化工学报2025，Vol.76Issue(8)：4061-4070,10.DOI:10.11949/0438-1157.20250068
Sm2O3/γ-Al2O3催化剂的COS催化水解性能及失活机制
COS catalyzed hydrolysis performance and deactivation mechanism of Sm2O3/γ-Al2O3 catalysts
摘要
Abstract
Low temperature catalytic hydrolysis of carbonyl sulfide(COS)is a key technology for promoting the clean conversion and utilization of gas.Modern syngas has low COS content after high temperature purification,but industrial gas sources(such as blast furnace and coke oven)have high COS content(75-400 mg·m-3).Therefore,the study of COS hydrolysis technology is of great significance for industrial gas purification and efficient preparation of syngas in the future.Previous studies have shown that γ-Al2O3 loaded with rare earth metals exhibits strong catalytic hydrolysis activity under low COS concentrations,but its behavior under low temperature and high COS concentrations remains unclear.This study investigates the enhancement effects of different rare earth metal oxides(La2O3,Sm2O3 and CeO2)on the catalytic hydrolysis behavior of γ-Al2O3.Based on the influence of gas composition and various structural characterizations,the interactions between the selected rare earth metals andγ-Al2O3 are analyzed.The results indicate that,under conditions of 70℃,1000 mg·m-3 COS,3％H2O and 0.5％O2,the modified catalyst(Sm2O3/γ-Al2O3)with Sm2O3(the mass fraction is 5％)loading shows the best performance.After 8 h of reaction,the selectivity of H2S is 86.3％,and the COS conversion rate remains above 90％,which is higher than that of unmodified γ-Al2O3(65.3％).Additionally,Sm doping enhances the resistance to H2S poisoning,attributed to the increased basic sites on the surface of γ-Al2O3.The presence of CO2 significantly weakens the effect of Sm2O3/γ-Al2O3 on COS conversion(reduced by 39.6％),which is due to the competitive adsorption of CO2 leading to catalyst deactivation,and this process is reversible.In addition,under the coexistence of H2S and CO2,CO2 preferentially adsorbs on the catalyst surface,occupies basic sites and rapidly deactivates the catalyst.关键词
低温催化/COS催化水解/碱性位点/H2S选择性Key words
low temperature catalysis/COS catalytic hydrolysis/basic sites/H2S selectivity分类
化学化工引用本文复制引用
杨敏,段新伟,吴俊宏,米杰,王建成,武蒙蒙..Sm2O3/γ-Al2O3催化剂的COS催化水解性能及失活机制[J].化工学报,2025,76(8):4061-4070,10.基金项目
国家自然科学基金面上项目(22278294) （22278294）
山西省自然科学基金面上项目(20210302123191) （20210302123191）
中央引导地方科技发展资金项目(YDZJSX2025C006) （YDZJSX2025C006）
