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In situ structural study of manganese and iron oxide promoted rhodium catalysts for oxygenate synthesis
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2020-09-23 , DOI: 10.1016/j.apcata.2020.117845
Pamela Carrillo , Rui Shi , Sanjaya D. Senanayake , Michael G. White

In situ x-ray diffraction (XRD) and absorption spectroscopy (XAS) was used to characterize the structure and phase composition of a novel Mn and Fe double-promoted Rh-based catalyst for CO hydrogenation to oxygenates. Catalysts with different Mn:Rh molar ratios were prepared by combining Mn and Rh precursors with Fe2O3 powder, which were then calcined in air and reduced under hydrogen. The resulting MnRh/Fe2O3 catalysts are found to be highly selective for ethanol synthesis (∼40 %) for CO hydrogenation under mild conditions (∼1 bar, 240 °C). Comparison of the reactivity results with quantitative phase information from in situ XRD measurements suggest that reduced metal oxides, MnO and FeOx, and metallic Rh co-exist as active phases to promote oxygenate selectivity. The results of this work also highlight the importance of in situ characterization for extracting meaningful information on the active phases of such complex, ternary catalysts which can vary under reaction conditions.



中文翻译:

锰和铁氧化物助催化的铑催化剂的原位结构研究

原位X射线衍射(XRD)和吸收光谱(XAS)用于表征新型的Mn和Fe双助Rh基催化剂的结构和相组成,该催化剂用于CO加氢生成含氧化合物。通过将Mn和Rh前驱体与Fe 2 O 3粉末混合来制备具有不同Mn:Rh摩尔比的催化剂,然后将其在空气中煅烧并在氢气下还原。发现所得的MnRh / Fe 2 O 3催化剂在温和条件下(〜1 bar,240°C)对乙醇加氢合成乙醇具有很高的选择性(〜40%)。将反应性结果与原位XRD测量得到的定量相信息进行比较表明,还原的金属氧化物MnO和FeO x,和金属Rh共存为活性相,以提高含氧化合物的选择性。这项工作的结果还强调了就地表征对于提取这类复杂的三元催化剂的活性相有意义的信息的重要性,这些信息在反应条件下可能会发生变化。

更新日期:2020-10-02
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