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Cu-SAPO-44选择性催化丙烯还原NO性能研究

张恒 周皞 温妮妮 王旭瑞 徐璐 苏亚欣

张恒, 周皞, 温妮妮, 王旭瑞, 徐璐, 苏亚欣. Cu-SAPO-44选择性催化丙烯还原NO性能研究[J]. 燃料化学学报, 2022, 50(8): 1064-1074. doi: 10.19906/j.cnki.JFCT.2022012
引用本文: 张恒, 周皞, 温妮妮, 王旭瑞, 徐璐, 苏亚欣. Cu-SAPO-44选择性催化丙烯还原NO性能研究[J]. 燃料化学学报, 2022, 50(8): 1064-1074. doi: 10.19906/j.cnki.JFCT.2022012
ZHANG Heng, ZHOU Hao, WEN Ni-ni, WANG Xu-rui, XU Lu, SU Ya-xin. Selective catalytic reduction of nitric oxide with propylene over one-step synthesized Cu-SAPO-44 catalysts[J]. Journal of Fuel Chemistry and Technology, 2022, 50(8): 1064-1074. doi: 10.19906/j.cnki.JFCT.2022012
Citation: ZHANG Heng, ZHOU Hao, WEN Ni-ni, WANG Xu-rui, XU Lu, SU Ya-xin. Selective catalytic reduction of nitric oxide with propylene over one-step synthesized Cu-SAPO-44 catalysts[J]. Journal of Fuel Chemistry and Technology, 2022, 50(8): 1064-1074. doi: 10.19906/j.cnki.JFCT.2022012

Cu-SAPO-44选择性催化丙烯还原NO性能研究

doi: 10.19906/j.cnki.JFCT.2022012
基金项目: 江苏省自然科学基金(BK20181161),国家自然科学基金(51278095),江苏省“333工程”科研项目(2018) 和江苏省高等学校优秀科技创新团队(2019)资助。
详细信息
    通讯作者:

    Tel: 0519-86332096, 021-67792522, E-mail: hzhou@czie.edu.cn

    suyx@dhu.edu.cn

  • 中图分类号: X511

Selective catalytic reduction of nitric oxide with propylene over one-step synthesized Cu-SAPO-44 catalysts

Funds: The project was supported by Natural Science Foundation of Jiangsu Province (BK20181161), National Natural Science Foundation of China (51278095), Jiangsu 333 Engineering Research Project (2018) and Jiangsu Provincial Excellent Science and Technology Innovation Team (2019).
  • 摘要: 以环己胺(CHA)和铜胺络合物(Cu-TEPA)为共模板剂,一步水热合成Cu-SAPO-44分子筛催化剂,用于贫燃条件下选择性催化丙烯还原NO(C3H6-SCR)。采用N2吸附-脱附、X射线衍射(XRD)、透射电子显微镜(TEM)、紫外可见光谱(UV-vis)、NH3程序升温脱附(NH3-TPD)和H2程序升温还原(H2-TPR)等方法对催化剂进行表征。与纯SAPO-44相比,Cu-TEPA的引入显著增强了分子筛的C3H6-SCR催化活性。当Cu/Al=0.25时,Cu-SAPO-44催化剂有着最大的比表面积、丰富的酸性位和较多的孤立Cu2+物种,具有最佳的脱硝性能。随着Cu-TEPA引入量的增加,铜物种会在分子筛表面聚集,生成相对较多无活性的CuO,从而降低了脱硝活性。原位红外光谱(In situ DRIFTS)研究表明,孤立的Cu2+有助于NO和 C3H6的吸附和活化,促进反应关键中间产物−NCO形成。50 h的持久性反应测试表明,Cu-SAPO-44催化剂始终保持>60%的NOx转化率和>90%的N2选择性,表现出良好的反应稳定性。
  • FIG. 1776.  FIG. 1776.

    FIG. 1776.  FIG. 1776.

