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 ›› 2014, Vol. 46 ›› Issue (7): 71-.

• 论文 • 上一篇    下一篇

镧系金属掺杂MCM-41的合成、表征及其脱硝性能研究

吴其胜 1,陈亦林 2   

  1. 1.盐城工学院,江苏盐城 224000;2.江苏大学材料学院
  • 出版日期:2014-07-10 发布日期:2014-07-07

Synthesis, characterization,and de-NOx performance  of lanthanum-doped MCM-41

Wu Qisheng1,Chen Yilin2   

  1. 1.Yancheng Institute of Technology,Yancheng 224000,China;2.School of Materials Science & Engineering,Jiangsu University
  • Online:2014-07-10 Published:2014-07-07

摘要: 以正硅酸乙酯、硝酸镧、硝酸铈为原料,十六烷基三甲基溴化铵作模板剂,水热条件下合成镧、铈掺杂介孔分子筛。采用 XRD、FT-IR和氮气吸附脱附等对镧系金属掺杂MCM-41 进行表征,并以氨为还原剂研究其选择性催化还原一氧化氮活性以及反应条件(包括镧系掺量、反应温度、空速、氨氮比等)对催化性能的影响。本文旨在掺杂镧系金属提高分子筛的脱硝性能。镧系掺杂的分子筛改变了骨架增强了反应活性,稀土金属的高电荷密度使分子筛催化活性提高。结果表明,镧系金属镧、铈成功进入MCM-41 介孔材料的骨架内并保持有序的六方介孔结构,随着镧系掺杂量的增加,介孔有序性降低。当n(镧系金属)/n(硅)=0.04 、空速为4 000 h-1、n(氨气)/n(一氧化氮)为1 时 Ln-MCM-41催化剂在350 ℃反应时能保持较高活性。镧系掺杂的介孔分子筛能更有效地提高催化性能。

关键词: 介孔分子筛, Ln-MCM-41, 选择性催化还原

Abstract: Using  tetraethylorthosilicate(TEOS),lanthanum  nitrate,and cerium nitrate as raw materials and cetyl-trimethyl- ammonium bromide(CTMAB) as the template agent,MCM-41 mesoporous molecular sieves were synthesized with La or Ce incorporated in the framework under hydrothermal conditions.The structure and the state of Ln-doped MCM-41 were characterized by the analysis of XRD,FT-IR,and nitrogen adsorption-desorption.Its activities of selective catalytic reduction of NO with ammonia as reductant as well as the influences  of lanthanide doping content,temperature,space velocity and n(NH3)/ n(NO) on catalytic performance were investigated.The aim of this work was to incorporate lanthanide to improve de-NOx performance of molecular sieves.Ln-MCM-41 changed skeleton structure,which could increase the number of lattice defects to improve reactivity and pore surface adsorption due to exchangeability of rare earth metal ions.The result  indicated that La and Ce were introduced into the framework of MCM-41 mesoporous materials and maintained an orderly hexagonal pore structure.The order degree declined with the increase of La and Ce doping amounts.Ln-MCM-41 could maintain high activity at 350 ℃ when n(Ln)/n(Si)=0.04,space velocity  was 4 000 h-1 ,and n(NH3)/n(NO)=1∶1.The lanthanide-doped MCM-41 molecular sieves will be helpful in promoting catalyst activity effectively.

Key words: mesoporous molecular sieves, Ln-MCM-41, selective catalytic reduction

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