Computational discovery of Mg-based garnet structures with enhanced battery performance

In the burgeoning landscape of power source technologies, Mg-ion batteries have emerged as a promising alternative to the widely used Li-ion batteries due to the large natural abundance and divalence of magnesium. As an attempt to develop working Mg-ion batteries, for which securing efficient cathod...

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Main Authors: Sanghyun Kim, Joo-Hyoung Lee
Format: Article
Language:English
Published: Elsevier 2025-08-01
Series:Materials Today Advances
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Online Access:http://www.sciencedirect.com/science/article/pii/S2590049825000487
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author Sanghyun Kim
Joo-Hyoung Lee
author_facet Sanghyun Kim
Joo-Hyoung Lee
author_sort Sanghyun Kim
collection DOAJ
description In the burgeoning landscape of power source technologies, Mg-ion batteries have emerged as a promising alternative to the widely used Li-ion batteries due to the large natural abundance and divalence of magnesium. As an attempt to develop working Mg-ion batteries, for which securing efficient cathode materials with high energy density and ion mobility is crucial, we carry out electronic structure calculations based on density functional theory (DFT) to uncover high-performance garnet-type cathode materials, Mg3V1.5Cr3.5O12 (MVCO) and Mg3V3Mn2O12 (MVMO), for efficient Mg-ion batteries. Our DFT calculations demonstrate that MVCO (MVMO) not only achieves a high average voltage of 2.79V (2.69V) and energy density of 856 Wh/kg (821 Wh/kg) but also presents small volume change of 4.5 % (4 %) and low ion migration barrier of 395 meV (190 meV). It is further found out that although oxygen atoms participate in the redox reaction during the (de)intercalation process, the strong orbital hybridization between oxygen and transition metal elements prevents forming (O-O)n− dimers and thus oxygen release is likely to be suppressed, ensuring structural stability. Combined with high likelihood of successful synthesizability as is evidenced through comparison with the amorphous limits, these materials properties make the proposed garnet-structured magnesium compounds appealing candidates for post-Li energy storage solutions.
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spelling doaj-art-4f70a91d73fe4c4bbb8cab02043dd1122025-08-20T04:00:45ZengElsevierMaterials Today Advances2590-04982025-08-012710060310.1016/j.mtadv.2025.100603Computational discovery of Mg-based garnet structures with enhanced battery performanceSanghyun Kim0Joo-Hyoung Lee1Department of Materials Science and Engineering, Gwangju Institute of Science and Technology (GIST), Buk-gu, Gwangju, 61005, South KoreaCorresponding author.; Department of Materials Science and Engineering, Gwangju Institute of Science and Technology (GIST), Buk-gu, Gwangju, 61005, South KoreaIn the burgeoning landscape of power source technologies, Mg-ion batteries have emerged as a promising alternative to the widely used Li-ion batteries due to the large natural abundance and divalence of magnesium. As an attempt to develop working Mg-ion batteries, for which securing efficient cathode materials with high energy density and ion mobility is crucial, we carry out electronic structure calculations based on density functional theory (DFT) to uncover high-performance garnet-type cathode materials, Mg3V1.5Cr3.5O12 (MVCO) and Mg3V3Mn2O12 (MVMO), for efficient Mg-ion batteries. Our DFT calculations demonstrate that MVCO (MVMO) not only achieves a high average voltage of 2.79V (2.69V) and energy density of 856 Wh/kg (821 Wh/kg) but also presents small volume change of 4.5 % (4 %) and low ion migration barrier of 395 meV (190 meV). It is further found out that although oxygen atoms participate in the redox reaction during the (de)intercalation process, the strong orbital hybridization between oxygen and transition metal elements prevents forming (O-O)n− dimers and thus oxygen release is likely to be suppressed, ensuring structural stability. Combined with high likelihood of successful synthesizability as is evidenced through comparison with the amorphous limits, these materials properties make the proposed garnet-structured magnesium compounds appealing candidates for post-Li energy storage solutions.http://www.sciencedirect.com/science/article/pii/S2590049825000487Multivalent cathode active materialMg-ion batteryDensity functional theoryHigh performance electrode
spellingShingle Sanghyun Kim
Joo-Hyoung Lee
Computational discovery of Mg-based garnet structures with enhanced battery performance
Materials Today Advances
Multivalent cathode active material
Mg-ion battery
Density functional theory
High performance electrode
title Computational discovery of Mg-based garnet structures with enhanced battery performance
title_full Computational discovery of Mg-based garnet structures with enhanced battery performance
title_fullStr Computational discovery of Mg-based garnet structures with enhanced battery performance
title_full_unstemmed Computational discovery of Mg-based garnet structures with enhanced battery performance
title_short Computational discovery of Mg-based garnet structures with enhanced battery performance
title_sort computational discovery of mg based garnet structures with enhanced battery performance
topic Multivalent cathode active material
Mg-ion battery
Density functional theory
High performance electrode
url http://www.sciencedirect.com/science/article/pii/S2590049825000487
work_keys_str_mv AT sanghyunkim computationaldiscoveryofmgbasedgarnetstructureswithenhancedbatteryperformance
AT joohyounglee computationaldiscoveryofmgbasedgarnetstructureswithenhancedbatteryperformance