Catalytic purification of acrylonitrile-containing exhaust gases from petrochemical industry by metal-doped mesoporous zeolites
Catalytic purification of acrylonitrile-containing exhaust gases from petrochemical industry by metal-doped mesoporous zeolites
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金属掺杂介孔沸石催化净化石油化工含丙烯腈废气
DOI：
10.1016/j.cattod.2015.03.021
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发表时间：
2015-12
期刊：
影响因子：
5.3
通讯作者：
Weimin Yang
中科院分区：
文献类型：
--
作者：
Runduo Zhang;Dongjun Shi;Ning Liu;Biaohua Chen;Lianghua Wu;Libin Wu;Weimin Yang
采用浸渍法制备了Cu/、Co/、Fe/、Pt/SBA-15、Cu/SBA-16和Cu/KIT-6等一系列以介孔分子筛为载体的金属催化剂，并通过N2吸附/脱附、XRD、XRF、TEM、XPS和H2-TPR等手段对催化剂进行了表征。在Cu/，Co/，Fe/SBA-15催化剂上，金属阳离子是催化剂的主要物种。CuO主要形成在Cu/KIT-6和Cu/SBA-16上，而金属Pt颗粒构成Pt/SBA-15上的主要物种。丙烯腈（C2 H3CN）的选择性催化燃烧（SCC）结果表明，Cu/SBA-15催化剂在T> 400 °C时C2 H3CN转化率接近完全，N2选择性约为64%。与其他介孔铜催化剂（Cu/KIT-6，Cu/SBA-16）相比，Cu/SBA-15的SCC活性更高，这是由于其较大的孔径有利于铜的分散。通过原位漫反射红外光谱（DRIFTS）进一步研究了Cu/SBA-15试样的应力腐蚀开裂机理，揭示了氧化机理。
A series of metal catalysts with mesoporous zeolites as the supporters including Cu/, Co/, Fe/, Pt/SBA-15, Cu/SBA-16, and Cu/KIT-6 was prepared via impregnation method, and further characterized by N2adsorption/desorption, XRD, XRF, TEM, XPS, and H2-TPR. The metallic cations were verified to be the main species over Cu/, Co/, Fe/SBA-15. CuO was largely formed over Cu/KIT-6 and Cu/SBA-16, while metallic Pt particles constituted the major species on Pt/SBA-15. The selective catalytic combustion (SCC) of acrylonitrile (C2H3CN) revealed that Cu/SBA-15 exhibiting a nearly complete C2H3CN conversion associated with N2selectivity around 64% atT> 400 °C was the most promising catalyst. In comparison with the other mesoporous copper catalysts (Cu/KIT-6, Cu/SBA-16), the higher SCC activity of Cu/SBA-15 was attributed to its larger pore aperture greatly facilitating the copper dispersion. SCC mechanism for Cu/SBA-15 sample was further investigated by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), revealing an oxidation mechanism.
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