The reactivity of various Ca-based sorbent materials in pelletized form with H2S or CO2 was investigated at high temperatures (750--880°C). An extensive study was conducted to compare the performance of sorbent pellets derived from plaster of Paris and limestone. Multicycle absorption and regeneration tests showed that plaster-based pellets out performed the limestone-based pellets primarily due to a higher surface area and mesoporosity.;The effect of pore-modifiers on the reactivity of limestone with H 2S was investigated by incorporating additives such as cornstarch, graphite and polyvinylalcohol (PVA) in the sorbent. Multicycle sulfidation and regeneration tests of the modified sorbent showed that starch did not improve the reactivity of the limestone, graphite reduced the reactivity, while PVA improved it.;The effect of the chemical additives MgO and SrO on the performance of CaO-based sorbent pellets was investigated. The effect of MgO was tested by starting with materials that contained MgCO3 in a natural form, such as dolomite. The effect of SrO was tested by starting with SrCO 3 either co-precipitated with CaCO3 or by wet-mixing SrCO 3 with limestone in slurry form. The MgO was found to improve the thermal stability of the CaO-based sorbent but lowered the overall absorption capacity of the material when reacted with CO2 or H2S, while SrO decreased the thermal stability of the sorbent when it was reacted with CO2; no absorption tests were run with H2S.;A study of the performance of pelletized CaO-based cores coated with a refractory material such as alumina and limestone or alumina and kaolin was conducted. The reactivity of the core and shell pellets with H2S was determined. The strength and durability of the pellets were determined by using crushing strength analysis and abrasion resistance tests. Pellets coated with either alumina and limestone or alumina and kaolin proved to be strong and adequate for use in industrial reactors.;A semi-empirical mathematical model was developed to represent the reaction of H2S with a sorbent pellet. The model was based on the well-known shrinking core model and it was applied successfully for the analysis of both pellet cores and core and shell pellets reacting with H2S.