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<p>This work presents a defect-engineered graphene–polymer–oxide hybrid electrode tailored for high-efficiency supercapacitors. The architecture integrates high-conductivity chemical vapor deposition (CVD) graphene and solution-processable reduced graphene oxide (rGO), both enhanced via multifunctional surface modifications including <i>π</i>–<i>π</i> conjugated polyaniline (PANI) wrapping, oxygen plasma treatment, and alkali metal intercalation. These modifications optimize charge carrier mobility, interfacial compatibility, and electronic conductivity. Experimental evaluations reveal a specific capacitance of 450 F/g, energy density of 85 Wh/kg, and power density of 70 kW/kg, with 92% retention after 10,000 cycles. To support design insights, density functional theory (DFT) and molecular dynamics (MD) simulations correlate defect density, Fermi level shifts, and charge transport pathways with electrochemical performance. The optimized hybrid system demonstrates superior electronic behavior while being compatible with roll-to-roll (R2R) electrode fabrication, enabling large-scale, cost-effective manufacturing. Cost projections indicate a reduction from $400/kg to $60/kg without compromising performance. These findings offer a robust design framework that bridges computational modeling with scalable processing, targeting advanced energy storage applications in electric vehicles, wearable electronics, and distributed energy systems. This study aligns with the journal’s focus on electronic materials with high-performance and scalable integration potential.</p> Graphical Abstract <p></p>

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Defect-Engineered Graphene–Polymer–Oxide Hybrid Electrodes for High-Efficiency Supercapacitors via Scalable Fabrication and Simulation-Guided Design

  • 期刊论文

  • 发表日期：

    2025年10月8日

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  • Maziyar Sabet

摘要

This work presents a defect-engineered graphene–polymer–oxide hybrid electrode tailored for high-efficiency supercapacitors. The architecture integrates high-conductivity chemical vapor deposition (CVD) graphene and solution-processable reduced graphene oxide (rGO), both enhanced via multifunctional surface modifications including π–π conjugated polyaniline (PANI) wrapping, oxygen plasma treatment, and alkali metal intercalation. These modifications optimize charge carrier mobility, interfacial compatibility, and electronic conductivity. Experimental evaluations reveal a specific capacitance of 450 F/g, energy density of 85 Wh/kg, and power density of 70 kW/kg, with 92% retention after 10,000 cycles. To support design insights, density functional theory (DFT) and molecular dynamics (MD) simulations correlate defect density, Fermi level shifts, and charge transport pathways with electrochemical performance. The optimized hybrid system demonstrates superior electronic behavior while being compatible with roll-to-roll (R2R) electrode fabrication, enabling large-scale, cost-effective manufacturing. Cost projections indicate a reduction from $400/kg to $60/kg without compromising performance. These findings offer a robust design framework that bridges computational modeling with scalable processing, targeting advanced energy storage applications in electric vehicles, wearable electronics, and distributed energy systems. This study aligns with the journal’s focus on electronic materials with high-performance and scalable integration potential.

Graphical Abstract