    图  1  Cu-SAPO-44催化剂C3H6-SCR活性测试反应示意图

    Figure  1  Reaction diagram of catalyst C3H6-SCR test

    图  2  不同Cu含量的Cu-SAPO-44催化剂的XRD谱图

    Figure  2  XRD patterns of Cu-SAPO-44 catalyst samples with different Cu content and PDF cards of SAPO-44

    图  3  不同Cu含量的Cu-SAPO-44催化剂N2吸附-脱附等温曲线(a)和孔径分布(b)

    Figure  3  N2 adsorption-desorption isotherm (a) and pore size distribution curves (b) of Cu-SAPO-44 catalyst samples with different Cu contents

    图  4  Cu0.25-SAPO-44催化剂的TEM照片((a): (1)−(4))和HR-TEM照片((a): (5), (6)); Cu0.25-SAPO-44催化剂的元素能谱分布(b)

    Figure  4  TEM images ((a): (1)−(4)) and High-resolution TEM images ((a): (5), (6)) of Cu0.25-SAPO-44 catalyst sample; EDS mapping results (b) of Cu, Al, Si and P elements of Cu0.25-SAPO-44 catalyst sample

    图  5  不同Cu含量的Cu-SAPO-44催化剂的NH3-TPD谱图

    Figure  5  NH3-TPD spectra of Cu-SAPO-44 catalyst samples with different Cu contents

    图  6  不同Cu含量的Cu-SAPO-44催化剂的UV-vis谱图

    Figure  6  UV-vis spectra of Cu-SAPO-44 catalyst samples with different Cu contents

    图  7  不同Cu含量的Cu-SAPO-44催化剂的H2-TPR谱图

    Figure  7  H2-TPR profiles of Cu-SAPO-44 catalyst samples with different Cu contents

    图  8  不同Cu含量Cu-SAPO-44催化剂的NOx、C3H6转化率和N2选择性

    Figure  8  NOx, C3H6 conversion and N2 selectivity of Cu-SAPO-44 catalyst samples with different Cu contents (Test conditions: NO 0.05%, C3H6 0.05%, O2 10%, H2O 5%)

    图  9  Cu0.25-SAPO-44催化剂样品的脱硝持久性测试

    Figure  9  Long term DeNOx test over Cu0.25-SAPO-44 catalyst

    图  10  SAPO-44(a)、Cu0.25-SAPO-44(b) 催化剂样品上吸附NO + O2 + C3H6的原位红外谱图

    Figure  10  In situ DRIFTS spectra of NO + O2 + C3H6 adsorbed on SAPO-44(a), Cu0.25-SAPO-44(b) catalyst samples for 45 min and then adding C3H6

    图  11  Cu0.25-SAPO-44催化剂上NO + C3H6 + O2反应的原位红外光谱谱图

    Figure  11  In situ DRIFTS spectra of NO + C3H6 + O2 over Cu0.25-SAPO-44 catalyst sample

    表  1  实验过程中使用的试剂

    Table  1  Reagents are used during the experiment

    ReagentPurityManufacturer
    Al2O3>70%Shandong Guanghui New Material Company
    CuSO4·5H2OAR, >99%Sinopharm Chemical Reagent Co. LTD
    H3PO4AR, >85%Sinopharm Chemical Reagent Co. LTD
    SiO2>40%Aldrich
    H2OARLab-produced
    TEPACP, >90%Sinopharm Chemical Reagent Co. LTD
    CHACP, >90%Sinopharm Chemical Reagent Co. LTD
    NO0.50%NO + 99.5%N2Changzhou Wujin Huayang gas
    C3H65.01%C3H6 + 94.99%N2Changzhou Wujin Huayang gas
    O2≥99.999%Changzhou Wujin Huayang gas
    N2≥99.999%Changzhou Wujin Huayang gas
    下载: 导出CSV

    表  2  Cu-SAPO-44系列催化剂各种元素的成分

    Table  2  Content of each component of series Cu-SAPO-44 catalysts

    SampleElement content w/%
    CuAlPSi
    Cu0.05-SAPO-441.14916.42516.4035.617
    Cu0.15-SAPO-443.35116.31715.5295.699
    Cu0.25-SAPO-445.01615.02113.4636.654
    Cu0.35-SAPO-446.59214.92513.7466.579
    Cu0.45-SAPO-447.97514.50213.1346.380
    下载: 导出CSV

    表  3  Cu-SAPO-44系列催化剂的孔隙结构

    Table  3  Texture properties of series Cu-SAPO-34 catalysts

    SampleSBET / (m2·g−1)Pore volume / (cm3·g−1)Pore size / nm
    Cu0.05-SAPO-443940.1461.853
    Cu0.15-SAPO-444290.1581.789
    Cu0.25-SAPO-444880.1821.498
    Cu0.35-SAPO-444520.1661.650
    Cu0.45-SAPO-444430.1651.689
    下载: 导出CSV
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  • 收稿日期:  2021-12-31
  • 录用日期:  2022-02-18
  • 修回日期:  2022-02-11
  • 网络出版日期:  2022-02-25
  • 刊出日期:  2022-08-26

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