Dissolving
pulp has been subjected to consecutive periodate/chlorite
treatments to afford 2,3-dicarboxyl cellulose (DCC, 1.02 mmol
g–1 COOH). Subsequent nanofibrillation afforded
stable nematic nf-DCC dispersions (average particle
size 2.1 nm × 525 nm) at significantly lower energy input compared
to TEMPO-oxidation. Acid-induced gelation triggered by extensive hydrogen
bonding sets the ordered state and affords free-standing hydrogels
that can be converted to highly transparent birefringent aerogels
by scCO2 drying. Uniaxial compression of the obtained ultra-lightweight
ductile nf-DCC aerogels down to 5% of their original
volume intriguingly preserves nematic orientation and transparence.
Simultaneously, strain hardening translates into exceptionally good
mechanical properties, such as toughness at nearly zero Poisson’s
ratio. Uniaxial compression has been furthermore demonstrated to be
a facile and efficient means for converting nf-DCC
aerogels of broad, multiscale pore size distribution into entirely
micro/mesoporous scaffolds of narrow size distribution at
far-reaching preservation of porosity. Following this approach, thermally
superinsulating nf-DCC aerogels (λ = 0.018
W m–1 K–1) have been prepared,
whose intriguing mechanical properties, transparence, and nematic
ordering bear great potential for other applications as well.