新型烟气脱硝催化材料制备与性能研究

选择性催化还原（SCR）技术是目前国内外广泛应用的固定源/移动源尾气脱硝技术，目前常用的五氧化二钒基类催化剂由于温度窗口窄、低温活性低，并且钒具有很高的生物毒性等，已逐渐被市场淘汰。经铜离子改性的SSZ-13分子筛催化剂因其优异的催化活性和水热稳定性受到了广泛关注，但铜改性SSZ-13分子筛仍然存在合成成本高昂以及硫中毒等问题，限制了其进一步工业应用。开发价格低廉、环境友好的低温抗硫中毒型SCR催化剂是解决上述问题的重要途径。
本文围绕这一科学技术问题，开展了新型SCR催化剂的制备与性能研究，本研究采用共沉淀法合成了一种新型核壳结构SSZ-13@LDH催化剂。以SSZ-13分子筛为核，在其表面原位共沉淀生长CuMgMnAl水滑石，并用XRD、TEM、SEM、BET、XPS和EDS等对制备的材料进行了表征。结果表明，在CuMgMnAl-LDH纳米片的原位生长过程中，SSZ-13分子筛在碱性环境下的脱硅行为促进了Cu2+和Al3+物种向CHA骨架扩散与迁移，这不仅产生了具有良好SCR活性的Cu2+活性物种，并且形成了更多的酸性位点。弱碱性条件下制备SSZ-13@LDH，有效保持了不耐强碱的基体材料的成分与结构，对核壳结构催化剂制备具有普适性。SCR测试结果表明，SSZ-13@ LDH煅烧后在宽温度窗口内表现出接近100%的SCR反应活性和长效的低温抗SO2性能。TGA、SO2-TPD和FTIR等测试结果证实LDH在抗硫反应中充当了物理吸附位点，NH3与LDH壳上预吸附的SO2反应，形成了可分解的硫酸铵类物质，具有良好的抗SO2活性。本研究所合成的核-壳型SCR催化剂为实际应用中柴油车脱硝技术奠定材料基础，同时也为合成铜基SSZ-13分子筛以及提高催化材料稳定性的探索上提供新策略。

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