3D-Printed Interfacially Jammed Emulsion Aerogels

3D printing ultralightweight porous structures using direct ink writing (DIW) while maintaining their mechanical robustness is highly challenging. This difficulty is amplified when low ink concentrations are used to create complex geometries. Herein, this shortfall was addressed by interfacially jammed emulsion gels. The gel emerged from the electrostatic interaction among synergized nanomaterials (graphene oxide (GO) and cellulose nanocrystals (CNCs)) in the aqueous phase and a ligand in the oil phase. This interaction led to the jamming of the nanoparticles and the creation of stable emulsion gels. The formed interfacial assemblies were further treated by post-jamming ionic cross-linking with NaHCO₃, which dictated the emulsion gels' rheological characteristics, enhancing the ink's viscoelastic properties for high-resolution 3D printing. The customizable emulsion system allows control over porosity from the macro- to the micro-scale and generates complex geometries with desired compositions. By manipulating post-annealing processes and varying concentrations, it is possible to achieve aerogels that feature a remarkably low density (∼2.63 mg/cm³) and adjustable mechanical robustness (elastic modulus of 0.45 MPa). Additionally, this method allows for producing aerogels with flexible or stiff characteristics as required, alongside the capability to tailor specific electromagnetic shielding effectiveness (ranging from 6791 to 19615 dB cm²/g), showcasing the technique's versatility and engineerability.