Department of Chemical and Biomolecular Engineering, Faculty of Engineering, National University of Singapore, 10 Kent Ridge Crescent, Singapore, 119260, Singapore.
Cambridge Centre for Advanced Research and Education in Singapore, 1 Create Way, Singapore, 138602, Singapore.
Nat Commun. 2018 Oct 18;9(1):4326. doi: 10.1038/s41467-018-06828-4.
Interactions between metal nanoparticles (NPs) and metal-organic frameworks (MOFs) in their composite forms have proven to exhibit beneficial properties, such as enhanced catalytic performance through synergistic effects. Herein, we show that Lewis basic sites can be created within an anionic defective MOF by engineering the electronic state of the pendant carboxylate groups situated at the defect sites. This is achieved from the concerted interactions between the pendant carboxylate groups, embedded Pd NPs and charge-balancing cations (M = Ce, Co, Ni, Cu, Mg, Li, Na or K). This work is the first example of generating a new collective property, i.e. Lewis basicity, in metal-carboxylate MOFs. Importantly, the choice of M, used during cation exchange, acts as a convenient parameter to tune the Lewis basicity of the MOF-based nanocomposites. It also provides a facile way to incorporate active metal sites and basic sites within carboxylate-based MOFs to engineer multifunctional nanocatalysts.
金属纳米粒子（NPs）和金属-有机骨架（MOFs）在其复合形式中的相互作用已被证明具有有益的性质，例如通过协同效应增强催化性能。在此，我们表明可以通过工程化位于缺陷位置的悬垂羧酸盐基团的电子状态，在阴离子缺陷 MOF 内创建路易斯碱性位。这是通过悬垂羧酸盐基团、嵌入的 Pd NPs 和电荷平衡阳离子（M = Ce、Co、Ni、Cu、Mg、Li、Na 或 K）之间的协同相互作用实现的。这项工作是首次在金属-羧酸盐 MOFs 中产生新的集体性质（即路易斯碱性）的例子。重要的是，在阳离子交换过程中使用的 M 用作调节基于 MOF 的纳米复合材料的路易斯碱性的方便参数。它还为在基于羧酸盐的 MOFs 中引入活性金属位和碱性位以工程化多功能纳米催化剂提供了一种简便的方法。
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