Mohammadi Leila, Vaezi Mohammad Reza
Department of Nano Technology and Advanced Materials, Materials and Energy Research Center, Karaj 31787316, Iran.
ACS Omega. 2023 Apr 25;8(18):16395-16410. doi: 10.1021/acsomega.3c01179. eCollection 2023 May 9.
A novel heterogeneous Zr-based metal-organic framework containing an amino group functionalized with nitrogen-rich organic ligand (guanidine), through a step-by-step post synthesis modification approach, was successfully modified by the stabilization of palladium metal nanoparticles on the prepared UiO-66-NH support in order to synthesize the Suzuki-Murray, Mizoroki-Heck, and copper-free Sonogashira reactions and also the carbonylative Sonogashira reaction incorporating HO as a green solvent under mild conditions. This newly synthesized highly efficient and reusable UiO-66-NH@cyanuric chloride@guanidine/Pd-NPs reported catalyst has been utilized to increase anchoring palladium onto the substrate with the aim of altering the construction of the intended synthesis catalyst to form the C-C coupling derivatives. Several strategies, including X-ray diffraction, Fourier transform infrared, scanning electron microscopy, Brunauer-Emmett-Teller, transmission microscopy electron, thermogravimetric analysis, inductively coupled plasma, energy-dispersive X-ray, and elemental mapping analyzes, were used to indicate the successful preparation of the UiO-66-NH@cyanuric chloride@guanidine/Pd-NPs. In these reactions, the UiO-66-NH-supported Pd-NPs illustrated superior performances compared to their catalyst, revealing the benefits of providing nanocatalysts. As a result, the proposed catalyst is favorable in a green solvent, and also, the outputs are accomplished with good to excellent outputs. Furthermore, the suggested catalyst represented very good reusability with no remarkable loss in activity up nine sequential runs.
通过逐步后合成修饰方法,成功制备了一种新型的含氨基的Zr基异质金属有机框架,该氨基用富氮有机配体(胍)官能化,通过在制备的UiO-66-NH载体上稳定钯金属纳米颗粒,合成了铃木-默里反应、水泽-赫克反应和无铜的Sonogashira反应,以及在温和条件下以水为绿色溶剂的羰基化Sonogashira反应。这种新合成的高效且可重复使用的UiO-66-NH@氰尿酰氯@胍/Pd-NPs报道的催化剂已被用于增加钯在底物上的锚定,目的是改变预期合成催化剂的结构以形成C-C偶联衍生物。采用了多种策略,包括X射线衍射、傅里叶变换红外光谱、扫描电子显微镜、布鲁诺尔-埃米特-泰勒比表面积测定、透射电子显微镜、热重分析、电感耦合等离子体、能量色散X射线和元素映射分析,以表明UiO-66-NH@氰尿酰氯@胍/Pd-NPs的成功制备。在这些反应中,UiO-66-NH负载的Pd-NPs与其催化剂相比表现出优异的性能,揭示了提供纳米催化剂的益处。因此,所提出的催化剂在绿色溶剂中是有利的,并且产物的产率良好至优异。此外,所建议的催化剂表现出非常好的可重复使用性,在连续九次运行中活性没有明显损失。