燃料化学学报(中英文)2025,Vol.53Issue(1):106-115,10.DOI:10.3724/2097-213X.2024.JFCT.0020
Mo-Sn催化剂上CO催化氧化的研究
Investigation on catalytic oxidation of CO over Mo-Sn catalysts
摘要
Abstract
With the rapid development of industry and the gradual improvement of environmental awareness,air pollution has emerged as a prominent environmental issue.Carbon monoxide(CO),generated from the incomplete combustion of carbon-containing substances such as coal and oil,as well as produced by the exhaust emissions of vehicles,is one of the primary sources of atmospheric pollution.Herein,the elimination of low-concentration CO has been widely used in various applications,including industrial flue gas purification,automobile exhaust treatment,and hydrogen fuel cell purification,etc.Therefore,studying the elimination process of low-concentration CO has important practical significance.At present,low-temperature catalytic oxidation of CO is widely recognized as the most direct,simple,inexpensive,and effective method for CO elimination.Additionally,as a classic and simple reaction process,CO oxidation reaction can be often used as a probe reaction to investigate metal-support interactions,adsorption/dissociation behaviors,the structure of active centers,and the structure-activity relationship of catalysts.SnO2 has been used as a catalyst for CO catalytic oxidation due to its low energy for oxygen vacancy formation and the proven reducibility and reactivity of lattice oxygen.However,due to less active sites on the surface of SnO2 for CO catalytic oxidation,complete conversion of CO can only be achieved at higher reaction temperatures,thereby limiting its application.Specifically,molybdenum oxide is a typical non-precious metal catalytic material that is widely used in low-temperature selective oxidation reactions due to its diverse coordination structures and easily adjustable electronic states.Previous research has found that the directional oxidation of alcohol/ethers to target products can be achieved by regulating the active site structure of Mo-Sn catalysts,which exhibited unique and excellent low-temperature oxidation performance.Its adjustable structure,variable valence state,and highly active oxygen species provide new ideas for expanding the application of Mo-Sn catalysts in low-temperature oxidation of CO.In order to further investigate the mechanism and structure-activity relationship of Mo-Sn catalysts in CO catalytic oxidation reaction,in this work,a series of Mo-Sn catalysts with different Mo/Sn molar ratios were prepared by precipitation impregnation method.CO oxidation reaction was used as a probe reaction to investigate the effect of different Mo contents on the catalytic performance of CO oxidation,and further elucidate the active center structure and structure-activity relationships of the catalysts.The results showed that the Mo1Sn20 catalyst achieved complete conversion of CO at 300℃,which was 50℃lower than that of pure SnO2.XRD,Raman,XPS,H2-TPR and in situ FT-IR were used to analyze the crystal structure,valence state of molybdenum species,and redox properties of the catalysts.Compared with pure SnO2 catalyst,when a lower content of Mo species is introduced,the increase in specific surface area of Mo1Sn20 catalyst provides more active sites for the reaction.The enhanced interaction between Mo and Sn leads to the partial transformation of MoO3 to MoOx,producing more Mo5+species.The presence of Mo5+species promotes the adsorption activation of oxygen as well as the migration of oxygen atoms.The synergistic effect of lattice oxygen and Mo5+species enhances the catalytic performance of the CO.This study not only provides a new strategy for efficient catalytic elimination of low concentration CO,but also deeply reveals the structure-activity relationship and active center structure of Mo-Sn catalysts in CO oxidation reactions.Also,it provides theoretical basis and experimental reference for the application of Mo-Sn catalysts in more important catalytic oxidation reactions.关键词
CO/催化氧化/Mo-Sn催化剂/Mo5+物种Key words
CO/catalytic oxidation/Mo-Sn catalyst/Mo5+species分类
化学化工引用本文复制引用
张伟,高秀娟,杨媛,曹国壮,王佳豪,宋法恩,伞晓广,韩怡卓,张清德..Mo-Sn催化剂上CO催化氧化的研究[J].燃料化学学报(中英文),2025,53(1):106-115,10.基金项目
The project was supported by the National Natural Science Foundation of China(22172187),the Central Guidance on Local Science and Technology Development Fund of Shanxi Province(YDZJSX2022A073),the Youth Innovation Promotion Association CAS(2014155),the Liaoning Educational Department Foundation(LJKMZ20220762,JYTMS20231510),the Natural Science Foundation of Liaoning Province(2023-MS-235,2023-MSLH-270),the Key Project in Science&Technology of SYUCT(2023DB005).国家自然科学基金(22172187),山西省中央引导地方科技发展资金项目(YDZJSX2022A073),中国科学院青年创新促进会人才项目(2014155),辽宁省教育厅基金会(LJKMZ20220762,JYTMS20231510),辽宁省自然科学基金(2023-MS-235,2023-MSLH-270)和沈阳化工大学科技重点项目(2023DB005)资助 (22172187)