The band structure, density of states, Mulliken populations, and frontier orbital of spodumene crystal were calculated using the first-principles method based on the density functional theory(DFT) and further analyzed in detail. The calculation results reveal that the O in spodumene is the most active and easily links with H+in the water, but the active Li is very low, so it is better to add activator to increase the concentrate grade and recovery rate of spodumene in the flotation process. Si–O bonds in spodumene crystal are mainly covalent, since the covalency of Al–O bonds is stronger than that of Li–O bonds,and minerals dissociate along the weakest Li–O bonds. In addition, the study of the frontier orbital indicates that both O and Si atoms have large contribution to the frontier orbital in the spodumene crystal. Oleate and dodecylamine are used as the collectors of spodumene. The results contribute to the understanding of crystal structures of spodumene, and can be used in guiding related practical applications.
