AbstractThere is a large interest in bio-polymers as environment-friendly alternatives to synthetic additives in papermaking. In this work, the behavior of three chitosans with different molecular weights and cationic charges were investigated as flocculation additives in papermaking on two systems: calcium carbonate (GCC) and pulp/GCC suspension. Comparison was made with two traditional cationic polymers used in wet end chemistry (poly-diallyldimethyl-ammonium chloride (PDADMAC) and poly-ethylene imine (PEI)). Flocculation efficiency was evaluated by flocculation parameters (mean floc size and number of counts) and by floc behavior under shear conditions, using a focused beam reflectance measurement (FBRM) technique. Results indicated different behaviors between the three chitosans when they were used for the flocculation of GCC and pulp/GCC suspensions. Chitosans were found to be more efficient over PDADMAC and PEI for flocculating small particles of the GCC suspension, but less efficient for increasing floc sizes, regardless of their MW or CCD. Flocculation parameters for pulp/GCC suspensions suggested the flocculation behavior of chitosan was close to that of PEI, but chitosan had higher efficiency and affinity towards cellulose fibers.