UiO-66中的铜-氧化锆界面可实现将CO选择性催化氢化为甲醇。
Copper-zirconia interfaces in UiO-66 enable selective catalytic hydrogenation of CO to methanol.
作者信息
Zhu Yifeng, Zheng Jian, Ye Jingyun, Cui Yanran, Koh Katherine, Kovarik Libor, Camaioni Donald M, Fulton John L, Truhlar Donald G, Neurock Matthew, Cramer Christopher J, Gutiérrez Oliver Y, Lercher Johannes A
机构信息
Institute for Integrated Catalysis, and Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA, 99354, USA.
Department of Chemistry, Minnesota Supercomputing Institute, Chemical Theory Center, and Inorganometallic Catalyst Design Center, University of Minnesota, Minneapolis, MN, 55455, USA.
出版信息
Nat Commun. 2020 Nov 18;11(1):5849. doi: 10.1038/s41467-020-19438-w.
Molecular interactions with both oxides and metals are essential for heterogenous catalysis, leading to remarkable synergistic impacts on activity and selectivity. Here, we show that the direct link between the two phases (and not merely being together) is required to selectively hydrogenate CO to methanol on catalysts containing Cu and ZrO. Materials consisting of isolated Cu particles or atomically dispersed Cu-O-Zr sites only catalyze the reverse water-gas shift reaction. In contrast, a metal organic framework structure (UiO-66) with Cu nanoparticles occupying missing-linker defects maximizes the fraction of metallic Cu interfaced to ZrO nodes leading to a material with high adsorption capacity for CO and high activity and selectivity for low-temperature methanol synthesis.
与氧化物和金属的分子相互作用对于多相催化至关重要，会对活性和选择性产生显著的协同影响。在此，我们表明，在含铜和氧化锆的催化剂上，将一氧化碳选择性氢化为甲醇需要两相之间存在直接联系（而不仅仅是共存）。由孤立的铜颗粒或原子分散的铜 - 氧 - 锆位点组成的材料仅催化逆水煤气变换反应。相比之下，一种金属有机骨架结构（UiO - 66），其中铜纳米颗粒占据连接体缺失缺陷，使与氧化锆节点界面处的金属铜比例最大化，从而得到一种对一氧化碳具有高吸附容量、对低温甲醇合成具有高活性和选择性的材料。
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