First-principles and quantum transport investigation of triclinic Mg11Ti25O60 as a high-voltage cathode material for magnesium-ion batteries
- 1Department of Physics, University of Gujrat Hafiz Hayat Campus Gujrat Pakistan [email protected] [email protected].
- 2Department of Physics, Gachon University 1342 Seongnam-daero, Sujeong-gu Seongnam-si Gyeonggi-do South Korea.
Abstract
Fabrication of functional intercalating cathode matrices is still a tough challenge for commercialization of rechargeable magnesium-ion batteries (MIBs). In general, the lattice stress and slow diffusion rate of Mg²⁺ ions are severe in conventional host materials. In order to tackle this multi-electron problem, a novel triclinic Mg₁₁Ti₂₅O₆₀ cathode framework is studied comprehensively using first principles calculations based on Density Functional Based Tight Binding (DFTB) and Non-Equilibrium Green's Function (NEGF) formalisms. Our atomistic simulations indicate that the extraction of magnesium is a highly coordinated, structural mechanism, where the magnesium is removed one at a time. In general, the divalent insertion strain is well accommodated by the structurally robust Ti-O framework, and the strong local coulombic interactions result in small thermodynamic fluctuations at discrete intermediate extraction steps, ensuring the long-term structural and volume stability. Electronically, the pristine material's performance is not restricted by the resistance barriers found with traditional oxide hosts, and shows metallic behavior. The material exhibits a theoretical specific capacity of 243.25 mA h g⁻¹, energy density of 819.75 W h kg⁻¹ and open circuit voltage (OCV) value of 3.37 V. The results obtained from NEGF-based quantum transport calculations show good energetic compatibility between the interface and the standard ethylene carbonate electrolytes. These results, coupled with the ab initio molecular dynamics (AIMD) demonstrate thermal stability at operating conditions and a reasonable migration barrier of 0.62 eV. The findings of this study predict Mg₁₁Ti₂₅O₆₀ as a promising high-voltage candidate for use in next-generation multivalent energy storage devices.
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BibTeX
@article{zahra2026firstprinciples,
title = {{First-principles and quantum transport investigation of triclinic Mg11Ti25O60 as a high-voltage cathode material for magnesium-ion batteries}},
author = {Syeda Eman Zahra and Amara Yousaf and Muhammad Tayyab Raza and Abdul Majid},
journal = {RSC advances},
year = {2026},
month = oct,
doi = {10.1039/d6ra06938j},
url = {https://europepmc.org/article/PMC/PMC13717622},
note = {CC BY},
}
RIS
TY - JOUR
TI - First-principles and quantum transport investigation of triclinic Mg11Ti25O60 as a high-voltage cathode material for magnesium-ion batteries
AU - Syeda Eman Zahra
AU - Amara Yousaf
AU - Muhammad Tayyab Raza
AU - Abdul Majid
PY - 2026
DA - 2026/10/29
JO - RSC advances
DO - 10.1039/d6ra06938j
UR - https://europepmc.org/article/PMC/PMC13717622
AB - Fabrication of functional intercalating cathode matrices is still a tough challenge for commercialization of rechargeable magnesium-ion batteries (MIBs). In general, the lattice stress and slow diffusion rate of Mg²⁺ ions are severe in conventional host materials. In order to tackle this multi-electron problem, a novel triclinic Mg₁₁Ti₂₅O₆₀ cathode framework is studied comprehensively using first principles calculations based on Density Functional Based Tight Binding (DFTB) and Non-Equilibrium Green's Function (NEGF) formalisms. Our atomistic simulations indicate that the extraction of magnesium is a highly coordinated, structural mechanism, where the magnesium is removed one at a time. In general, the divalent insertion strain is well accommodated by the structurally robust Ti-O framework, and the strong local coulombic interactions result in small thermodynamic fluctuations at discrete intermediate extraction steps, ensuring the long-term structural and volume stability. Electronically, the pristine material's performance is not restricted by the resistance barriers found with traditional oxide hosts, and shows metallic behavior. The material exhibits a theoretical specific capacity of 243.25 mA h g⁻¹, energy density of 819.75 W h kg⁻¹ and open circuit voltage (OCV) value of 3.37 V. The results obtained from NEGF-based quantum transport calculations show good energetic compatibility between the interface and the standard ethylene carbonate electrolytes. These results, coupled with the ab initio molecular dynamics (AIMD) demonstrate thermal stability at operating conditions and a reasonable migration barrier of 0.62 eV. The findings of this study predict Mg₁₁Ti₂₅O₆₀ as a promising high-voltage candidate for use in next-generation multivalent energy storage devices.
SN - 2046-2069
ER -