Issue 12, 2024

First-principles evaluation of MnO2 polymorphs as cathode material in lithium-ion batteries

Abstract

Polymorphic materials, e.g. manganese dioxide (MnO2) exhibit promise in energy storage applications, such as serving as cathode material for Li-ion batteries (LIBs). The flexibility to arrange the polyhedral building blocks within their lattice structures allows tunable properties for enhanced performance. In this work, we carried out first-principles simulations to scrutinize the structural, thermodynamic and kinetic properties of polymorphic MnO2 during Li-ion intercalation. We explored polymorph-specific metrics in dictating its overall performance as cathode material in LIBs, such as thermal and mechanical stability during reversible Li-ion intercalation, achievable energy density, volumetric storage capacity, and Li-ion mobility. Our comprehensive analyses reveal that there are inherent trade-offs among the evaluated properties for optimal performance. For instance, tunneled polymorphs such as α and β phases of MnO2 allow fast Li-ion diffusion, yet suffer from limited capacity and strain-induced structural vulnerabilities. On the other hand, the spinel (λ) phase of MnO2 offers a higher voltage window but shows significantly more sluggish Li-ion transport behavior. Overall, the findings and insights presented in this study will provide practical guidelines for materials selection and structural engineering of MnO2 polymorphs for advanced battery applications.

Graphical abstract: First-principles evaluation of MnO2 polymorphs as cathode material in lithium-ion batteries

Supplementary files

Article information

Article type
Paper
Submitted
26 2 2024
Accepted
16 5 2024
First published
17 5 2024
This article is Open Access
Creative Commons BY license

Sustainable Energy Fuels, 2024,8, 2718-2729

First-principles evaluation of MnO2 polymorphs as cathode material in lithium-ion batteries

W. Sun, C. A. Orme, M. A. Worsley and L. F. Wan, Sustainable Energy Fuels, 2024, 8, 2718 DOI: 10.1039/D4SE00279B

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