Natural gas regeneration of carbonate melts following SO2 capture from non-ferrous smelter emissions

Sulfur emission in the form of SO2 in flue gases is the one of the most serious atmospheric pollutants associated with coal combustion and non-ferrous metal production. The carbonate eutectic method for removing SO2 from flue gases at 723-923 K was initially proposed in the 1970's but despite its great efficiency (SO2 concentration in the flue gas after purification reached 0.003 vol%) it could not be implemented by industry due to the complexity of the carbonate melt regeneration stage. Earlier we proposed a method suited to coal-firing power stations where the melt was regenerated using CO as a reducing agent. However, most metallurgical plants do not use coal and therefore lack a large source of CO. Here we propose a method for removing sulfur from the carbonate eutectic melt by purging it with natural gas or a natural gas/air mixture, which are available in the vast majority of metallurgical plants. This reaction leads to the reduction of sulfate to H2S gas that leaves the melt. The experiments we conducted show that nearly complete sulfur removal from the melt is possible at 823 K and that the reaction rate is sufficiently high for a large scale process. The proposed modifications provide solutions to two major problems previously encountered: (i) high temperature corrosion of the reaction cell can be avoided, since a stainless steel cell with high chromium content is stable with respect to the carbonate eutectic melt at 823 K, and (ii) removal of sulfur in the form of H2S provides considerable freedom in choosing the final industrially useful product: either sulfuric acid, using H2S dry combustion, or elemental sulfur via the Claus process. One can foresee that this carbonate melt-based SO2 removal technique may become a practical and economically attractive method for limiting sulfur emission to the atmosphere from non-ferrous metallurgical processing plants.