Unveiling the dominant role of rGO in tailored PVA@TiO2–metal oxide nanostructures for high-performance aerospace Lithium-ion batteries

Meeting the escalating global demand for high-performance materials in next-generation energy storage and flexible electronics necessitates the development of multifunctional nanocomposites with tailored physicochemical properties. In this study, we design and investigate novel polymer-based nanocomposites comprising polyvinyl alcohol and titanium dioxide (PVA@TiO2, denoted as PT) further functionalized with magnesium oxide (MgO), silicon dioxide (SiO2), or reduced graphene oxide (rGO) to form PVA@TiO2@MgO (PTM), PVA@TiO2@ SiO2 (PTS) and PVA@TiO2@rGO (PTG), respectively. The composites were engineered to improve electrical conductivity, structural porosity, and interfacial interaction—key features for energy-related applications. Morphological and EDX analyses confirmed the formation of a homogeneously distributed nanoporous architecture with an average pore size of approximately 0.27 μm. Experimentally, PTG exhibited superior electrical conductivity (0.59 S/m) compared to PT (0.36 S/m), as well as increased apparent porosity (70 %) and surface roughness (6.8 μm), highlighting its potential for ion transport and charge storage. To complement the experimental findings, we conducted a theoretical investigation using DFT:B3LYP/6-31 g (d, p) to simulate the interactions between PVA chains and various carbon derivatives. Significant enhancements were observed in the PTG–2
system compared to PT–2
, including a decrease in total dipole moment (from 4.1454 to 2.7966 Debye), a reduced HOMO–LUMO bandgap (from 1.1616 to 0.5241 eV), and a more favorable total energy profile. Moreover, PTG–2
exhibited the most reactive and stable configuration, with a high binding energy of 7.3419 kcal/mol, attributed to abundant active sites on rGO (–COOH, Cdouble bondO, OH, and C–O–C) and their strategic spatial arrangement, which facilitates lithium-ion coordination and transport. Significantly, this work establishes for the first time that rGO is not merely a conductive additive but the decisive structural and electronic modifier within PVA@TiO2 frameworks—governing electron mobility, interfacial stability, and structural uniformity. This dual experimental–theoretical validation highlights rGO's dominant role in advancing lightweight, thermally stable, and high-performance lithium-ion batteries, thereby offering a new paradigm for aerospace-grade energy storage systems.