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

SO2和H2O对CeO2/TiO2/堇青石催化剂选择催化还原NOx性能的影响

束韫,  张凡,  王洪昌,  朱金伟

downloadPDF
文章导航 > 燃料化学学报（中英文）  > 2014 >  42(09): 1111-1118
束韫, 张凡, 王洪昌, 朱金伟. SO2和H2O对CeO2/TiO2/堇青石催化剂选择催化还原NOx性能的影响[J]. 燃料化学学报（中英文）, 2014, 42(09): 1111-1118.
引用本文: 束韫, 张凡, 王洪昌, 朱金伟. SO2和H2O对CeO2/TiO2/堇青石催化剂选择催化还原NOx性能的影响[J]. 燃料化学学报（中英文）, 2014, 42(09): 1111-1118.
shu
SHU Yun, ZHANG Fan, WANG Hong-chang, ZHU Jin-wei. Influence of SO2 and H2O on the selective catalytic reduction of NOx over CeO2/TiO2/cordierite catalyst[J]. Journal of Fuel Chemistry and Technology, 2014, 42(09): 1111-1118.
Citation: SHU Yun, ZHANG Fan, WANG Hong-chang, ZHU Jin-wei. Influence of SO2 and H2O on the selective catalytic reduction of NOx over CeO2/TiO2/cordierite catalyst[J]. Journal of Fuel Chemistry and Technology, 2014, 42(09): 1111-1118.
shu

SO2和H2O对CeO2/TiO2/堇青石催化剂选择催化还原NOx性能的影响

  • 中国环境科学研究院 大气污染控制技术研究中心, 北京 100012

基金项目: 国家自然科学基金（2012AA062505）；中央级公益性科研院所基本科研业务专项（2013-YSKY-01）。
详细信息
    通讯作者:

    张凡，研究员，Tel：010-84915188，E-mail：zhangfan5188@vip.sina.com。

  • 中图分类号: X51

Influence of SO2 and H2O on the selective catalytic reduction of NOx over CeO2/TiO2/cordierite catalyst

  • Research Center of Air Pollution Control Technology, Chinese Research Academy of Environmental Sciences, Beijing 100012, China

