Immolative Side Chains on Conjugated Polymer Unlock One-Pot Synthesis of Conductive Carbon Nanotube-Cellulose Aerogels

Cellulose-based aerogels, particularly those incorporating cellulose nanocrystals (CNC), are gaining attention for their lightweight, high surface area, and tunable properties. This study introduces a novel approach to enhance CNC-based aerogels by incorporating single-walled carbon nanotubes (SWNTs) as conductive fillers, improving both mechanical strength and electrical conductivity. We use a conjugated polymer (CP), poly­(fluorene-co-phenylene) with a self-immolative linker (SIL), to achieve better solubility and uniform dispersion of SWNTs in DMF. The SIL remains stable under ambient conditions but degrades rapidly with a simple tetra-n-butylammonium fluoride (TBAF) treatment. Leveraging the solubility of CNCs in a TBAF/DMSO mixture, we prepared CP-SWNT-cellulose composite aerogels through simple mixing, followed by solvent exchange, and freeze-drying. These aerogels, held together by hydrogen bonding, exhibit enhanced mechanical properties, electrical conductivity, and elasticity. With 9.3% SWNT content by weight, the aerogels demonstrate impressive shape recovery and conductivity, making them good candidates for piezoresistive pressure sensors. This work presents a straightforward strategy for developing high-performance conductive aerogels with broad potential in advanced technological applications.