Abstract

In the present work, phosphorylated cellulose (PC) gel has been produced following an environmentally benign approach using agro-based chemicals with improved yield. The PC gels produced were transparent, negatively charged with high consistency, charge content (1133.33 mmol/kg), degree of substitution (DS) of 0.183 and increased yield (>87 %). The XPS and EDS analysis confirms the covalently bonded phosphate groups at weight percent of 9.42 % and 11.01 %, respectively. The life cycle assessment (LCA) shows that PC gel production via the phosphorylation route is an ecologically favourable strategy compared with traditional TEMPO oxidation, resulting in 1.67 times lower CO2 emission. The rheological studies of PC gels show shear-thinning behaviour with improved 3D printability followed by heat-induced crosslinking of phosphate groups. The mechanistic insights for the condensation of phosphate to form a phosphoric ester group during cross-linking were evaluated through 31P solid-state NMR and XPS studies. Interestingly, the 3D-printed structures showed high structural stability under both compression and tensile load in both dry and wet conditions, with high water absorption (5408.33 %) and swelling capacity of 700 %. The structures show improved methylene blue (MB) remediation capabilities with a maximum removal efficiency of 99 % for 10–200 mg/L and more than seven times reusability. This work provides a green, facile and energy-efficient strategy for fabricating PCs with easy processability through additive manufacturing techniques for producing value-added products, opening up new avenues for high-performance applications.

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