留言板

尊敬的读者、作者、审稿人, 关于本刊的投稿、审稿、编辑和出版的任何问题, 您可以本页添加留言。我们将尽快给您答复。谢谢您的支持!

姓名
邮箱
手机号码
标题
留言内容
验证码

铜基铈钴镧复合氧化物催化剂制备及其选择催化还原NO

郭锡坤,  陈都,  郭伟斌,  胡忠

downloadPDF
文章导航 > 燃料化学学报（中英文）  > 2013 >  41(05): 619-626
郭锡坤, 陈都, 郭伟斌, 胡忠. 铜基铈钴镧复合氧化物催化剂制备及其选择催化还原NO[J]. 燃料化学学报（中英文）, 2013, 41(05): 619-626.
引用本文: 郭锡坤, 陈都, 郭伟斌, 胡忠. 铜基铈钴镧复合氧化物催化剂制备及其选择催化还原NO[J]. 燃料化学学报（中英文）, 2013, 41(05): 619-626.
shu
GUO Xi-kun, CHEN Du, GUO Wei-bin, HU Zhong. Preparation of Ce-Co-La-O composite oxide supported Cu-based catalyst and its performance for selective catalytic reduction of NO[J]. Journal of Fuel Chemistry and Technology, 2013, 41(05): 619-626.
Citation: GUO Xi-kun, CHEN Du, GUO Wei-bin, HU Zhong. Preparation of Ce-Co-La-O composite oxide supported Cu-based catalyst and its performance for selective catalytic reduction of NO[J]. Journal of Fuel Chemistry and Technology, 2013, 41(05): 619-626.
shu

铜基铈钴镧复合氧化物催化剂制备及其选择催化还原NO

  • 1.

    汕头大学 理学院, 广东 汕头 515063;

  • 2.

    汕头大学 医学院第一附属医院, 广东 汕头 515041

基金项目: 广东省科技计划(2006B36702003); 汕头市重点科技计划(汕府科2011[46])。
详细信息
    通讯作者:

    郭伟斌(1974- ), 男, 硕士, 高级工程师,主要研究方向为计算机技术在化学工程中的应用研究, Tel: 0754-88282806, E-mail: gwbok@163.com。

  • 中图分类号: O643.3

Preparation of Ce-Co-La-O composite oxide supported Cu-based catalyst and its performance for selective catalytic reduction of NO

  • 1.

    College of Science, Shantou University, Shantou 515063, China;

  • 2.

    The First Affiliated Hospital of Shantou University Medical Collage, Shantou 515041, China

