Carbonate melt regeneration for efficient capture of SO2 from coal combustion

Abstract

Sulfur emission in the form of SO2 in flue gas is the most serious pollutant associated with coal combustion. Calcium carbonate sulfur scrubbing, the process most commonly in use today, is costly, produces a large amount of waste and leaves a considerable amount of SO2 in the gas. The carbonate eutectic method for removing SO2 from flue gas at 450–650 °C was initially proposed in the 1970's but despite its great efficiency could not be used due to the complexity of the carbonate melt regeneration stage. We propose a simple way to remove sulfur from the carbonate eutectic melt by purging it with CO. In contrast to expectation, this reaction leads to the reduction of sulfate to carbonyl sulfide gas that leaves the melt, rather than to sulfide ions that remain in the melt. The experiments conducted show that nearly complete sulfur removal from the melt is possible at 550 °C and that the reaction rate is sufficiently high for a large scale process. The proposed modifications provide solutions to two critical issues: (i) at 550 °C there is no problem of corrosion because a reaction cell of stainless steel with high chromium content is stable with respect to the carbonate eutectic melt at that temperature and (ii) removal of sulfur in the form of COS, rather than H2S, provides considerable freedom in choosing the final product: either sulfuric acid or elemental sulfur. In addition, we verified that fly ash does not dissolve in the carbonate eutectic melt and therefore will not interfere with SO2 removal. One can foresee that the carbonate melt-based SO2 removal technique may become a practical and viable method for limiting sulfur emission to the atmosphere.