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铁源对Fe/ZSM-5催化剂氨选择性催化还原NO的影响

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郑昌坤, 韩帅, 曹昱, 刘心悦, 蔡宸珉, 李乐之, 叶青. 铁源对Fe/ZSM-5催化剂氨选择性催化还原NO的影响[J]. 环境化学, 2019, 38(4): 887-893. doi: 10.7524/j.issn.0254-6108.2018051704
引用本文: 郑昌坤, 韩帅, 曹昱, 刘心悦, 蔡宸珉, 李乐之, 叶青. 铁源对Fe/ZSM-5催化剂氨选择性催化还原NO的影响[J]. 环境化学, 2019, 38(4): 887-893. doi: 10.7524/j.issn.0254-6108.2018051704
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ZHENG Changkun, HAN Shuai, CAO Yu, LIU Xinyue, CAI Chenmin, LI Lezhi, YE Qing. Effects of Fe sources on catalytic performance of Fe/ZSM-5 for the selective catalytic reduction of NO with NH3[J]. Environmental Chemistry, 2019, 38(4): 887-893. doi: 10.7524/j.issn.0254-6108.2018051704
Citation: ZHENG Changkun, HAN Shuai, CAO Yu, LIU Xinyue, CAI Chenmin, LI Lezhi, YE Qing. Effects of Fe sources on catalytic performance of Fe/ZSM-5 for the selective catalytic reduction of NO with NH3[J]. Environmental Chemistry, 2019, 38(4): 887-893. doi: 10.7524/j.issn.0254-6108.2018051704
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铁源对Fe/ZSM-5催化剂氨选择性催化还原NO的影响

  • 1.

    北京工业大学区域大气复合污染防治北京市重点实验室, 北京, 100124

  • 基金项目:

    国家自然科学基金（21277008，20777005）和北京市自然科学基金（8082008）资助.

Effects of Fe sources on catalytic performance of Fe/ZSM-5 for the selective catalytic reduction of NO with NH3

  • 1.

    Key Laboratory of Beijing on Regional Air Pollution Control, Beijing University of Technology, Beijing, 100124, China

  • Fund Project: Supported by the National Natural Science Foundation of China (21277008,20777005) and Natural Science Foundation of Beijing (8082008).

  • 摘要: 采用浸渍法，在相同的铁含量条件下，以硝酸铁、氯化亚铁、硫酸亚铁为前驱体制备了3种不同铁源Fe/ZSM-5分子筛催化剂.研究了铁源对Fe/ZSM-5催化剂NH3-SCR活性的影响，并采用X射线衍射（XRD）、比表面积和孔结构（BET）、X射线光电子能谱（XPS）、氢气程序升温还原（H2-TPR）及氨程序升温脱附（NH3-TPD）等表征手段对催化剂的结构和理化性质进行测定.结果表明，不同的铁源对Fe/ZSM-5催化剂低温段（低于350℃）的NH3-SCR催化性能影响较大，其低温活性顺序为：Fe（Cl）/ZSM-5 > Fe（S）/ZSM-5 > Fe（N）/ZSM-5.以氯化亚铁为铁源的Fe（Cl）/ZSM-5催化剂取得最佳的NH3-SCR催化活性，在233℃时NO转化率达到90%.表征结果表明，样品Fe（Cl）/ZSM-5中形成了最多的孤立Fe3+物种及中酸位数量.孤立Fe3+物种有利于增强Fe/ZSM-5催化剂的低温还原性能，改性过程中形成的中等强度酸性位有利于提高催化剂低温NH3-SCR催化性能.
    Abstract: With the same iron content, three types of Fe/ZSM-5 molecular sieve catalysts with different iron sources (ferrous nitrate, ferrous chloride and ferrous sulfate) were prepared by impregnation method. The effects of iron sources on the NH3-SCR performance of Fe/ZSM-5 catalysts were investigated and the physicochemical properties of the samples were characterized by XRD, BET, XPS, H2-TPR and NH3-TPD techniques. The results indicated that iron source had a great influence on the low-temperature (3-SCR performance of Fe/ZSM-5 catalysts. The order of activity of those catalysts at low temperatures was as follows:Fe(Cl)/ZSM-5 > Fe(S)/ZSM-5 > Fe(N)/ZSM-5. The sample with ferrous chloride as precursor obtained the best NH3-SCR activity, and the NO conversion of Fe(Cl)/ZSM-5 reached 90% at 233℃. Characterization result showed that the Fe(Cl)/ZSM-5 sample possessed the largest amount of isolated Fe3+ species and moderately acidic sites. Isolated Fe3+ species is beneficial to enhance the low temperature reduction performance of the Fe/ZSM-5 catalyst, and moderately acidic sites are favorable for the low-temperature catalytic performance.
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  • [1] JIANG S Y,ZHOU R X. Ce doping effect on performance of the Fe/β catalyst for NOx reduction by NH3[J]. Fuel processing technology,2015,133:220-226.
    [2] KIM Y J,KWON H J,ILJEONG H,et al. Mn-Fe/ZSM5 as a low-temperature SCR catalyst to remove NOx from diesel engine exhaust[J]. Applied catalysis B: Bnvironmental,2012,126:9-21.
    [3] 孙亮,许悠佳,曹青青,等. 氧化锰基催化剂低温NH3选择性还原NOx反应及其机理[J]. 化学进展,2010,22(10):1882-1890.

