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铜前驱体对Cu/SSZ-13催化剂NH3选择催化还原NO性能的影响
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作者单位:

1.桂林理工大学;2.广西玉柴机器股份有限公司

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O 643

基金项目:

国家自然科学基金资助项目(11564010);广西创新驱动重大专项金资助项目(AA18118010);广西自然科学基金(2020JJB120022);有色金属及材料加工新技术教育部重点实验室开放基金(20AA-13)


Effects of copper precursors on catalytic performance of Cu/SSZ-13 catalyst for NH3 selective catalytic reduction of NO
Author:
Affiliation:

1.桂林理工大学;2.Yuchai Engineering Research Institute,Guangxi Yuchai Machinery Co,Ltd,Nanning;3.School of Materials Science and Engineering,Guilin University of Technology,Guilin

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    摘要:

    采用离子交换法,分别以乙酸铜、氯化铜、硝酸铜和硫酸铜为前驱体制备了4种铜物种含量几乎相同的Cu/SSZ-13分子筛催化剂。探究了前驱体对NH3选择性催化还原NO(NH3-SCR)的影响,并通过XRD,ICP,N2吸-脱附,SEM,H2-TPR,XPS,NH3-TPD等表征分析对样品的物化性质进行了系统探究。催化活性结果表明,铜前驱体对Cu/SSZ-13分子筛中低温范围的氨选择性催化还原性能具有显著差异。其中催化剂起燃温度T50(转化率 ≥ 50 %时的温度)的高低顺序为Cu(乙酸铜)/SSZ-13 < Cu(氯化铜)/SSZ-13 < Cu(硫酸铜)/SSZ-13 < Cu(硝酸铜)/SSZ-13。表征结果表明,铜前驱体会影响分子筛催化剂中铜物种的分布和数量以及酸性。以乙酸铜为前驱体制备的Cu/SSZ-13催化剂具有最多的孤立Cu2+以及强L酸位数量,有助于样品低温段NH3-SCR催化反应的进行。

    Abstract:

    Cu/SSZ-13 catalysts with the nearly same content of copper species were prepared by ion exchange technology with copper acetate, copper chloride, copper nitrate and copper sulfate as precursors, respectively. The effects of copper source on NH3 selective catalytic reduction (NH3-SCR) were probed detailedly. The physicochemical properties of the catalysts were investigated by XRD, ICP, N2 absorption-desorption, SEM, H2-TPR, XPS and NH3-TPD. The results of activity test display that the performance of Cu/SSZ-13 zeolite for ammonia selective catalytic reduction at low temperature is significantly different. The light off temperature T50 (the temperature when conversion efficiency ≥ 50 %) follows the order of Cu (copper acetate) / SSZ-13 < Cu (copper chloride) / SSZ-13 < Cu (copper sulfate) / SSZ-13 < Cu (copper nitrate) / SSZ-13. The characterization results manifest that the distribution and quantity of copper species and the acidity of zeolite catalysts are affected by copper source. The Cu/SSZ-13 catalyst prepared with copper acetate as precursor possesses the largest number of isolated Cu2+ and strong L acid sites, which are conducive to the low-temperature NH3-SCR reaction.

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周硕,王辉,王苏宁,刘来君.铜前驱体对Cu/SSZ-13催化剂NH3选择催化还原NO性能的影响[J].稀有金属材料与工程,2022,51(2):669~674.[Zhou Shuo, Wang Hui, Wang Suning, Liu Laijun. Effects of copper precursors on catalytic performance of Cu/SSZ-13 catalyst for NH3 selective catalytic reduction of NO[J]. Rare Metal Materials and Engineering,2022,51(2):669~674.]
DOI:10.12442/j. issn.1002-185X.20210154

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  • 收稿日期:2021-02-25
  • 最后修改日期:2021-03-25
  • 录用日期:2021-03-25
  • 在线发布日期: 2022-03-09
  • 出版日期: 2022-02-28