Surfactant-Mediated Highly Conductive Cellulosic Inks for High-Resolution 3D Printing of Robust and Structured Electromagnetic Interference Shielding Aerogels

Technological fusion of emerging three-dimensional (3D) printing of aerogels with gel processing enables the fabrication of lightweight and functional materials for diverse applications. However, 3D-printed constructs via direct ink writing for fabricating electrically conductive structured biobased aerogels suffer several limitations, including poor electrical conductivity, inferior mechanical strength, and low printing resolution. This work addresses these limitations via molecular engineering of conductive hydrogels. The hydrogel inks, namely, CNC/PEDOT-DBSA, featured a unique formulation containing well-dispersed cellulose nanocrystal decorated by a poly(3,4-ethylene dioxythiophene) (PEDOT) domain combined with dodecylbenzene sulfonic acid (DBSA). The rheological properties were precisely engineered by manipulating the solid content and the intermolecular interactions among the constituents, resulting in 3D-printed structures with excellent resolution. More importantly, the resultant aerogels following freeze-drying exhibited a high electrical conductivity (110 ± 12 S m-1), outstanding mechanical properties (Young's modulus of 6.98 MPa), and fire-resistance properties. These robust aerogels were employed to address pressing global concerns about electromagnetic pollution with a specific shielding effectiveness of 4983.4 dB cm2 g-1. Importantly, it was shown that the shielding mechanism of the 3D printed aerogels could be manipulated by their geometrical features, unraveling the undeniable role of additive manufacturing in materials design.