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Title
Preparation and properties of MnCu/Ce catalyst for CO preferential oxidation reaction
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作者
武嘉欣韩蛟李学邢月张财顺刘道胜侯晓宁刘雅杰张磊高志贤
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Author
WU Jiaxin;HAN Jiao;LI Xue;XING Yue;ZHANG Caishun;LIU Daosheng;HOU Xiaoning;LIU Yajie;ZHANG Lei;GAO Zhixian
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单位
辽宁石油化工大学 石油化工学院中石油天津天然气管道有限公司山西师范大学 化学与材料科学学院晋中学院 化学化工系
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Organization
School of Petrochemical Engineering, Liaoning Petrochemical University
Petrochina Tianjin Gas Pipeline Co., LTD., Petrochina
School of Chemistry and Materials Science, Shanxi Normal University
Department of Chemistry and Chemical Engineering, Jinzhong University
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摘要
采用共浸渍法制备较低Cu含量的MnCu/Ce催化剂,通过XRD、BET、H2-TPR、XPS和CO2-TPD等表征手段对催化剂进行表征,考察催化剂焙烧温度对催化剂结构、性质及其在含有CO2的富氢气氛下对CO优先氧化性能的影响。结果表明,MnCu/Ce催化剂均有Cu/Mn-O-Ce固溶体形成,其中,在焙烧温度600 ℃制备的催化剂中,Mn与Cu、Ce之间相互作用较强,形成较多三元氧化物固溶体,氧空位/Ce3+含量高,具备良好的CO-Prox活性。此外,对反应条件的考察发现,添加不同分压Ar对催化剂的CO-Prox活性影响较小,气体空速和氧过量系数对催化剂活性影响较大,且反应原料气中CO2的存在对CO-Prox反应有负面影响。氧过量系数为1.2、空速范围为20266−30400 mL/(g·h)时,CO转化率最高,达到94.7%。
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Abstract
The MnCu/Ce catalyst with a lower Cu content was prepared by co-impregnation method, and then was characterized by XRD, BET, H2-TPR, XPS and CO2-TPD. The effects of calcination temperature on the structure and properties of the catalyst and the preferential oxidation of CO in a hydrogen-rich atmosphere containing CO2 were investigated. The results indicated that Cu/Mn-O-Ce solid solution was formed in all MnCu/Ce catalysts. Of theses sample, the one calcined at 600 ℃ had strong interaction among Mn, Cu and Ce, formed more ternary oxide solid solution with more oxygen vacancies/Ce3+, and revealed good CO-Prox activity. In addition, it was found that the addition of different percentage of Ar had little effects on the CO-Prox activity of the catalyst, while the space velocity and oxygen excess coefficient had great effects on the catalytic performance, and the presence of CO2 in the reaction feedstock gas had a negative effect on the CO-Prox reaction. At an oxygen excess coefficient of 1.2 and the space velocity of 20266−30400 mL/(g·h), the highest CO conversion rate reached 94.7%.
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关键词
低含量铜焙烧温度氧化铈CO2/H2气氛反应条件
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KeyWords
low content copper;roasting temperature;cerium oxide;CO2/H2 atmosphere;reaction condition
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基金项目(Foundation)
国家自然科学基金(22379059),辽宁省应用基础研究计划项目(2023JH2/101300224),辽宁省教育厅服务地方项目(揭榜挂帅)(LJKFZ20220201),辽宁省教育厅面上项目(LJKMZ20220728),山西省应用基础研究青年基金项目(20210302124338)和辽宁石油化工大学引进人才科研启动基金资助项目(2019-XJJL-028)
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DOI
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引用格式
武嘉欣, 韩蛟, 李学, 邢月, 张财顺, 刘道胜, 侯晓宁, 刘雅杰, 张磊, 高志贤. CO优先氧化反应MnCu/Ce催化剂的制备及性能[J]. 燃料化学学报(中英文), 2024, 52(4): 565-576.
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Citation
WU Jiaxin, HAN Jiao, LI Xue, XING Yue, ZHANG Caishun, LIU Daosheng, HOU Xiaoning, LIU Yajie, ZHANG Lei, GAO Zhixian. Preparation and properties of MnCu/Ce catalyst for CO preferential oxidation reaction[J]. Journal of Fuel Chemistry and Technology, 2024, 52(4): 565-576.
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