Electrochemical transport and interfacial Chemistry of MoO ₂ –ordered mesoporous carbon nanocomposites for lithium-ion batteries

The development of high-performance electrode materials depends critically on interfacial interactions and adhesion phenomena at the nanoscale. In this study, molybdenum dioxide – ordered mesoporous carbon (MoO2–OMC) nanocomposites were investigated through validated multiphysics simulations to elucidate the coupled effects of ion transport, interfacial electrochemistry, and structural stability. The ordered mesoporous carbon framework, with uniform ~4.5 nm channels and high surface area, anchors MoO2 nanoparticles via oxygen-containing functional groups (e.g. hydroxyl, carbonyl), forming weak chemical bonds that prevent aggregation and improve interfacial adhesion by reducing nanoparticle mobility. This anchoring promotes stable solid electrolyte interphase (SEI) formation through preferential adsorption of electrolyte decomposition products, resulting in improved lithium-ion accessibility (via 4.5 nm pores) and charge transfer kinetics (e.g. reducing resistance to 50–108 Ω.cm2 as per EIS simulations. By systematically varying electrode thickness (10–150 µm) and MoO2:OMC mass ratios (20:80 to 80:20), the study identifies the 50:50 composition as optimal, delivering superior reversible capacity, low charge transfer resistance, and long-term cycling durability. The novelty of this work lies in integrating pore-scale transport dynamics (modeled via Navier – Stokes and Nernst – Planck equations) with surface chemistry and interfacial adhesion mechanisms, offering a framework for designing nanostructured composites with optimized electrochemical performance (e.g. 95.5% capacity retention at 50:50 ratio) and mechanical integrity. These insights extend beyond energy storage applications, demonstrating the role of interfacial engineering in advanced nanomaterials through a reduced charge transfer resistance (50–108 Ω.cm2).