• 论文
主办单位:煤炭科学研究总院有限公司、中国煤炭学会学术期刊工作委员会
过渡金属改性锰金属有机骨架催化剂低温NH3 -SCR 脱硝活性研究
  • Title

    Study on low⁃temperature NH3 -SCR activity of manganese metal organic framework catalyst modified by transition metal

  • 作者

    李海霞杨昌泽张安超孙志君张新民

  • Author

    LI Haixia,YANG Changze,ZHANG Anchao,SUN Zhijun,ZHANG Xinmin

  • 单位

    河南理工大学机械与动力工程学院

  • Organization
    School of Mechanical and Power Engineering,Henan Polytechnic University
  • 摘要

    采用过渡金属硝酸盐溶液浸渍 Mn-MOF(金属有机骨架)前驱体材料经过煅烧后获得了 3种掺杂型锰基催化剂:MnFeOxMnNiOxMnCeOx。 MnMeOx催化剂进行低温氨气选择性催化还 原(NH3-SCR)活性及抗硫性能测试。 结果表明在空速(GHSV)为 30 000 h-1 MnFeO和 MnNiOx催化剂表现出最佳的低温 NH3-SCR 脱硝性能和抗硫性能脱硝效率大于 90%的工作窗口 范围分别为100~250 °C125~275 °C。 铈元素的掺杂未能显著提高催化剂的脱硝性能。 不同空 速测试结果表明空速对催化剂性能有显著影响空速越大催化剂脱硝效率越低但对 N的生成 量影响较小。 通过 X-射线粉末衍射 (XRD)、扫描电子显微镜(SEM)、N吸附-脱附射线光电 子能谱(XPS)、氢气程序升温还原性能测试(H-TPR)、氨气程序升温脱附测试(NH-TPD)等对掺 杂催化剂的理化性质进行研究。 结果表明铁或镍的掺杂增大了催化剂的比表面积改变了 Mn-MOF 烧结过程中 MnO晶体的成型过程增加了催化剂表面 Mn4+ 和表面氧Oα 含量改善了 催化剂的氧化还原性能增加了催化剂的活性位点。 相比之下铈元素的掺杂降低了催化剂的比表 面积和表面氧含量抑制了催化剂的氧化还原性能和表面活性位点的形成导致其脱硝活性较差。 研究表明适当的硝酸盐浸渍 Mn-MOF 能够制备高效的低温 NH-SCR 脱硝催化剂


  • Abstract

    MnFeO, MnNiOand MnCeOwere synthesized by impregnating the precursor material of Mn MOF (metal⁃organic framework) with transition metal nitrate solution. Low temperature selective catalytic reduction (SCR) activity and sulfur resistance of MnMeOcatalyst were investigated. The results showed that the MnFeOand Mn⁃ NiOcatalysts had the best low⁃temperature NH-SCR denitration performance and sulfur resistance when the space velocity was 30 000 h-1. The working window ranges of their denitration efficiency greater than 90% were 100-250 °C and 125 275 °C respectively. The doping of cerium did not significantly improve the denitration performance of the catalyst. The results of different space velocity tests showed that the space velocity had a significant effect on the performance of the catalysts. The larger the space velocity the lower the denitration efficiency of the catalysts,but the variation of space velocity had less effect on the amount of NO production. The physicochemical properties of the doped catalysts were studied by X-ray powder diffraction (XRD),scanning electron microscope (SEM),Nad⁃ sorption⁃desorption,X-ray photoelectron spectroscopy (XPS),Hydrogen temperature⁃programmed reduction perform⁃ ance test (H-TPR),and Ammonia temperature⁃programmed desorption test (NH-TPD). The results showed that the doping of Fe or Ni increased the specific surface area of the catalyst,changed the formation process of MnOcrystal during Mn-MOF sintering,and increased Mn4+ and surface oxygen on the catalyst surface. Doping metal ions improved the redox performance of the catalyst and increased the active center of the catalyst. In contrast,the do⁃ ping of cerium element reduced the specific surface area and surface oxygen content of the catalyst,inhibited the redox performance and the formation of surface active sites,resulting in poor denitration activity. The results showed that ap⁃ propriate nitrate impregnation Mn-MOF could prepare an efficient low⁃temperature NH-SCR denitration catalyst.


  • 关键词

    Mn-MOFMnOx 基NH3 -SCR浸渍法低温

  • KeyWords

    Mn-MOF;MnOx -based;NH3 -SCR;impregnation;low⁃temperature

  • 引用格式
    李海霞,杨昌泽,张安超,等. 过渡金属改性锰金属有机骨架催化剂低温 NH3 -SCR 脱硝活性研究[J].煤炭学报,2022,47(S1):356-364.
  • Citation
    LI Haixia,YANG Changze,ZHANG Anchao,et al. Study on low⁃temperature NH3 -SCR activity of manga⁃ nese metal organic framework catalyst modified by transition metal[J]. Journal of China Coal Society,2022, 47(S1):356-364.
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