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Co-assembly route to facile synthesis of hierarchical core-shell nano-CuMOR@SBA-15 composite for one-step conversion of DME to ethanol with enhanced catalytic performance
Journal of Porous Materials ( IF 2.6 ) Pub Date : 2020-01-31 , DOI: 10.1007/s10934-020-00862-8
Haibo Han , Dezhi Han , Kang Li , Jie Lei , Youhe Wang , Peng Bai , Mark J. Rood , Zifeng Yan

Abstract

Core-shell composite catalysts have attracted attention due to their pore connectivity and synergistic catalytic effect. In this work, the novel core-shell nano-CuMOR@SBA-15 composite (NCMSC) was fabricated via the co-assembly method using the P123 triblock copolymer as template. The prepared samples were characterized by XRD, 129Xe NMR, SEM, TEM techniques, and N2 adsorption-desorption. Results indicate that the NCMSC’s crystal core was encapsulated by ordered mesoporous Cu/SBA-15-like shell to form hierarchically porous NCMSC composite. Compared to the CuMOR, CuMOR + SBA-15 mixture, MOR + CuSBA-15 mixture and CuSBA-15, the NCMSC composite exhibited improved catalytic performance to convert dimethyl ether (DME) to ethanol with DME conversion of 42.8% and ethanol selectivity of 96.1%. Moreover, the life of the NCMSC composite catalyst was much longer and the induction of the reaction was shorter than other catalysts. This could be ascribed to the synergistic effect of nano-CuMOR@SBA-15 composite by combining carbonylation activity of CuMOR with the hydrogenation activity of CuSBA-15.This novel NCMSC composite can be a candidate catalyst of one-step conversion of DME to ethanol.



中文翻译:

易于组装的分级组装核壳纳米CuMOR @ SBA-15纳米复合材料的合成路线,用于将DME一步转化为乙醇并提高催化性能

摘要

核-壳复合催化剂由于其孔连通性和协同催化作用而引起了人们的关注。在这项工作中,以P123三嵌段共聚物为模板,通过共组装法制备了新型核壳纳米CuMOR @ SBA-15复合材料(NCMSC)。通过XRD,129 Xe NMR,SEM,TEM技术和N 2表征制备的样品吸附-解吸。结果表明,NCMSC的晶体核被有序介孔的Cu / SBA-15样壳包裹,形成了分层多孔的NCMSC复合材料。与CuMOR,CuMOR + SBA-15混合物,MOR + CuSBA-15混合物和CuSBA-15混合物相比,NCMSC复合材料具有更好的催化性能,可将二甲醚(DME)转化为乙醇,DME转化率为42.8%,乙醇选择性为96.1。 %。此外,与其他催化剂相比,NCMSC复合催化剂的寿命更长,反应的诱导时间更短。通过将CuMOR的羰基化活性和CuSBA-15的氢化活性相结合,可以归因于纳米CuMOR @ SBA-15复合材料的协同作用。这种新型的NCMSC复合材料可以作为DME一步转化为乙醇的候选催化剂。 。

更新日期:2020-01-31
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