Thorough characterization
and fundamental understanding of cellulose
fibers can help us develop new, sustainable material streams and advanced
functional materials. As an emerging nanomaterial, cellulose nanofibrils
(CNFs) have high specific surface area and good mechanical properties;
however, handling and processing challenges have limited their widespread
use. This work reports an in-depth characterization of self-fibrillating
cellulose fibers (SFFs) and their use in smart, responsive filters
capable of regulating flow and retaining nanoscale particles. By combining
direct and indirect characterization methods with polyelectrolyte
swelling theories, it was shown that introduction of charges and decreased
supramolecular order in the fiber wall were responsible for the exceptional
swelling and nanofibrillation of SFFs. Different microscopy techniques
were used to visualize the swelling of SFFs before, during, and after
nanofibrillation. Through filtration and pH adjustment, smart filters
prepared
via in situ
nanofibrillation showed an ability
to regulate the flow rate through the filter and a capacity of retaining
95% of 300 nm (diameter) silica nanoparticles. This exceptionally
rapid and efficient approach for making smart filters directly addresses
the challenges associated with dewatering of CNFs and bridges the
gap between science and technology, making the widespread use of CNFs
in high-performance materials a not-so-distant reality.