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Ce-MnOx低温净化氮氧化物和一氧化碳的催化性能研究
引用本文:韩新宇,刘凯杰,边梦瑶,张一波,杨向光.Ce-MnOx低温净化氮氧化物和一氧化碳的催化性能研究[J].无机盐工业,2021,53(12):35-42.
作者姓名:韩新宇  刘凯杰  边梦瑶  张一波  杨向光
作者单位:1.中国科学技术大学,安徽合肥 2300262.中国科学院赣江创新研究院3.中国科学院长春应用化学研究所
基金项目:国家自然科学基金项目(22072141);国家自然科学基金项目(22176185);国家自然科学基金项目(21872133);中国科学院青年创新促进会人才项目(2018263);江西省自然科学基金项目(20212BAB213032);中国科学院重点部署项目(ZDRWCN-2021-3-3-3);中国科学院赣江创新研究院自主部署项目(E055C003)
摘    要:为协助工业界实现碳达峰与碳中和的目标,聚焦于低温烟气中氮氧化物(NOx)和一氧化碳(CO)的协同脱除,以铈(Ce)和锰(Mn)的无机盐为前驱体,采用共沉淀法、机械球磨法、溶液燃烧法和溶胶-凝胶法制备了Ce元素改性的Mn基氨选择性催化还原(NH3-SCR)/一氧化碳(CO)氧化双效纳米催化剂。使用固定床-在线质谱/色谱测试系统对催化剂性能进行了评价,并利用X射线衍射、氮气-物理吸附等表征手段对Ce-MnOx纳米催化剂进行了表征分析。结果表明,反向共沉淀法制备的催化剂具有最优的NOx和CO协同脱除性能,在100 000 mL/(g·h)的高空速条件下,140 ℃以上能够实现CO净化率超过85%,100 ℃以上能够脱除气体中80%以上的NOx,且运行20 h后仅出现微弱的性能衰减。其活性组分为具有高比表面积(100 m2/g以上)的CeMnOx,因此能够吸附更多气体进行反应,表现出优异的催化性能。

关 键 词:低温选择性催化还原  一氧化碳催化氧化  稀土元素  锰氧化物  
收稿时间:2021-10-24

Catalytic performance study of Ce-MnOx for low-temperature purification of nitrogen oxides and carbon monoxide
HAN Xinyu,LIU Kaijie,BIAN Mengyao,ZHANG Yibo,YANG Xiangguang.Catalytic performance study of Ce-MnOx for low-temperature purification of nitrogen oxides and carbon monoxide[J].Inorganic Chemicals Industry,2021,53(12):35-42.
Authors:HAN Xinyu  LIU Kaijie  BIAN Mengyao  ZHANG Yibo  YANG Xiangguang
Affiliation:1. University of Science and Technology of China,Hefei 230026,China2. Ganjiang Innovation Academy,Chinese Academy of Sciences3. Changchun Institute of Applied Chemistry,Chinese Academy of Sciences
Abstract:In order to assist the industry in achieving the goal of emission peak and carbon neutrality,focusing on the syner-gistic removal of oxynitrides(NOx) and carbon monoxide(CO) in low-temperature flue gas,inorganic salts of cerium(Ce) and manganese(Mn) were used as precursors,then Mn-based ammonia selective catalytic reduction(NH3-SCR)/CO oxidation bi-functional nanocatalysts modified by Ce were prepared by co-precipitation,mechanical ball milling,solution combustion and sol-gel methods.The catalytic performance was evaluated on a fixed bed reactor with online mass spectrometry/chromato-graphy system.The structure of Ce-MnOx nanocatalysts were characterized and analyzed by X-ray diffraction,N2-physisorp-tion and other techniques.The results showed that the catalyst prepared by the reverse co-precipitation method had the best performance for synergistic removal of NOx and CO.At a high space velocity of 100 000 mL/(g·h),more than 85% of CO purification can be achieved above 140 ℃,more than 80% of NOx in the gas can be removed above 100 ℃,and only a slight performance degradation occurs after 20 h of operation.The active component was CeMnOx with a high specific surface area above 100 m2/g,which could adsorb more gas for reaction and showed excellent catalytic performance.
Keywords:low-temperature selective catalytic reduction  catalytic oxidation of carbon monoxide  rare earth elements  man-ganese oxide  
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