The present current topic demonstrates the formation of novel graphene-based 3D macro structures having lateral sizes of several tens of micrometers, i.e., crown-cork-like structures consisting of stacks of curved multilayer graphene via a chemical vapor deposition method. Based on the elemental, structural and morphological analyses using Raman spectroscopy, energy dispersive X-ray spectroscopy, scanning electron microscope, transmission electron microscope and X-ray diffraction, its origin and formation mechanism are fully discussed. Employing a solid-state reaction using Fe as both a catalyst and a substrate, we have found a new growth form in the precipitation process of C in Fe, established a synthesis method, and obtained new hybrid structures that can be used for electromagnetic response substances and long-term anti-corrosion coatings.
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