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

被引:0
作者
Yan, Kaixuan [1 ,2 ]
Song, Xin [1 ]
Zhou, Chunliang [2 ]
Liu, Junnan [2 ]
Cui, Rongji [1 ,3 ]
Gao, Panting [1 ]
Tang, Zhicheng [1 ,3 ]
机构
[1] Yantai Zhongke Res Inst Adv Mat & Green Chem Engn, Shandong Lab Adv Mat & Green Mfg Yantai, Yantai 264006, Peoples R China
[2] Harbin Engn Univ, Yantai Res Inst, Yantai 264000, Peoples R China
[3] Chinese Acad Sci, Lanzhou Inst Chem Phys, Natl Engn Res Ctr Fine Petrochem Intermediates, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Peoples R China
来源
MOLECULAR CATALYSIS | 2025年 / 575卷
关键词
Synergistic effects; Bimetallic; Carbonyl sulfide; Catalytic hydrolysis; MCM-41; CARBONYL SULFIDE; ACTIVATED CARBON; METAL OXIDES; EFFICIENT; GAS; HYDROGENATION; ADSORPTION; CS2;
D O I
10.1016/j.mcat.2025.114897
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
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 Cu25Ce5/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 Cu25/MCM-41 into moderately basic sites, avoiding excessive oxidation of H2S. 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 H2S. The reduction of Cu2+ and Ce3+ indicated their direct participation in the oxidation of H2S. Firstly, COS adsorbed on the catalyst surface is converted into H2S and CO2 through a catalytic hydrolysis reaction. Subsequently, H2S adsorbed on the catalyst surface undergoes partial oxidation to sulfide, and partial further oxidation by oxygen-containing functional groups on the surface to S, SO32-, and SO42-, which results in the toxic deactivation of the catalyst.
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页数:11
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