    SUN L,XU Y,CAO Q,et al. Reactions and mechanisms of low-temperature selective catalytic reduction of NOx by NH3 over manganese oxide-based catalysts[J]. Progress in Chemistry,2010,22(10):1882-1890 (in Chinese).

    [4] DING S P,LIU F D,SHI X Y,et al. Promotional effect of Nb additive on the activity and hydrothermal stability for the selective catalytic reduction of NOx with NH3 over CeZrOx catalyst[J]. Applied catalysis B: Environmental,2016,180:766-774.
    [5] XIA Y,ZHAN W,GUO Y,et al. Fe-Beta zeolite for selective catalytic reduction of NOx with NH3: Influence of Fe content[J]. Chinese Journal of Catalysis,2016,37(12):2069-2078.
    [6] ROMERO-SAEZ M, DIVAKAR D, ARANZABAL A, et al. Catalytic oxidation of trichloroethylene over Fe-ZSM-5: Influence of the preparation method on the iron species and the catalytic behavior[J]. Applied catalysis B: Environmental,2016,180:210-218.
    [7] GAO F,KOLLAR M,KUKKADAPU R K,et al. Fe/SSZ-13 as an NH3-SCR catalyst: A reaction kinetics and FTIR/Mossbauer spectroscopic study[J]. Applied Catalysis B: Environmental,2015,164:407-419.
    [8] 石晓燕,刘福东,单文坡,等. 水热老化对不同方法制备的Fe-ZSM-5用于NH3选择性催化还原NOx的影响[J]. 催化学报,2012,33(3):454-464.

    SHI X Y,LIU F D,SHAN W P,et al. Hydrothermal deactivation of Fe/ZSM-5 prepared by different methods for the selective catalytic reduction of NOx with NH3[J]. Chinese Journal of Catalysis,2012,33(3):454-464 (in Chinese).

    [9] GAO F,ZHENG Y,KUKKADAPU R K,et al. Iron loading effects in Fe/SSZ-13 NH3-SCR catalysts: Nature of the Fe ions and structure-function relationships[J]. ACS Catalysis,2016,6:2939-2954.
    [10] BRANDENBERGER S,KROCHER O,TISSLER A,et al. The determination of the activities of different iron species in Fe-ZSM-5 for SCR of NO by NH3[J]. Applied catalysis B: Environmental,2010,95:348-357.
    [11] BIN F,SONG C L,LV G,et al. Selective catalytic reduction of nitric oxide with ammonia over zirconium-doped copper/ZSM-5 catalysts[J]. Applied Catalysis B: Environmental,2014,150-151:532-543.
    [12] PANG L,FAN C,SHAO L,et al. The Ce doping Cu/ZSM-5 as a new superior catalyst to remove NO from diesel engine exhaust[J]. Chemical Engineering Journal,2014,253:394-401.
    [13] 王坤鹏,宋崇林,宾峰,等. Cu/ZSM-5分子筛催化剂SCR催化性能[J]. 燃烧科学与技术,2012,18:73-78. WANG K P,SONG C L,BIN F,et al. Performance of selective catalytic reduction over Cu/ZSM-5

    zeolite catalysts[J]. Journal of Combustion Science and Technology,2012,18:73-78 (in Chinese).

