Freestanding 3D Multilayer Graphene Foams from Nanotextured Ni-Cu Templates

Three-dimensional (3D) graphene foams are attractive as lightweight conductive scaffolds with large surface area and broadband light absorption but achieving reproducible porosity and preserving the architecture after metal-template removal remain challenging. Here we report a stepwise route to freestanding 3D multilayer graphene foams based on (i) hydrogen-bubble-assisted electrodeposition of porous Ni on Cu foils, (ii) time-controlled pre-annealing at 1000 °C to drive Cu diffusion and form porous Ni-Cu alloy templates, (iii) in situ graphene CVD at 1000 °C under fixed growth conditions, and (iv) wet etching to remove the metal scaffold without a polymer support. The influence of pre-annealing (0, 1, 3, and 7 h) on template evolution, graphene growth, and foam stability was systematically investigated via SEM, EDS, XRD and Raman studies. Before etching, Raman spectroscopy indicates low-defect graphenic coatings with locally heterogeneous few-layer-like to multilayer-like signatures. Only samples pre-annealed for at least 3 h preserved the porous 3D architecture after metal removal, indicating the formation of self-supporting graphenic networks with improved post-etch morphological stability. Raman and XRD analyses further revealed a progressive reduction in structural degradation, residual strain, and stacking disorder with increasing pre-annealing time. Among the investigated samples, the foams obtained after 3 and 7 h of template pre-annealing combined preserved 3D morphology with low sheet resistance (10–20 Ω/□), negligible optical transmittance (<5%), and strong broadband visible-light absorption (75–90%).