    摘要
  • 摘要: 采用改进的共沉淀法制备铈钴镧复合氧化物(Ce-Co-La-O)载体,等体积浸渍负载活性组分Cu,制得铜基铈钴镧复合氧化物(Cu/Ce-Co-La-O)催化剂。考察该催化剂在富氧条件下对C3H6选择性还原NO反应(C3H6-SCR)的催化性能,并且利用BET、XRD、H2-TPR、Py-IR、TG和SEM等方法,研究催化剂结构与性能的关系。实验结果表明,Co能显著增加B(Brφnsted)酸的酸量并有效提高还原能力;La能进一步增加B酸的酸量并明显提高热稳定性;Ce-Co-La-O能够形成固溶体结构,发生良好的相互协同作用。因此,Cu/Ce-Co-La-O催化剂具有良好的低温催化活性和热稳定性,最佳催化活性温度为250 ℃,NO转化率高达81.6%,600 ℃时NO转化率仍可达52.5%。
    Abstract: Ce-Co-La-O composite oxide support was prepared by a modified coprecipitation method and the Cu-based catalyst (Cu/Ce-Co-La-O) was then obtained through incipient impregnation; the performance of the Cu/Ce-Co-La-O catalyst in the selective reduction of NO with propylene in excess oxygen was investigated and the relationship between the catalyst structure and performance was explored by means of surface area measurement, X-ray diffraction (XRD), temperature-programmed reduction (H2-TPR), pyridine absorption infrared spectrum (Py-IR), thermal gravimetric analysis (TG) and scanning electron microscope (SEM). The results indicated that Co promoter can increase the amount of Brnsted acidic sites of the Cu-based catalyst and enhance its reducibility. La promoter can further increase the amount of Brnsted acidic sites and the catalyst thermal stability. Meanwhile, Ce-Co-La-O may form a sosoloid and have a synergistic effect on the catalytic performance of Cu/Ce-Co-La-O. Consequently, the Cu/Ce-Co-La-O catalyst exhibits excellent low-temperature activity and thermal stability in the selective reduction of NO; the conversion of NO reaches a maximum of 81.6% at 250 ℃ and is still 52.5% even at 600 ℃.
    • HTML全文
    • 参考文献(36)
  • HUO H, ZHANG Q, WANG M Q, STREETS D G, HE K B. Environmental implication of electric vehicles in China[J]. Environ Sci Technol, 2010, 44(13): 4856-4861.
    ARCHANA P, PRADEEP S, THOMAS R, SHAOBIN W, JIULING C, VICTOR R, ZHONGHUA Z.Catalytic reduction of NO by CO over copper-oxide supported mesoporous silica[J]. App Catal A, 2011, 409: 55-65.
    吴大旺, 张秋林, 林涛, 龚茂初, 陈耀强. Fe对 Mn/CeO2-TiO2 催化剂低温NH3选择性催化还原NO的影响[J]. 无机材料学报, 2012, 27(5): 495-500. (WU Da-wang, ZHANG Qiu-lin, LIN Tao, GONG Mao-chu, CHEN Yao-qiang. Effect of Fe on the selective catalytic reduction of NO by NH3 at low temperature over Mn/CeO2-TiO2 catalyst[J]. Journal of Inorganic Materials, 2012, 27(5): 495-500.)
    任丙南. 选择性催化还原低温催化剂的制备和表征[D]. 北京: 中国矿业大学(北京), 2011. (REN Bing-nan. Preparation and characterization of catalysts for selective catalytic reduction of NO with NH3 at low-temperature[D]. Beijing: China University of Mining and Technology(Beijing), 2011.)
    陆光. 柱层粘土催化剂上丙烯选择还原NO反应的研究[D]. 大连: 大连理工大学, 2011. (LU Guang. Selective reduction of NO with C3H6 over Cu-Ti-PILC catalysts[D]. Dalian: Dalian Uiversity of Technology, 2011.)
    IWAMOTO M, HAMADA H. Removal of nitrogen monoxide from exhaust gases through novel catalylic processes[J]. Catal Today, 1991, 10(1): 57-71.
    郭金玲, 贾美林, 照日格图, 沈岳年. Cu-Mn-O 催化剂的结构对丙烷还原 NO 反应的性能影响[J]. 化学学报, 2011, 69(5): 555-564. (GUO Jin-ling, JIA Mei-lin, ZHAORIGETU, SHEN Yue-nian. Effect of Cu-Mn-O structure on the activity for the reduction of NO by propane[J]. Acta Chimica Sinica, 2011, 69(5): 555-564.)
    张秀丽, 贺泓, 余运波. 氢气对Ag/Al2O3和Cu/Al2O3催化剂选择性催化C3H6还原NOx反应的影响[J]. 催化学报, 2007, 28(2): 117-123. (ZHANG Xiu-li, HE Hong, YU Yun-bo. Effect of H2 on selective catalytic reduction of NOx by C3H6 over Ag/Al2O3 and Cu/Al2O3 catalysts[J]. Chinese Journal of Catalysis, 2007, 28(2): 117-123.)
