Exploring the synergistic effect of anionic and cationic fibrillated cellulose as sustainable additives in papermaking

While cationic cellulose has yet to find a place in the paper industry, manufacturers show certain interest in a more recent material: cellulose nanofibers (CNFs), generally with negative surface charge. This work suggests both to be combined to increase the mechanical properties of recycled paper while preventing the use of synthetic polyelectrolytes as retention agents. On one hand, a bleached pulp was cationized by etherification, both as-is and following mechanical refining (15,000 PFI revolutions) and submitted to high-pressure homogenization, generating two different kinds of cationic CNFs. On the other, the same pulp was submitted to an enzymatic pretreatment and high-pressure homogenization, producing a negatively charged cellulose micro/nanofiber (CMNF). Two different cellulose-based systems consisting of each type of cationic CNF and the enzymatic CMNF were applied in the papermaking of both virgin and recycled paper. This study demonstrates the effective use of the cationic CNFs as retention agents during sheet formation, which together with the enzymatic CMNFs significantly enhanced the mechanical properties of both types of paper. The study found that refining before cationization favored the retention effect, primarily due to increased surface area and charge of the cationic CNFs, where remarkable increases in the breaking length of virgin (125.1%) and recycled paper (46.5%) were reached. The synergy between cationic CNFs and enzymatic CMNFs outperformed the use of commercial polyacrylamide, a non-biodegradable polyelectrolyte. This research highlights the potential of tailored CNFs in producing high-performance papers, while promoting sustainability and offering a plausible strategy to increase paper recycling rates.