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添加钼对FeO/SBA-15催化剂在丙烯选择性氧化中结构和性能的影响

Influence of Adding Molybdenum on Structure and Performance of FeO/SBA-15 Catalysts in Selective Oxidation of Propene.

作者信息

Genz Nina Sharmen, Ressler Thorsten

机构信息

Institut für Chemie Technische Universität Berlin Straße des 17. Juni 135 10623 Berlin Germany.

出版信息

ChemistryOpen. 2019 Aug 21;8(8):1133-1142. doi: 10.1002/open.201900219. eCollection 2019 Aug.

Abstract

Mixed iron and molybdenum oxide catalysts supported on nanostructured silica, SBA-15, were synthesized with various Mo/Fe atomic ratios ranging from 0.07/1.0 to 0.57/1.0. Structural characterization of as-prepared MoO_FeO/SBA-15 samples was performed by nitrogen physisorption, X-ray diffraction, and DR-UV-Vis spectroscopy. Adding molybdenum resulted in a pronounced dispersion effect on supported iron oxidic species. Increasing atomic ratio up to 0.21Mo/1.0Fe was accompanied by decreasing species sizes. Strong interactions between iron and molybdenum during the synthesis resulted in the formation of Fe-O-Mo structure units, possibly Fe(MoO)-like species. Reducibility of MoO_FeO/SBA-15 catalysts was investigated by temperature-programmed reduction experiments with hydrogen as reducing agent. The lower reducibility obtained when adding molybdenum was ascribed to both dispersion and electronic effect of molybdenum. Catalytic performance of MoO_FeO/SBA-15 samples was studied in selective gas-phase oxidation of propene with O as oxidant. Adding molybdenum resulted in an increased acrolein selectivity and a decreased selectivity towards total oxidation products.

摘要

以纳米结构二氧化硅SBA - 15为载体,合成了钼铁原子比在0.07/1.0至0.57/1.0范围内的混合铁钼氧化物催化剂。通过氮气物理吸附、X射线衍射和漫反射紫外可见光谱对制备的MoO_FeO/SBA - 15样品进行结构表征。添加钼对负载的铁氧化物种产生了显著的分散作用。原子比增加到0.21Mo/1.0Fe时,物种尺寸减小。合成过程中铁与钼之间的强相互作用导致形成了Fe - O - Mo结构单元,可能是类似Fe(MoO)的物种。以氢气为还原剂,通过程序升温还原实验研究了MoO_FeO/SBA - 15催化剂的还原性能。添加钼时还原性能降低归因于钼的分散和电子效应。以O为氧化剂,在丙烯的选择性气相氧化反应中研究了MoO_FeO/SBA - 15样品的催化性能。添加钼导致丙烯醛选择性增加,对完全氧化产物的选择性降低。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8d27/6709520/37ac13aa92ff/OPEN-8-1133-g001.jpg

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