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Effect of linker functionalisation on the catalytic properties of Cu nanoclusters embedded in MOFs in direct CO and CO2 reduction by H2
Faraday Discussions ( IF 3.3 ) Pub Date : 2021-03-10 , DOI: 10.1039/d1fd00012h
Cornelia Elizabeth Lisette Pompe 1 , Petra Ágota Szilágyi 2
Affiliation  

Metal–organic frameworks are promising host supporting matrices for catalytically active guests. In particular, their crystallinity renders them desirable as their pores may act as atom-precise templates for the growth of nanoparticles or nanoclusters therein. This is very advantageous for studying the fundamentals of heterogeneous catalytic processes, especially for site-selective ones, in which the catalyst particle size and shape are of import. Furthermore, metal–organic frameworks may be decorated with organic functional groups, which affect a number of the frameworks’ physical and chemical properties, while remaining isotopological, i.e. having identical structural features and thus templating characteristics. Effectively, this allows for the independent tuning of the Brønsted and Lewis acidity of the substrate while the geometry of the catalytically active guest remains identical. In this study, we systematically study the effect of amino functionalisation of UiO-66(Zr) as a supporting matrix for Cu nanoclusters on the direct reduction of carbon dioxide with hydrogen. In particular, we have found that through modulation of the acidity of the inorganic nodes, framework functionalisation effectively controls the reaction selectivity.

中文翻译:

连接器功能化对嵌入 MOF 中的 Cu 纳米团簇在直接 CO 和 H2 还原 CO2 中催化性能的影响

金属-有机框架是催化活性客体的有前途的宿主支撑基质。特别是,它们的结晶度使它们成为可取的,因为它们的孔可以充当用于在其中生长纳米颗粒或纳米团簇的原子精确模板。这对于研究多相催化过程的基本原理非常有利,特别是对于位点选择性催化过程,其中催化剂的粒径和形状很重要。此外,金属-有机骨架可以用有机官能团装饰,这会影响许多骨架的物理和化学性质,同时保持同位素,具有相同的结构特征和模板特性。有效地,这允许独立调节底物的布朗斯台德和路易斯酸度,同时催化活性客体的几何形状保持相同。在这项研究中,我们系统地研究了 UiO-66(Zr) 作为 Cu 纳米团簇的支撑基质的氨基官能化对用氢气直接还原二氧化碳的影响。特别是,我们发现通过调节无机节点的酸度,框架功能化有效地控制了反应选择性。
更新日期:2021-03-10
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