Chemically Cross-Linked Cellulose Nanocrystal Aerogels with Shape Recovery and Superabsorbent Properties

Cellulose nanocrystals (CNCs) are entering the marketplace as new high-strength nanoadditives from renewable resources. These high aspect ratio particles have potential applications as rheological modifiers, reinforcing agents in composites, coatings, and porous materials. In this work, chemically cross-linked CNC aerogels were prepared based on hydrazone cross-linking of hydrazide and aldehyde-functionalized CNCs. The resulting aerogels were ultralightweight (5.6 mg/cm3) and highly porous (99.6%) with a bimodal pore distribution (mesopores <50 nm and macropores >1 μm). Chemically cross-linked CNC aerogels showed enhanced mechanical properties and shape recovery ability, particularly in water, compared to previous reports of physically cross-linked CNC aerogels. Specifically, the aerogel shape recovered more than 85% after 80% compression, even after 20 compress and release cycles. These CNC aerogels can absorb significant amounts of both water (160 ± 10 g/g of aerogel) and dodecane (72 ± 5 g/g of aerogel) with cyclic absorption capacity. We demonstrate that CNC aerogels can be used as superabsorbents and for oil/water separations and they may also find application as insulating or shock-absorbing materials. The cross-linking technology developed here presents new ways to design CNC networked structures and suggests an alternate route to incorporate CNCs into matrix materials, such as epoxies and foams.