Chitosan was selected as a natural coagulating agent for the removal of acid dyes (Acid Blue 292; AB292, and Acid Red 398; AR398) from dye-containing solutions. The study was organised in two phases. In phase 1, chitosan was used alone as a natural coagulant for the removal of the dyes. For this purpose, the effect of different parameters including pH, chitosan dosage and initial dye concentration on the dye removal efficiency was examined. In phase 2 of the study, the application of chitosan as a natural coagulant aid in conjunction with polyaluminium chloride (PAC) was assessed. According to the results of phase 1, the best removal efficiencies occurred in an acidic pH range (less than 6) for both of the dyes. Also, excellent dye removal results (about 90%) were achieved with relatively low dosages of chitosan (30–35 mg L−1 for AB292 and 50–60 mg L−1 for AR398). However, the initial concentration of the dyes severely influenced the coagulation performance of chitosan, which can constrain the performance of chitosan as a natural coagulant. On the basis of the results of phase 2, chitosan, as a natural coagulant aid, noticeably enhanced the dye removal efficiency of PAC, especially in the case of AB292. Small amounts of chitosan (3 or 5 mg L−1) enhanced the dye removal efficiency of PAC up to 2.5 times for AB292.

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