    王新葵, 张万生, 王爱琴, 王晓东, 杨学锋, 张涛. Au/Fe2O3/Al2O3催化剂上丙烯选择催化还原NO[J]. 催化学报, 2008, 29(6): 503-505. (WANG Xin-kui, ZHANG Wan-sheng, WANG Ai-qin, WANG Xiao-dong, YANG Xue-feng, ZHANG Tao. Selective catalytic reduction of NO with propene over Au/Fe2O3/Al2O3 catalysts[J]. Chinese Journal of Catalysis, 2008, 29(6): 503-505.)
    石新雨, 储伟. 载体及银含量等参数对丙烯选择还原 NO用银基催化剂性能的影响[J]. 天然气化工, 2009, 34(4): 47-52. (SHI Xin-yu, CHU Wei. Effect of support and Ag loading on the performance of silver-based catalysts for selective catalytic reduction of NO by C3H6[J]. Natural Gas Chemical Industry, 2009, 34(4): 47-52.)
    DORADO F, GARCFA P B, LUCAS A D, RAMOS M J, ROMERO A. Hydrocarbon selective catalytic reduction of NO over Cu/Fe-pillared clays: Diffuse reectance infrared spectroscopy studies[J]. J Mol Catal A, 2010, 332(1/2): 45-52.
    王玉东, 张豪杰, 何丹农. Pd-ZrO2/Al2O3 催化剂对丙烯选择性催化还原 NO 的催化活性研究[J]. 无机材料学报, 2011, 26(3): 311-316. (WANG Yu-dong, ZHANG Hao-jie, HE Dan-nong. Selective catalytic reduction of NO with propylene over Pd-ZrO2/Al2O3 catalysts[J]. Journal of Inorganic Materials, 2011, 26(3): 311-316.)
    YE Q, YAN L N, WANG H P, CHENG S Y, WANG D, KANG T F, DAI H X. Enhanced catalytic performance of rare earth-doped Cu/H-Sep for the selective catalytic reduction of NO with C3H6[J]. Appl Catal A, 2012, 431-432: 42-48.
    叶青, 闫立娜, 霍飞飞, 王海平, 程水源, 康天放. Fe 柱撑海泡石负载 Cu 催化剂: 结构特点及其 C3H6选择性催化还原 NO 催化性质[J]. 无机化学学报, 2012, 28(1): 103-112. (YE Qing, YAN Li-na, HUO Fei-fei, WANG Hai-ping,CHENG Shui-yuan, KANG Tian-fang. Cu-supported on Fe-pillared sepiolite: Characterization and selective catalytic reduction (SCR) of NO by propene[J]. Chinese Journal of Inorganic Chemistry, 2012, 28(1): 103-112.)
    GANEMI B, BJORNBOM E, DEMIVEL B. Zeolite Cu-ZSM-5: Material characteristics and NO decomposition[J]. Microporous Mesoporous Mater, 2000, 38(2/3): 287-300.
    LIU L J, CAO Y, SUN W J, YAO Z J, LIU B, GAO F, DONG L. Morphology and nanosize effects of ceria from different precursors on the activity for NO reduction[J]. Catal Today, 2011, 175(1): 48-54.
    BORNINGARI T, PANAGIOTIS G S.Co-doping a metal (Cr, Fe, Co, Ni, Cu, Zn, Ce, and Zr) on Mn/TiO2 catalyst and its effect on the selective reduction of NO with NH3 at low-temperatures[J]. Appl Catal B, 2011, 110: 195-206
    LIU J, ZhAO Z, CHEN Y S, XU C M, DUAN A J, JIANG G Y. Different valent ions-doped cerium oxides and their catalytic performances for soot oxidation[J]. Catal Today, 2011, 175(1): 117-123.
    CIAMBELLI P, CORBO P, MIGLIARDINI F. Potentiatities and limitations of lean de-NOx catalysts in reducing automotive exhaust emissions[J]. Catal Today, 2000, 59(3/4): 279-286.
    张存满, 张靖, 宫振华, 马建新. 介孔 MgAl2O4涂层整体式氢气燃烧催化剂的制备与表征[J]. 化学学报, 2012, 70(4): 385-391. (ZHANG Cun-man, ZHANG Jing, GONG Zhen-hua, MA Jian-xin. Synthesis and characterization of H2 combustion monolithic catalyst based on mesoporous MgAl2O4 spinel coating[J]. Acta Chimica Sinica, 2012, 70(4): 385-391.)
    万义玲, 张传辉, 郭杨龙, 郭耘, 卢冠忠. CeO2-MnOx 催化剂上氯乙烯有机废气的催化燃烧[J]. 催化学报, 2012, 33(3): 557-562. (WAN Yi-ling, ZHANG Chuan-hui, GUO Yang-long, GUO Yun, LU Guan-zhong. Catalytic combustion of vinyl chloride emission over CeO2-MnOx catalyst[J]. Chinese Journal of Catalysis, 2012, 33(3): 557-562.)
    LIOTTA L F, CARLO G D, PANTALEO G, VENEZIA A M, DEGANELLO G. Co3O4/CeO2 composite oxides for methane emissions abatement:Relationship between Co3O4-CeO2 interaction and catalytic activity[J]. AppL Catal B, 2006, 66(3/4): 217-227.
    BENJAR A M, REDDY M, KATTA L, THRIMURTHULU G. Novel nanocrystalline Ce1-xLaxO2-δ (x=0.2) solid solutions: Structural characteristics and catalytic performance[J]. Chem Mater, 2010, 22(2): 467-475.
