Laser-Fabricated GO/ZIF-67 Hybrid Nanocomposites for High-Performance 3D-Printed Supercapacitors

This study introduces a modified Laser Ablation Synthesis in Solution (LASiS), a surfactant-free and rapid synthesis approach that enables uniform MOF nucleation on graphene oxide (GO) and precise control over crystallinity, for fabricating graphene oxide (GO)-integrated cobalt-based ZIF-67 hybrid nanocomposites tailored for supercapacitor applications. By tuning LASiS parameters, we precisely controlled framework size, morphology, and crystallinity, enabling sustainable and scalable production. The incorporation of GO during synthesis markedly enhances the uniform dispersion of ZIF-67 frameworks, minimizing aggregation and establishing interconnected conductive pathways via strong π-π stacking interactions. Following thermal reduction at 250 °C, the Co/ZIF-67–rGO composites exhibit outstanding electrochemical performance, achieving a specific capacitance of 1152 Fg−1 at 1 Ag−1 in a three-electrode configuration, driven by the synergistic combination of pseudocapacitive cobalt centers and double-layer capacitance from rGO. Structural analyses confirm the preservation of ZIF crystallinity and robust interfacial integration with the graphene sheets. Embedding these nanocomposites into fully 3D-printed supercapacitors yields a specific capacitance of 875 Fg−1, demonstrating their suitability for additive manufacturing despite minor increases in interfacial resistance. The 3D-printed supercapacitor devices delivered an energy density of 77.7 Wh/kg at a power density of 399.6 W/kg. Collectively, these results highlight the potential of LASiS-engineered MOF-based nanocomposites as scalable, high-performance materials for next-generation energy storage devices.