First principle investigation on properties of MnO2 as an electrode material for Li, Na, Mg, and Al -ion batteries

• Published in: Computational Condensed Matter 2024-03, Vol.38, p.e00886, Article e00886
• Main Authors: Hafizi, Mahziar, Hassani, Samin, Yousefi-Mashhour, Hatef, Kalantarian, Mohammad Mahdi, Javaheri, Masoumeh, Massoudi, Abouzar
• Format: Article
• Language: English
• Subjects: Cathode; Density functional theory; MnO2 oxide electrode; Rate-capability; Rechargeable intercalation battery
• ISSN: 2352-2143; 2352-2143
• DOI: 10.1016/j.cocom.2024.e00886

This study uses noble evaluations in Density Functional Theory (DFT) framework to investigate the structural, electrochemical, magnetic, and electrical properties of AMn2O4 (A = Li, Na, Mg, and Al) cathode materials for various metal-ion batteries. The calculations are performed by four DFT methods (GGA/+U, LSDA/+U). Considering volume change Both GGA and LSDA methods showed that NaMn2O4 had the highest and AlMn2O4 had the lowest volume reduction, caused by electronegativity of Al and the initial unit cell volume. The cell voltages were calculated with two different approaches called as internal and Fermi energy. It was concluded that the probable low cycle-ability of this family can be attributed to remarkable alteration of magnetic moment of manganese transition metal during extraction/insertion of intercalating ions. The electrical properties of AMn2O4 materials were investigated evaluating BGs and electrical rate-capability. For each material two kinds of band-gap (BG) and two criterions for rate-capability were considered, i.e. ILBG/ELBG, and Delta/CCTB, respectively. The BG evaluation showed that all the considered materials have appropriate conductivity. Both of the evaluated Delta and CCTB approaches predicted high rate-capability for the AMn2O4 materials. Our calculations demonstrated that MnO2 is a suitable and highly considerable cathode material for the Li and beyond-Li -ion batteries.