    李想, 孟明, 姚金松, 谢亚宁, 胡天斗, 刘涛. Mn/Ce/La/Al2O3 催化剂中锰物种的精细结构研究[J]. 无机化学学报, 2007, 23(2): 211-216. (LI Xiang, MENG Ming, YAO Jin-song, XIE Ya-ning, HU Tian-dou, LIU Tao. Fine structures of manganese species in highly dispersed Mn/Ce/La/Al2O3catalysts[J]. Chinese Journal of Inorganic Chemistry, 2007, 23(2): 211-216.)
    HONG J P, CHU W, CHERNAVSKIIC P A, KHODAKOV A Y. Effects of zirconia promotion on the structure and performance of smaller and larger pore silica-supported cobalt catalysts for Fischer-Tropsch synthesis[J]. Appl Catal A, 2010, 382(1): 28-35.
    LIU J, ZHAO Z, WANG J Q, XU C M, DUAN A J, JIANG G Y, YANG Q. The highly active catalysts of nanometric CeO2-supported cobalt oxides for soot combustion[J]. Appl Catal B, 2008, 84(1/2): 185-195.
    LUO M F, MA J M, LU J Q, SONG Y P, WANG Y J. High-surface area CuO-CeO2 catalysts prepared by a surfacant-templated method for low-temperature CO oxidation[J]. J Catal, 2007, 246(1): 52-59.
    HE M, LUO M F, FANG P. Characterization of CuO species and thermal solid-solid interaction in CuO/CeO2-Al2O3 catalyst by in-situ XRD, raman spectroscopy and TPR[J]. J Rare Earths, 2006, 24(2): 188-192.
    袁文辉, 周辰辰, 李莉. 改进溶胶-凝胶法合成CeO2-ZrO2固溶体及催化性能研究[J].无机材料学报, 2010, 25(8): 820-824. (YUAN Wen-hui, ZHOU Chen-chen, LI Li. Study on catalytic properties of nano-CeO2-ZrO2: Mixed oxides prepared by modified sol-gel method[J]. Joumal of Inorganic Materials, 2010, 25(8): 820-824.)
    罗金勇, 孟明, 查宇清, 贺博, 韦世强. 高分散 CuO/CeO2-Al2O3 催化剂中铜物种的精细结构表征[J]. 无机化学学报, 2006, 22(5): 861-866. (LUO Jin-yong, MENG Ming, ZHA Yu-qing, HE Bo, WEI Shi-qiang. Characterization on the fine structures of the copper species in the highly dispersed CuO/CeO2-Al2O3 catalysts[J]. Chinese Journal of Inorganic Chemistry, 2006, 22(5): 861-866.)
    DATKA J, TUREK A M, JEHNG J M, WACHS I E. Acidic properties of supported niobium oxide catalysts: An infrared spectroscopy investigation[J]. J Catal, 1992, 135(1): 186-199.
    尹元根. 多相催化剂的研究方法[M]. 北京: 化学工业出版社, 1988, 582-584. (YIN Yuan-gen. Research methods of heterogeneous catalysts[M]. Beijing: Chemical Industry Press, 1988, 582-584.)
    林绮纯, 林维明, 郝吉明, 李俊华, 傅立新. 载体酸性对铜基交联黏土催化剂上C3H6选择性催化还原NO反应的影响[J].高等学校化学学报, 2006, 27(1): 85-88. (LIN Qi-chun, LIN Wei-ming, HAO Ji-ming, LI Jun-hua, FU Li-xin. Effect of support acidity on selective catalytic reduction of NO by C3H6 over Cu-based pillared clay catalyst[J]. Chemical Journal of Chinese Universities, 2006, 27(1): 85-88.)
    谭宇新. 贫燃条件下汽车尾气净化催化剂的研究. 广州: 华南理工大学, 2000. (TAN Yu-xin. Study on automobile exhaust catalyst under lean-burn conditions. Guangzhou:South China University of Technology, 2000.)
    YANG R T, THARAPPIWATTANANON N,LONG R Q. Lon-exchanged pillared clays for selective catalytic reduction of NO by ethylene in thepresence of oxygen[J]. Appl Catal B, 1998, 19(3/4): 289-304.
    TROVARELLI A, BOARO M, ROCCHINI E, LEITENBURG C, DOLCETTI G. Some recent developments in the characterization of ceria-based catalysts[J]. J Alloys Comp, 2001, 323-324: 584-591.
    • 相关文章
    • 施引文献
  • 资源附件(0)
  • 加载中
WeChat 点击查看大图
计量
  • 文章访问数:  1777
  • HTML全文浏览量:  18
  • PDF下载量:  584
  • 被引次数: 0
出版历程
  • 收稿日期:  2012-11-01
  • 修回日期:  2013-01-19
  • 刊出日期:  2013-05-30

目录

    /

    返回文章
    返回
    友情链接： 新型炭材料 中国科学院 中国知网 万方论文查重系统

    主办单位：中国科学院山西煤炭化学研究所 中国化学会主编：房倚天

    电子邮件：rlhx@sxicc.ac.cn

    版权所有 © 《燃料化学学报（中英文）》编辑部 本系统由 北京仁和汇智信息技术有限公司 开发    百度统计

    x 关闭 永久关闭

    2023年《燃料化学学报（中英文）》评优结果公布！