes

Abstract LiNi0.5Mn1.5O4 (LNMO) is a high-capacity spinel-structured material with an average lithiation/de-lithiation potential at ca. 4.6–4.7 V vs Li+/Li, far exceeding the stability limits of electrolytes. An efficient way to enable LNMO in lithium-ion batteries is to reformulate an electrolyte co...

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Main Authors: Bingning Wang, Hieu A. Doan, Seoung-Bum Son, Daniel P. Abraham, Stephen E. Trask, Andrew Jansen, Kang Xu, Chen Liao
Format: Article
Language:English
Published: Nature Portfolio 2025-04-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-57961-w
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author Bingning Wang
Hieu A. Doan
Seoung-Bum Son
Daniel P. Abraham
Stephen E. Trask
Andrew Jansen
Kang Xu
Chen Liao
author_facet Bingning Wang
Hieu A. Doan
Seoung-Bum Son
Daniel P. Abraham
Stephen E. Trask
Andrew Jansen
Kang Xu
Chen Liao
author_sort Bingning Wang
collection DOAJ
description Abstract LiNi0.5Mn1.5O4 (LNMO) is a high-capacity spinel-structured material with an average lithiation/de-lithiation potential at ca. 4.6–4.7 V vs Li+/Li, far exceeding the stability limits of electrolytes. An efficient way to enable LNMO in lithium-ion batteries is to reformulate an electrolyte composition that stabilizes both graphitic (Gr) negative electrode with solid-electrolyte-interphase and LNMO with cathode-electrolyte-interphase. In this study, we select and test a diverse collection of 28 single and dual additives for the Gr||LNMO battery system. Subsequently, we train machine learning models on this dataset and employ the trained models to suggest 6 binary compositions out of 125, based on predicted final area-specific-impedance, impedance rise, and final specific-capacity. Such machine learning-generated new additives outperform the initial dataset. This finding not only underscores the efficacy of machine learning in identifying materials in a highly complicated application space but also showcases an accelerated material discovery workflow that directly integrates data-driven methods with battery testing experiments.
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issn 2041-1723
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spelling doaj-art-3ea13c104604432c82a6eb48ddfcaf0c2025-08-20T03:06:52ZengNature PortfolioNature Communications2041-17232025-04-0116111010.1038/s41467-025-57961-wData-driven design of electrolyte additives supporting high-performance 5 V LiNi0.5Mn1.5O4 positive electrodesBingning Wang0Hieu A. Doan1Seoung-Bum Son2Daniel P. Abraham3Stephen E. Trask4Andrew Jansen5Kang Xu6Chen Liao7Chemical Sciences and Engineering Division, Argonne National LaboratoryMaterials Science Division, Argonne National LaboratoryChemical Sciences and Engineering Division, Argonne National LaboratoryChemical Sciences and Engineering Division, Argonne National LaboratoryChemical Sciences and Engineering Division, Argonne National LaboratoryChemical Sciences and Engineering Division, Argonne National LaboratorySES AI CorpsChemical Sciences and Engineering Division, Argonne National LaboratoryAbstract LiNi0.5Mn1.5O4 (LNMO) is a high-capacity spinel-structured material with an average lithiation/de-lithiation potential at ca. 4.6–4.7 V vs Li+/Li, far exceeding the stability limits of electrolytes. An efficient way to enable LNMO in lithium-ion batteries is to reformulate an electrolyte composition that stabilizes both graphitic (Gr) negative electrode with solid-electrolyte-interphase and LNMO with cathode-electrolyte-interphase. In this study, we select and test a diverse collection of 28 single and dual additives for the Gr||LNMO battery system. Subsequently, we train machine learning models on this dataset and employ the trained models to suggest 6 binary compositions out of 125, based on predicted final area-specific-impedance, impedance rise, and final specific-capacity. Such machine learning-generated new additives outperform the initial dataset. This finding not only underscores the efficacy of machine learning in identifying materials in a highly complicated application space but also showcases an accelerated material discovery workflow that directly integrates data-driven methods with battery testing experiments.https://doi.org/10.1038/s41467-025-57961-w
spellingShingle Bingning Wang
Hieu A. Doan
Seoung-Bum Son
Daniel P. Abraham
Stephen E. Trask
Andrew Jansen
Kang Xu
Chen Liao
Data-driven design of electrolyte additives supporting high-performance 5 V LiNi0.5Mn1.5O4 positive electrodes
Nature Communications
title Data-driven design of electrolyte additives supporting high-performance 5 V LiNi0.5Mn1.5O4 positive electrodes
title_full Data-driven design of electrolyte additives supporting high-performance 5 V LiNi0.5Mn1.5O4 positive electrodes
title_fullStr Data-driven design of electrolyte additives supporting high-performance 5 V LiNi0.5Mn1.5O4 positive electrodes
title_full_unstemmed Data-driven design of electrolyte additives supporting high-performance 5 V LiNi0.5Mn1.5O4 positive electrodes
title_short Data-driven design of electrolyte additives supporting high-performance 5 V LiNi0.5Mn1.5O4 positive electrodes
title_sort data driven design of electrolyte additives supporting high performance 5 v lini0 5mn1 5o4 positive electrodes
url https://doi.org/10.1038/s41467-025-57961-w
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