    [14] BUKHTIYAROVA G A,BUKHTIYAROVA V I,SAKAEVA N S,et al. XPS study of the silica-supported Fe-containing catalysts for deep or partial H2S oxidation[J]. Journal of Molecular Catalysis A: Chemical,2000,158:251-255.
    [15] ATES A. Characteristics of Fe-exchanged natural zeolites for the decomposition of N2O and its selective catalytic reduction with NH3[J]. Applied catalysis B: Environmental,2007,76:282-290.
    [16] ATES A,REITZMANN A,WATERS G. Surface oxygen generated upon N2O activation on iron containing ZSM-5 type zeolites with different elemental composition[J]. Applied Catalysis B: Environmental,2012,119-120:329-339.
    [17] YUAN E,WU G,DAI W,et al. One-pot construction of Fe/ZSM-5 zeolites for the selective catalytic reduction of nitrogen oxides by ammonia[J]. Catalysis Science and Technology,2017,7:3036-3044.
    [18] QI G,YANG R T. Selective catalytic oxidation (SCO) of ammonia to nitrogen over Fe/ZSM-5 catalysts[J]. Applied Catalysis A: General,2005,287(1):25-33.
    [19] SHI X,HE H,XIE L. The effect of Fe species distribution and acidity of Fe-ZSM-5 on the hydrothermal stability and SO2 and hydrocarbons durability in NH3-SCR reaction[J]. Chinese Journal of Catalysis,2015,36:649-656.
    [20] CHEN P,JABLONSKA M,WEIDE P,et al. Formation and effect of NH4+ intermediates in NH3-SCR over Fe-ZSM-5 zeolite catalysts[J]. American Chemical Society,2016,6:7696-7700.
    [21] DOU B J,LV G,WANG C,et al. Cerium doped copper/ZSM-5 catalysts used for the catalytic reduction of nitrogen oxide with ammonia[J]. Chemical Engineering Journal,2015,270(2):549-556.
    [22] BRANDENBERGER S,KROCHER O,WOKAUN A,et al. The role of Brønsted acidity in the selective catalytic reduction of NO with ammonia over Fe-ZSM-5[J]. Journal of Catalysis,2009,268:297-306.
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  • 收稿日期:  2018-05-17
  • 刊出日期:  2019-04-15

铁源对Fe/ZSM-5催化剂氨选择性催化还原NO的影响

  • 1. 北京工业大学区域大气复合污染防治北京市重点实验室, 北京, 100124
  • 收稿日期:  2018-05-17
基金项目:

国家自然科学基金（21277008，20777005）和北京市自然科学基金（8082008）资助.

摘要: 采用浸渍法，在相同的铁含量条件下，以硝酸铁、氯化亚铁、硫酸亚铁为前驱体制备了3种不同铁源Fe/ZSM-5分子筛催化剂.研究了铁源对Fe/ZSM-5催化剂NH3-SCR活性的影响，并采用X射线衍射（XRD）、比表面积和孔结构（BET）、X射线光电子能谱（XPS）、氢气程序升温还原（H2-TPR）及氨程序升温脱附（NH3-TPD）等表征手段对催化剂的结构和理化性质进行测定.结果表明，不同的铁源对Fe/ZSM-5催化剂低温段（低于350℃）的NH3-SCR催化性能影响较大，其低温活性顺序为：Fe（Cl）/ZSM-5 > Fe（S）/ZSM-5 > Fe（N）/ZSM-5.以氯化亚铁为铁源的Fe（Cl）/ZSM-5催化剂取得最佳的NH3-SCR催化活性，在233℃时NO转化率达到90%.表征结果表明，样品Fe（Cl）/ZSM-5中形成了最多的孤立Fe3+物种及中酸位数量.孤立Fe3+物种有利于增强Fe/ZSM-5催化剂的低温还原性能，改性过程中形成的中等强度酸性位有利于提高催化剂低温NH3-SCR催化性能.

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