Pulse Electrodeposition-Assisted Ni Catalysts for Methane-Derived Carbon Nanostructure Growth on Woven Carbon Fabrics

Engineering carbon nanostructures directly on carbon fiber fabrics offers an effective route to constructing hierarchical multifunctional coating systems. In this study, methane-based chemical vapor deposition (CVD) was employed to investigate nanocarbon coating formation on woven carbon fabrics supported by electrodeposited Ni catalysts. Catalyst morphology was systematically engineered through surface pretreatment, electric-field configuration, and pulse electrodeposition. At 700 °C, methane activation was insufficient to sustain continuous nanocarbon growth, indicating a temperature-dependent activation threshold. Raising the growth temperature to 900 °C enabled sustained methane decomposition and produced dense nanocarbon coatings; hydrogen assistance suppressed amorphous deposition and promoted more ordered nanofilament features. Pulse electrodeposition refined Ni catalyst dispersion and nucleation density, improving coating uniformity compared with direct-current deposition. Structural ordering was further supported by Raman spectroscopy (D and G bands with an average ID/IG of 0.678 ± 0.068 for methane-grown samples versus 0.798 ± 0.011 for electrodeposition-only controls) and by HRTEM revealing multi-layer graphitic walls (~0.34 nm interlayer spacing). Together, the results support a methane-derived dissolution–diffusion–precipitation growth pathway governed by catalyst morphology, temperature, and gas composition. This controllable, textile-compatible catalyst engineering approach provides a scalable route to hierarchical graphitic coatings for carbon-fabric-based composites, electromagnetic interference shielding, and thermal management applications.