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The atom distribution and electronic properties of (010), (001) and (100) planes of MnWO4 and FeWO4 were studied based on a DFT calculation. The surface stabilities of the three planes were compared according to their surface energies. The most stable one is (010) plane, followed by (001) and (100). (010) and (001) are the main planes for absorption of anion collector ions, which is supported by their bonding relationship and charge density distribution of surface atoms and finally proved by the results of flotation test and stereomicroscope analysis. In addition, the tungsten atoms can be viewed as the absorption site for collectors in (001) plane but not in (010) plane, which can explain the phenomenon in flotation test that the recovery of wolframite can hardly be further boosted even with a high dosage of BHA.