无机盐工业
主管:中海油天津化工研究设计院有限公司
主办:中海油天津化工研究设计院有限公司
   中海油炼油化工科学研究院(北京)有限公司
   中国化工学会无机酸碱盐专业委员会
ISSN 1006-4990 CN 12-1069/TQ

无机盐工业 ›› 2021, Vol. 53 ›› Issue (12): 35-42.doi: 10.19964/j.issn.1006-4990.2021-0644

• 无机新型材料——碳资源转化与利用 • 上一篇    下一篇

Ce-MnOx低温净化氮氧化物和一氧化碳的催化性能研究

韩新宇1,2(),刘凯杰1,2(),边梦瑶1,2,张一波1,2,3(),杨向光1,2,3   

  1. 1.中国科学技术大学,安徽合肥 230026
    2.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
  • 收稿日期:2021-10-24 出版日期:2021-12-10 发布日期:2021-12-16
  • 作者简介:韩新宇(1998— ),男,研究方向为固定源烟气脱硝催化剂的制备、改性及机理研究;E-mail: xinyuhan@mail.ustc.edu.cn
  • 基金资助:
    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)

Catalytic performance study of Ce-MnOx for low-temperature purification of nitrogen oxides and carbon monoxide

HAN Xinyu1,2(),LIU Kaijie1,2(),BIAN Mengyao1,2,ZHANG Yibo1,2,3(),YANG Xiangguang1,2,3   

  1. 1. University of Science and Technology of China,Hefei 230026,China
    2. Ganjiang Innovation Academy,Chinese Academy of Sciences
    3. Changchun Institute of Applied Chemistry,Chinese Academy of Sciences
  • Received:2021-10-24 Published:2021-12-10 Online:2021-12-16

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

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.

Key words: low-temperature selective catalytic reduction, catalytic oxidation of carbon monoxide, rare earth elements, man-ganese oxide

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