Reverse Conversion Treatment of Gaseous Sulfur Trioxide Using Metastable Sulfides from Sulfur-Rich Flue Gas

Sulfur trioxide (SO3) is an unstable pollutant, and its removal from the gas phase of industrial flue gas remains a significant challenge. Herein, we propose a reverse conversion treatment (RCT) strategy to reduce S(VI) in SO(3 )to S(IV) by combining bench-scale experiments and theoretical studies. We first demonstrated that metastable sulfides can break the S-O bond in SO3, leading to the re-formation of sulfur dioxide (SO2). The RCT performance varied between mono- and binary-metal sulfides, and metastable CuS had a high SO3 conversion efficiency in the temperature range of 200-300 degrees C. Accordingly, the introduction of selenium (Se) lowered the electronegativity of the CuS host and enhanced its reducibility to SO3. Among the CuSe1-xSx composites, CuSe0.3S0.7 was the optimal RCT material and reached a SO2 yield of 6.25 mmol/g in 120 min. The low-valence state of selenium (Se2-/Se1-) exhibited a higher reduction activity for SO3 than did S2-/S1-; however, excessive Se doping degraded the SO3 conversion owing to the re-oxidation of SO2 by the generated SeO32-. The density functional theory calculations verified the stronger SO3 adsorption performance (E-ads = -2.76 eV) and lower S-O bond breaking energy (E-a = 1.34 eV) over CuSe0.3S0.7 compared to those over CuS and CuSe. Thus, CuSe1-xSx can serve as a model material and the RCT strategy can make use of field temperature conditions in nonferrous smelters for SO3 emission control.

Automated summary

This study proposes a reverse conversion treatment (RCT) strategy to reduce S(VI) in SO3 to S(IV). By introducing selenium (Se), the reducibility of CuS to SO3 is enhanced. The results demonstrate that CuSe0.3S0.7 is the optimal RCT material with high SO3 conversion efficiency.