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Due to the same active Al atoms contained by spodumene, beryl and feldspar, the characteristic surface crystal chemistry of minerals was found to be the major contributing factor for the selective flotation separation. The surface crystal chemistry and anisotropy of spodumene flotation with sodium oleate (NaOL) were studied using single mineral flotation tests, zeta potential measurements, infrared spectral analysis, density functional theory calculation and molecular dynamics simulation. The results show that the flotation recovery rate first increases but then decreases with increasing pH. The flotation recovery rate reaches maximum value at pH 8.5. Within the appropriate particle size range, when the particle size is much more coarse the flotation recovery is higher which shows Al sites on the surface of minerals reacting with NaOL by chemisorption. The order of broken bond densities on the surface of the spodumene crystal planes and interaction energy with NaOL is (110), (001), which is the main cause for the difference in flotation behaviour of spodumene for different particle size fractions., Due to the same active Al atoms contained by spodumene, beryl and feldspar, the characteristic surface crystal chemistry of minerals was found to be the major contributing factor for the selective flotation separation. The surface crystal chemistry and anisotropy of spodumene flotation with sodium oleate (NaOL) were studied using single mineral flotation tests, zeta potential measurements, infrared spectral analysis, density functional theory calculation and molecular dynamics simulation. The results show that the flotation recovery rate first increases but then decreases with increasing pH. The flotation recovery rate reaches maximum value at pH 8.5. Within the appropriate particle size range, when the particle size is much more coarse the flotation recovery is higher which shows Al sites on the surface of minerals reacting with NaOL by chemisorption. The order of broken bond densities on the surface of the spodumene crystal planes and interaction energy with NaOL is (110), (001), which is the main cause for the difference in flotation behaviour of spodumene for different particle size fractions. more...