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Synergistic effect of Cu and Ce bimetallic over MCM-41 zeolite for enhancing the catalytic hydrolysis performance of COS

Journal 2025 · IF 4.9 · 发表于 2025 年 2 月 14 日
作者: Kaixuan Yan,Xin Song,Chunliang Zhou,Junnan Liu,Rongji Cui,Panting Gao,Zhicheng Tang
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摘要

The presence of sulfur-containing impurities in natural gas not only diminishes its utilization value, but also results in the emission of sulfur-containing pollutants. In this study, a Cu-Ce bimetallic-loaded MCM-41 catalyst was prepared by ammonia evaporation method for the catalytic hydrolysis of carbonyl sulfide (COS). The desulfurization efficiency of Cu 25 Ce 5 /MCM-41 can reach a 100 % COS removal rate and maintain for 3.5 h. CuO furnishes the predominant weakly acidic and weakly basic sites for the desulfurization process, which are conducive to the adsorption of COS. Meanwhile, CeOx provides a greater abundance of moderately basic sites for the desulfurization process, which help to improve the removal efficiency of COS. The incorporation of Ce into the catalyst enhances the resistance to sulfur poisoning of Cu and prolongs the lifespan of the catalyst. The incorporation of Ce is capable of transforming the strongly basic sites on the surface of Cu 25 /MCM-41 into moderately basic sites, avoiding excessive oxidation of H 2 S. Additionally, the introduction of Ce offers a degree of protection for CuO, which improves the ability of the catalyst to resist sulfur poisoning. The combined effect of Cu and Ce was found to be instrumental in enhancing the adsorption of COS and in slowing down the oxidation of H 2 S. The reduction of Cu 2+ and Ce 3+ indicated their direct participation in the oxidation of H 2 S. Firstly, COS adsorbed on the catalyst surface is converted into H 2 S and CO 2 through a catalytic hydrolysis reaction. Subsequently, H 2 S adsorbed on the catalyst surface undergoes partial oxidation to sulfide, and partial further oxidation by oxygen-containing functional groups on the surface to S, SO 3 2- , and SO 4 2- , which results in the toxic deactivation of the catalyst.

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