过渡金属元素掺杂改性SCR对零价汞的催化氧化性能

Catalytic Oxidation Performance of SCR Doped with Transition Metal Elements for Removal of Elemental Mercury

  • 摘要: 为提高商用SCR催化剂对Hg0(零价汞)的催化氧化活性,研究了过渡金属对其进行掺杂改性的方法,并利用固定床反应平台考察了不同试验条件下改性催化剂对Hg0的氧化效率. 结果表明:Y、Zn、Ni和Zr等过渡金属的掺杂可明显抑制SCR催化剂的催化活性,而Fe、Cu掺杂改性SCR催化剂对Hg0的催化氧化性能有显著提升. 在反应温度为350 ℃、空速比为370 000 h-1、φ(HCl)为1×10-5的条件下,Fe、Cu掺杂改性的SCR催化剂对Hg0的氧化效率均能达到90%以上,并且Fe掺杂改性后的SCR催化剂的脱硝性能也未受到明显影响. 借助XRD和XPS等表征手段,对反应前后Fe掺杂改性SCR催化剂进行了研究,表明Fe改性SCR催化剂遵循Mars-Maessen和Langmuir-Hinshelwood机制,可明显提高对Hg0的催化氧化效率,因此,应用前景较好.

     

    Abstract: In order to improve the catalytic oxidation activity of the commercial selective catalytic reduction (SCR) catalyst for removal of Hg0 in flue gas, a transition metal oxides doped SCR catalyst by impregnation method was employed to improve the Hg0 catalytic oxidation. Moreover, the fixed bed reaction platform was used to investigate the modified catalyst under different test conditions for Hg0 catalytic oxidation efficiency. Hg0 catalytic oxidation efficiencies of the modified catalysts by transition metals were tested in a pack-bed reactor system under different experimental conditions. The results showed that the catalytic performance of the SCR catalyst was remarkably inhibited by Y, Zn, Ni and Zr, and greatly enhanced by Fe and Cu. The Hg0 oxidation efficiency of the SCR doped with Fe or Cu was over 90% when the reaction temperature, space velocity and HCl concentration were set as 350 ℃, 370,0 h-1 and 1×10-5, respectively. Furthermore, Fe doping the catalyst did not obviously affect the NOx removal efficiency of the SCR catalyst. In addition, XRD and XPS were employed to characterize the SCR catalyst doped with Fe. The results indicated that the SCR catalyst doped with Fe showed good performance of Hg0 oxidation according to the Mars-Maessen and Langmuir-Hinshelwood mechanisms. Therefore, SCR modified with Fe has good application prospects for the simultaneous removal of elemental mercury and NOx.

     

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