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The flotation of kaolinite using a series of tertiary amines (N,N-dimethyl-dodecyl amine (DRN), N,N-diethyl-dodecyl amine (DEN), N,N-dipropyl-dodecyl amine (DPN) and N,N-dibenzyl-bodecyi amine (DBN)) was investigated. The results show that the maximum recoveries of kaolinite for DEN, DPN and DRN are 93%, 88% and 84%, respectively, but that of DBN is very low. On the basis of zeta potential and FT-IR spectra, the ionization of surface hydroxyl and isomorphic exchange of surface ions account for the charging mechanisms of kaolinite surface. The adsorption mechanism of tertiary amines on kaolinite surface is mainly electrostatic. The isoelectric point (IEP) of kaolinite increases from 3.4 to some more positive points after the interaction of kaolinite with the four tertiary amines. The FT-IR spectra of kaolinite change with the presence of some new sharp shapes belonging to the tertiary amines. The inductive electronic effects and space-steric effects of -CH_3, -C_2H_5, -C_3H_7 and -C_7H_7 bonding to N atom result in different collecting power of the four tertiary amines.