The precombustion desulfurization of coal was investigated by photochemical methods and by the application of a novel pyrite depressant in froth flotation. Semiconductor photoelectrochemical catalysis was extensively examined. As much as 41% of the organic sulfur was removed and 72% overall desulfurization of micronized Illinois No. 2 coal was obtained. Zinc oxide, in colloidal suspension, produced a small increase in the overall desulfurization at longer reaction times when compared to direct photolysis. The major limiting factor in organic sulfur removal from coal appears to be accessibility rather than reactivity. Kinetic experiments conducted with the model organosulfur compound, dibenzothiophene, showed high photochemical reactivity with nearly complete conversion occurring in 5 minutes in a saturated solution at 25°C. Scanning electron microscopic examination of product coals showed empty casts in places once occupied by iron pyrite. Additionally, a novel process was developed for separating clean coal from metal sulfide minerals such as pyrite and marcasite. The process comprises depressing the metal sulfide minerals with a reagent resulting from the alkaline oxidation and polymerization of a polyphenol or a quinone, and selectively floating clean coal from the depressed metal sulfide minerals. The process was investigated using microflotation, conventional Denver cell flotation, and microbubble column flotation. Up to 90% pyritic sulfur rejection was achieved from a coal and coal pyrite synthetic mixture. The process efficiency is a function of pH with greater improvements generally occurring at acidic pH when compared with the results obtained in the absence of the quinonoid reagent. However, in the case of microbubble column flotation with micronized coals, the largest overall pyritic sulfur and ash rejection occurred under alkaline conditions. Data from x-ray photoelectron spectroscopy and calorimetry indicate the quinonoid reagent modified the surface properties of minerals by reversible adsorption. / Ph. D.