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Zr-based metal-organic frameworks drived Rh-Mn catalysts for highly selective CO hydrogenation to C2 oxygenates
Journal of Industrial and Engineering Chemistry ( IF 5.9 ) Pub Date : 2020-06-01 , DOI: 10.1016/j.jiec.2020.03.008
Xiaoya Xue , Jun Yu , Ying Han , Xiuzhen Xiao , Zhangping Shi , Haifang Mao , Dongsen Mao

Abstract A series of Zr-based metal-organic frameworks (UiO-66) supported Rh–Mn catalysts with various metal loadings were prepared by using a co-impregnation method, and the catalytic activities were investigated for the direct synthesis of ethanol-based C2+ oxygenates from CO hydrogenation. The catalysts were comprehensively characterized by means of N2 sorption, XRD, TEM, XPS, H2-TPR, and DRIFT. The structural and textural properties of the catalysts show clearly that the overall framework structure of UiO-66 can be beneficial to the high dispersion of supported metals, but the synergistic effect of Rh and Mn would be influenced by the metal loading or Mn/Rh ratio. When the loadings of Rh and Mn reached 3 wt.% and 3 wt.%, the catalyst has the best catalytic activity with the highest yield of C2+ oxygenates of 200.1 g/(kg h), which can be attributed to the enhanced CO dissociation ability of Rh sites and weaker Rh−CO band strength.

中文翻译:

Zr 基金属有机骨架驱动 Rh-Mn 催化剂用于高选择性 CO 加氢成 C2 氧化物

摘要 采用共浸渍法制备了一系列 Zr 基金属有机骨架 (UiO-66) 负载的不同金属负载量的 Rh-Mn 催化剂,并研究了直接合成乙醇基 C2+ 的催化活性。来自 CO 加氢的氧化物。通过N2吸附、XRD、TEM、XPS、H2-TPR和DRIFT等手段对催化剂进行了综合表征。催化剂的结构和质构特性清楚地表明,UiO-66的整体骨架结构有利于负载金属的高分散性,但Rh和Mn的协同效应会受到金属负载量或Mn/Rh比的影响. 当 Rh 和 Mn 的负载量分别达到 3 wt.% 和 3 wt.% 时,催化剂的催化活性最好,C2+ 氧化物的产率最高,为 200.1 g/(kg h),
更新日期:2020-06-01
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