Complete nanofibrillation of cellulose prepared by phosphorylation

In this work, we prepared phosphorylated pulp with a phosphorous content of 1.23 mmol/g by adding an aqueous solution of NH₄H₂PO₄ and urea to softwood pulp sheets followed by drying and curing with hot air and obtained cellulose nanofibers (CNFs) with a uniform width of 3–4 nm in approximately 100% gravimetric yield by high-pressure homogenization of the phosphorylated pulp slurry. After phosphorylation, no significant decrease in the pulp recovery ratio was observed, and the viscosity-average degree of polymerization of phosphorylated pulp was almost equal to that of the original pulp. In addition, the crystal structure and crystallinity index were almost unchanged during phosphorylation. The obtained phosphorylated CNF dispersion was highly transparent, and the maximum total light transmittance was nearly 100% when the CNF content was 0.2 wt%. The maximum viscosity of the CNF dispersions was nearly 10–100 times greater than that of conventional thickeners. Furthermore, we found that not only insufficient but also excessive phosphorylation negatively affected the gravimetric yield, transparency and viscosity.