O2对多孔粘土异质结构(Fe- pch)负载Fe催化剂上C3H6选择性催化还原NO的影响

S. Y
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摘要

以K10蒙脱土为原料,采用有机模板插层法制备多孔粘土异质结构(PCH),以四乙基硅酸盐(TEOS)为硅源。采用浸渍法将Fe负载在PCH载体上,制备Fe-PCH催化剂。在固定床微反应器中,在0.1% C3 H6、0.1% no、0~10%O2的N2平衡气氛下进行了催化活性试验。总流量为100ml/min,对应的气体时空速(GHSV)为15000h-1。利用漫反射红外傅里叶变换光谱仪(DRIFTS)研究了微反应途径。分析了O2对SCR-C3 H6对Fe-PCH反应性的影响。结果表明,FePCH催化剂在无氧条件下表现出最好的催化性能,在4000℃时达到100%的最大NO转化率,当O2浓度低于临界值[O2]临界值时,随着O2浓度的增加,催化活性逐渐降低。当O2浓度高于[O2]临界值时,NO转化率仅为20%~30%。采用透射电镜(TEM)、N2吸附/解吸和x射线光电子能谱(XPS)技术对Fe-PCH催化剂进行了表征。结果表明,Fe-PCH具有超微孔和介孔结构。Fe-PCH催化剂上的活性组分主要是α- fe2o3纳米棒,暴露(024)和(104)面。利用原位漂移技术对Fe-PCH催化剂表面的活性中间体进行了检测,分析了氧对催化活性影响的机理。结果表明,在C3 H6 -SCR过程中,氧可以抑制Fe-PCH催化剂上异氰酸酯的形成,这可能是导致NO转化率降低的原因。最后,提出了C3 H6 -SCR在Fe-PCH催化剂上的合理反应路径。
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Effect of O2 on Selective Catalytic Reduction of NO by C3H6 over Fe Catalysts Supported on Porous Clay Heterostructures (Fe-PCH)
K10 montmorillonite was used as the raw clay to prepare porous clay heterostructures (PCH) by organic template intercalation and tetraethylorthosilicate (TEOS) was used as silicone source. Fe was load on the PCH support by impregnation method to prepare Fe-PCH catalysts. The catalytic activity tests were carried out in a fixed bed micro-reactor in the atmosphere of 0.1% C3 H6 , 0.1%NO, 0~10%O2 in N2 balance. The total flow rate was 100ml/min and corresponding gas hourly space velocity (GHSV) was 15000h-1. The mircro-reaction pathways were studied by Diffuse Reflection Infrared Fourier Transform Spectrometer (DRIFTS). The influence of O2 on the SCR-C3 H6 reactivity over Fe-PCH was analyzed. The results showed that FePCH catalyst exhibited the best catalytic performance without oxygen, which reached the maximum NO conversion of 100% at 4000 C. When the concentration of O2 is below a critical value, [O2 ]crit, the catalytic activity gradually decreased with the increasing concentration of O2 . When the concentration of O2 is above [O2 ]crit, the NO conversion was only 20%~30%. Fe-PCH catalysts were characterized by transmission electron microscope (TEM), N2 adsorption/desorption and X-ray photoelectron spectroscopy (XPS) techniques. The results showed that Fe-PCH had supermicroporous and mesoporous structures. The active components on Fe-PCH catalyst were mainly α-Fe2 O3 nanorods, exposing (024) and (104) planes. The in situ DRIFTS technique was used to detect the reactive intermediates over the surface of Fe-PCH catalyst, which could help analyze the mechanism of the influence of oxygen on catalytic activity. The results presented that oxygen could inhibit the formation of isocyanate species over Fe-PCH catalyst during C3 H6 -SCR, which might be the reason for the decrease of NO conversion. Finally, a reasonable reaction path of C3 H6 -SCR over Fe-PCH catalyst was proposed.
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