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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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  • 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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