Pyrite (FeS₂) is the major source of sulfur in various coals, and its efficient removal has proven to be a more difficult task than expected. Flotation is generally considered to be the most practicable process for the preparation of coal fines. However, even this technique is usually unable to remove more than 50% of pyrite from a 65-mesh coal sample, which is the typical feed to flotation. There are three major reasons for the low separation efficiency of liberated pyrite from coal by flotation. They include self-induced hydrophobicity of pyrite caused by superficial oxidation, nonselective hydraulic entrainment of pyrite particles into froth product, and incomplete liberation of pyrite from coal that results in composite coal-pyrite particles, i.e., middlings. The present study was undertaken to address problems associated with these recovery mechanisms of pyrite and develop techniques to enhance pyrite rejection in coal flotation. To better understand self-induced hydrophobicity of pyrite, chronoamperometry and voltammetry on freshly fractured electrodes were used to explore incipient oxidation and reduction of the mineral. Voltammetry on rotating ring-disc electrodes (RRDE) was carried out to provide information on soluble species and kinetics of oxidation and reduction processes. X-ray photoelectron spectroscopy (XPS) was used for chemical identification of oxidation products. Galvanic coupling with sacrificial anodes was investigated as a practical method to cathodically protect pyrite and prevent its oxidation. Microflotation tests were conducted under controlled potentials at different solution pH's, and the results were correlated with electrochemical studies. The feasibility of improving pyrite rejection by controlling its surface chemistry was tested in flotation experiments conducted with a 2"-diameter microbubble flotation column and a conventional 5-liter Denver flotation cell. Effects of froth stability on the microbubble flotation of coal were studied with an objective of minimizing hydraulic entrainment of pyrite. The operating parameters were systematically varied to study their effects on water recovery which was used as a measure of froth stability. It has been demonstrated that the upgrading of coal in a flotation column can be significantly improved when froth stability is properly controlled. In an attempt to enhance the rejection of pyrite in middlings, various column circuits were experimentally examined and theoretically analyzed. The effect of circuit configuration on the overall circuit performance was evaluated by separation efficiency and separation curves. It has been shown that the overall separation efficiency of column flotation is rather insensitive to circuitry due to the unique characteristics of the unit flotation column, i.e., the addition of the wash water into the froth. / Ph. D.