    摘要
  • 摘要: 采用浸渍法制备了以堇青石为基底、氧化铈为活性组分的整体式脱硝催化剂CeO2/TiO2/堇青石催化剂。通过与商业钒基催化剂（V2O5-WO3/TiO2/堇青石）的对比研究发现，CeO2/TiO2/堇青石催化剂表现出了优良的抗硫抗水性能，经过30 h抗硫抗水实验，CeO2/TiO2/堇青石催化剂的氮氧化物转化率仍能保持在70%以上，仅下降了5%。BET、XRD、FT-IR和TG表征结果表明，在含硫含水气氛中反应时，CeO2/TiO2/堇青石和V2O5-WO3/TiO2/堇青石催化剂表面均有硫酸铵盐的生成，且前者的生成量明显低于后者。NH3-DRIFT分析结果表明，在含硫含水气氛中两种催化剂表面Brønsted酸性都被增强，而Lewis酸性有所减弱。进一步的XPS分析结果表明，烟气中的SO2+H2O会使催化剂表面Ce4+向Ce3+发生转化，从而导致化学吸附氧含量增加，这是CeO2/TiO2/堇青石催化剂具有优良抗硫抗水性能的重要原因。
    Abstract: A monolithic CeO2/TiO2/cordierite deNOx catalyst was prepared by an impregnation method, with cordierite as the substrate and CeO2 as the active component. The CeO2/TiO2/cordierite catalyst exhibits excellent resistance against SO2 and H2O in the selective catalytic reduction (SCR) of NOx with NH3, compared with the commercial vanadium-based catalyst (V2O5-WO3/TiO2/cordierite); the CeO2/TiO2/cordierite catalyst gives a conversion of NOx above 70% after 30 h resistance test against SO2+H2O, only declined by 5%. BET, XRD, FT-IR and TG results indicated that ammonium sulfate is formed on the surface of both CeO2/TiO2/cordierite and V2O5-WO3/TiO2/cordierite catalysts during the SCR reaction in the presence of SO2 and H2O, but on the former, the amount of ammonium sulfate deposited is much less. NH3-DRIFT results suggested that the surface Brønsted acidity is strengthened, whereas the surface Lewis acidity is weakened during the SCR reaction in the presence of SO2 and H2O. XPS results further displayed that SO2+H2O in flue gas may induce a reduction of Ce from Ce4+ to Ce3+ on CeO2/TiO2/cordierite catalyst, resulting in an increase of the chemisorbed oxygen amount, which contributes to the excellent resistance of the CeO2/TiO2/cordierite catalyst against SO2 and H2O during the SCR reaction.
    • HTML全文
    • 参考文献(32)
  • BUSCA G, LIETTI L, RAMIS G, BERTI F. Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: A review[J]. Appl Catal B: Environ, 1998, 18(1/2): 1-36.
    沈伯雄, 熊丽仙, 刘亭, 王静, 田晓娟. 纳米负载型V2O5-WO3/TiO2催化剂碱中毒及再生研究[J]. 燃料化学学报, 2010, 38(1): 85-90. (SHEN Bo-xiong, XIONG Li-xian, LIU Ting, WANG Jing, TIAN Xiao-juan. Alkali deactivation and regeneration of nano V2O5-WO3/TiO2 catalysts[J]. Journal of Fuel Chemistry and Technology, 2010, 38(1): 85-90.)
    DUNN J P, KOPPULA P R, STENGER H G. Oxidation of sulfur dioxide to sulfur trioxide over supported vanadia catalysts[J]. Appl Catal B: Environ, 1998, 19(2): 103-117.
    BOGER T, HEIBEL A K, SORENSEN C M. Monolithic catalysts for the chemical industry[J]. Ind Eng Chem Res, 2004, 43(16): 4602-4614.
    LONG R Q, YANG R T. Superior Fe-ZSM-5 catalyst for selective catalytic reduction of nitric oxide by ammonia[J]. J Am Chem Soc, 1999, 121(23): 5595-5596.
    XU W Q, YU Y B, ZHANG C B, HE H. Selective catalytic reduction of NO by NH3 over a Ce/TiO2 catalyst[J]. Catal Commun, 2008, 9: 1453-1457.
    沈伯雄, 郭宾彬, 史展亮, 吴春飞, 梁材. CeO2/ACF的低温SCR烟气脱硝性能研究[J]. 燃料化学学报, 2007, 35(1): 125-128. (CHEN Bo-xiong, GUO Bing-bing, SHI Zhang-liang, WU Chun-fei, LIANG Cai. Selective catalytic reduction of NO over carbon nanotubes supported CeO2[J]. Journal of Fuel Chemistry and Technology, 2007, 35(1): 125-128.)
    ZHU Z P, LIU Z Y, NIU H X, LIU S J. Promoting effect of SO2 on activated carbon-supported vanadia catalyst for NO reduction by NH3 at low temperatures[J]. J Catal, 1999, 187(1): 245-248.
    LONG R Q, YANG R T. Selective catalytic reduction of nitrogen oxides by ammonia over Fe3+-exchanged TiO2-pillared clay catalysts[J]. J Catal, 1999, 186(2): 254-268.
    HOU Y Q, HUANG Z G, GUO S J. Effect of SO2 on V2O5/ACF catalysts for NO reduction with NH3 at low temperature[J]. Catal Commun, 2009, 10(11): 1538-1541.
    CHEN J, YANG R T. Selective catalytic reduction of NO with NH3 on SO2-4/TiO2 super acid catalyst[J]. J Catal, 1993, 139(1): 277-288.
    LONG R Q, Chang M, YANG R T. Enhancement of activities by sulfation on Fe-exchanged TiO2-pillared clay for selective catalytic reduction of NO by ammonia[J]. Appl Catal B: Environ, 2001, 33(2): 97-107.
