Abstract
Compared to the Claus process, selective H2S catalytic oxidation to sulfur is a promising reaction, as it is not subject to thermodynamic limitations and could theoretically achieve ~100% H2S conversion to sulfur. In this study, we investigated the effects of Co and Fe co-doping in ABO3 perovskite on H2S selective catalytic oxidation. A series of LaFexCo1−xO3 (x = 0, 0.2, 0.4, 0.6, 0.8, 1.0) perovskites were synthesized by the sol-gel method. Compared to LaFeO3 and LaCoO3, co-doped LaFexCo1−xO3 significantly improved the H2S conversion and sulfur selectivity at a lower reaction temperature. Nearly 100% sulfur yield was achieved on LaFe0.4Co0.6O3 under 220 °C with exceptional catalyst stability (above 95% sulfur yield after 77 h). The catalysts were characterized by XRD, BET, FTIR, XPS, and H2-TPR. The characterization results showed that the structure of LaFexCo1−xO3 changed from the rhombic phase of LaCoO3 to the cubic phase of LaFeO3 with Fe substitution. Doping with appropriate iron (x = 0.4) facilitates the reduction of Co ions in the catalyst, thereby promoting the H2S selective oxidation. This study demonstrates a promising approach for low-temperature H2S combustion with ~100% sulfur yield.
Highlights
Academic Editors: Baiqian Dai, Natural gas processing/utilizing processes, petroleum refining processes, and coal chemistry produce H2 S-containing waste gas [1,2,3].The removal of H2 S from industry waste gas is crucial as H2 S is a toxic and corrosive gas, leading to severe pollution and equipment/pipeline corrosion [4]
A series of LaFex Co1−x O3 catalysts were synthesized by the sol-gel method and investigated for H2 S selective oxidation
The incorporation of Fe into LaCoO3 had a great influence on the conversion and selectivity of H2 S selective oxidation reaction
Summary
Academic Editors: Baiqian Dai, Natural gas processing/utilizing processes, petroleum refining processes, and coal chemistry produce H2 S-containing waste gas [1,2,3].The removal of H2 S from industry waste gas is crucial as H2 S is a toxic and corrosive gas, leading to severe pollution and equipment/pipeline corrosion [4]. A catalyst with remarkable catalytic activity, excellent selectivity, outstanding stability, and desired stoichiometric H2 S/O2 operating conditions is urgently needed. Perovskite oxides such as ABO3 have been extensively investigated. For (distorted) perovskites with lower symmetry, the first shell coordination numbers are smaller It is well-recognized that the tuning of A and B site cations can affect the catalytic activity and stability of perovskite oxides. It is desired to obtain catalysts with ~100% H2 S conversion and ~100% sulfur selectivity, and the influence of co-doping Fe and Co into the B-site of perovskite could be further explored. On the basis of these results, the catalytic and deactivation mechanisms of H2 S selective oxidation over LaFex Co1−x O3 are discussed
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