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The flocculation behavior of ultrafine kaolinite suspension was investigated through settlement tests and FTIR method wasemployed to probe the adsorption mechanism of flocculant on kaolinite. The results show that the maximum settling rate of kaoliniteoccurs at pH value of 3.33, which is close to the point of zero charge(PZC) of kaolinite (3.5). This result is in good agreement withthe double electric layer theory. Kaolinite suspension reaches the largest settling rate at a low concentration of 39 g/t for polydiallyl-dimethyl-ammonium chloride(PDADMA) flocculant, whereas for polyacrylamides(PAM) the dosage is required to be 500 g/t.When macromolecule polymer is adsorbed on surface, kaolinite particles may be flocculant due to the bridging effect. There arecation flocculant characteristic bands on the spectrum of kaolinite but no obvious shifting. Thus, the adsorption of polydiallyl-dimethyi-ammonium chloride on kaolinite surface is physical adsorption.