    GARCÍA B E, PINILLA J L, LÁZARO M J, MOLINER R. Role of sulphates on the mechanism of NH3-SCR of NO at low temperatures over presulphated vanadium supported on carbon-coated monoliths[J]. J Catal, 2005, 233(1): 166-175.
    ROY S, VISWANATH B, HEGDE M S. Low-temperature selective catalytic reduction of NO with NH3 over Ti0.9M0.1O2-δ (M=Cr, Mn, Fe, Co, Cu)[J]. J Phys Chem C, 2008, 112(15): 6002-6112.
    金瑞奔. 负载型Mn-Ce系列低温SCR脱硝催化剂制备、反应机理及抗硫性能研究. 杭州: 浙江大学, 2010. (JIN Rui-ben. Study on the supported Mn-Ce low temperature SCR DeNOx catalysts: Preparation, reaction mechanism and SO2 tolerance. Hangzhou: Zhejiang University, 2010.)
    HUANG Z, ZHU Z P, LIU Z Y. Combined effect of H2O and SO2 on V2O5/AC catalysts for NO reduction with ammonia at lower temperatures[J]. Appl Catal B: Environ, 2002, 39(4): 361-368.
    FREDERICKSON L D, HAUSEN D M. Infrared spectra-structure correlation study of vanadium-oxygen compounds[J]. Anal Chem, 1963, 35(8): 818-824.
    TOPSØE N Y. Mechanism of the selective catalytic reduction of nitric-oxide by ammonia elucidated by in situ on-line fourier transform infrared spectroscopy[J]. Science, 1994, 265(5176): 1217-1219.
    TAKAGI M, KAWAI T, SOMA M. Mechanism of catalytic reaction between NO and NH3 on V2O5 in the presence of oxygen[J]. J Phys Chem, 1976, 80(4): 430-437.
    MARBÁN G, FUERTES T. Mechanism of low temperature selective catalytic reduction of NO with NH3 over carbon-supported Mn3O4-role of surface NH3 species: SCR mechanism[J]. J Catal, 2004, 226(1): 138-155.
    HUANG J H, TONG Z Q, HUANG Y. Selective catalytic reduction of NO with NH3 at low temperatures over iron and manganese oxides supported on mesoporous silica[J]. Appl Catal B: Environ, 2008, 78(3/4): 309-314.
    CHEN L, LI J H, GE M F. DRIFT study on cerium-tungsten titiania catalyst for selective catalytic reduction of NOx with NH3[J]. Environ Sci Technol, 2010, 44(24): 9590-9598.
    GUAN B, LIN H, ZHU L. Selective catalytic reduction of NOx with NH3 over Mn, Ce substitution Ti0.9V0.1O2-δ nanocomposites catalysts prepared by self-propagating high-temperature synthesis method[J]. J Phys Chem C, 2011, 115(26): 12850-12863.
    DAMYANOVA S, PEREZ C A, SCHMAL M. Characterization of ceria-coated alumina carrier[J]. Appl Catal A: Gen, 2002, 234(1/2): 271-282.
    LI Y, ZHANG B C, TANG X L. Hydrogen production from methane decomposition over Ni/CeO2 catalysts[J]. Catal Commun, 2006, 7(6): 380-386.
    LIU F D, HE H, ASAKURA K. Influence of sulfation on iron titanate catalyst for the selective catalytic reduction of NOx with NH3[J]. Appl Catal B: Environ, 2011, 103(3/4): 369-377.
    PEÑA D A, UPHADE B S, REDDY E P. Identification of surface species on titania supported manganese, chromium, and copper oxide low-temperature SCR catalysts[J]. J Phys Chem B, 2004, 108(28): 9927-9936.
    CENTENO M A, CARRIZOSA I, ODRIOZOLA J A. NO-NH3 co-adsorption on vanadia/titania catalysts: Determination of the reduction degree of vanadium[J]. Appl Catal B: Environ, 2001, 29(4): 307-314.
    WAQIF M, BAZIN P, SAUR O. Study of ceria sulfation[J]. Appl Catal B: Environ, 1997, 11(2): 193-205.
    PÃRVULESCU V I, BOGHOSIAN S, PÃRVULESCU V, JUNG S M, GRANGE P. Selective catalytic reduction of NO with NH3 over mesoporous V2O5-TiO2-SiO2 catalyst[J]. J Catal, 2003, 217(1): 172-185.
    NOLAN M. Molecular adsorption on the doped(110) ceria surface[J]. J Phys Chem C, 2009, 113(6): 2425-2432.
    LIETTI L. Reactivity of V2O5-WO3/TiO2 de-NOx catalysts by transient methods[J]. Appl Catal B: Environ, 1996, 10(4): 281-297.
    • 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:  558
  • HTML全文浏览量:  21
  • PDF下载量:  808
  • 被引次数: 0
出版历程
  • 收稿日期:  2014-04-11
  • 修回日期:  2014-06-13
  • 刊出日期:  2014-09-30

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！