Genz Nina Sharmen, Ressler Thorsten
Institut für Chemie Technische Universität Berlin Straße des 17. Juni 135 10623 Berlin Germany.
ChemistryOpen. 2019 Aug 21;8(8):1133-1142. doi: 10.1002/open.201900219. eCollection 2019 Aug.
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.
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。