Regenerable materials with abundant basic sites and sulfur storage space are highly desirable for the removal of H 2 S. In this work, we synthesized a flower-like MgO/Carbon material by one-step carbonization of magnesium gluconate and applied it for H 2 S oxidation at room temperature. The results demonstrate that the high content of MgO and super-hydrophilic surface of the MgO/Carbon provide abundant basic sites for the adsorption and dissociation of H 2 S. Moreover, carbon defects and a well‐developed pore structure offer active sites for the desulfurization reaction and large space for storage of sulfur products. Consequently, the MgO/Carbon materials exhibit excellent H 2 S oxidation performance, which is far superior to that of commercial activated carbon. In addition, the MgO/Carbon materials show extraordinary regeneration capacity and maintain their high performance even after 5 cycles of desulfurization/regeneration. Furthermore, mechanisms for the H 2 S oxidation process, deactivation and regeneration are proposed based on the experimental and characterization results. Considering the simple preparation process, excellent desulfurization and regeneration performance of as-prepared MgO/Carbon material, our findings provide a new strategy for the design of efficient desulfurizers.
Xinlei Yu,Xun Tao,Yunfei Gao,Lu Ding,Yanqin Wang,Guangsuo Yu,Fuchen Wang
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 ABO3perovskite 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 LaFeO3and LaCoO3, co-doped LaFexCo1−xO3significantly improved the H2S conversion and sulfur selectivity at a lower reaction temperature. Nearly 100% sulfur yield was achieved on LaFe0.4Co0.6O3under 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−xO3changed from the rhombic phase of LaCoO3to the cubic phase of LaFeO3with 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.Keywords:hydrogen sulfide;selective oxidation;perovskite oxides;oxygen vacancy
Yiran Xiong,Langlang Wang,Ping Ning,Jianfei Luo,Xiang Li,Li Yuan,Yibing Xie,Yixing Ma,Xueqian Wang
The rational design of catalyst structures holds paramount significance for realizing efficient catalytic reactions. In this study, an Fe 3 O 4 @MnO 2 core–shell catalyst was successfully synthesized using a facile one-pot method and applied in the selective oxidation of H 2 S in blast furnace gas. The introduction of the MnO 2 shell suppressed the further growth and aggregation of Fe species, leading to outstanding catalytic stability. Simultaneously, abundant oxygen vacancies facilitated the adsorption and activation of oxygen, thereby enhancing H 2 S oxidation. Experimental results revealed that the Fe 3 O 4 @MnO 2 catalyst (Fe/Mn = 4:1) displayed 100 % H 2 S conversion and 95.7 % sulfur selectivity at 150 °C in a humid gas stream containing O 2 and CO. Remarkably, no discernible decline in catalytic activity was observed after 170 h of operation, indicating the promising industrial prospects of this catalyst. This study provides an effective strategy for designing efficient and stable desulfurization catalysts.
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