We
herein report the production of environmentally inspired all-cellulose
composites in response to the ever-growing concern on the extensive
usage of nonbiodegradable materials derived from nonrenewable resources.
Hydroxypropyl methylcellulose (HPMC) was used as a film-forming matrix,
while microcrystalline cellulose (MCC) was added as a reinforcement
filler. Because the efficiency of fillers in transferring mechanical
strength to polymer matrixes relies upon the dispersion level of the
former within the latter, this contribution set out to improve the
homogeneity of the composite films through a green, solvent-free approach.
Indeed, as-received MCC actually decreased the tensile strength, Young’s
modulus, and elongation at break of HPMC films in ca. 80%, 33%, and
90%, respectively. High-pressure microfluidization was demonstrated
to break MCC particles down, not to play a role on cellulose crystallinity,
and to expose surface groups and/or create mechanoradicals, as suggested
by a combination of spectroscopic, structural, morphological, and
rheological techniques, capable of interacting with HPMC and increasing
MCC colloidal stability, thus lessening particle aggregation and improving
its dispersion within film matrix. A central composite design guided
the optimization of the filler–matrix interaction, which presented
a quadratic behavior; that is, overprocessing led to impaired mechanical
properties. Seven cycles was the most cost-effective processing condition
leading to the strongest, stiffest composites. This study sheds light
on the effect of high-pressure microfluidization on cellulosic particles
and on the impact of these in all-cellulose composites.