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Copper-gold nanoparticles encapsulated within surface-tethered dendrons as supported catalysts for the Click reaction
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2018-07-04 , DOI: 10.1016/j.apcata.2018.07.007
Aibolat Koishybay , Daniel F. Shantz

The synthesis, characterization, and catalytic testing of copper and copper:gold nanoparticles in melamine-based dendrons supported on SBA-15 is reported. It was found that by first making small gold nanoparticles using the dendrons as templates, stable copper(0) overlayers could then be successfully deposited. These samples were used as catalysts for the click reaction, with the most active samples possessing rates of 8.9 mol triazole produced/(mol copper – hour), nearly 50 times high than literature reports of copper nanoparticles in solution. In contrast, the gold nanoparticles themselves are inert for this reaction, consistent with the copper being deposited as an overlayer on the gold nanoparticles. Copper leaching was shown to be less pronounced for particles formed in the dendrons versus copper simply deposited on SBA-15. Larger dendrons lead to suppressed rates due to diffusion resistance with rates decreasing from 8.9 to 5.2 to 0.69 mol triazole produced/(mole Cu-hour) for G1, G2, and G3 respectively. Infrared spectroscopy was used to monitor the reaction in real time, and provided information about the various surface intermediates formed.



中文翻译:

封装在表面束缚树枝状结构中的铜金纳米粒子,作为Click反应的负载型催化剂

报道了在SBA-15上负载的基于三聚氰胺的树枝状结构中铜和铜:金纳米颗粒的合成,表征和催化测试。发现通过首先使用树枝状结构作为模板制备小的金纳米颗粒,然后可以成功地沉积稳定的铜(0)覆盖层。这些样品用作点击反应的催化剂,活性最高的样品具有8.9 mol三唑/(mol铜-小时)的生成率,比溶液中铜纳米颗粒的文献报道高近50倍。相反,金纳米颗粒本身对该反应是惰性的,这与铜作为覆盖层沉积在金纳米颗粒上是一致的。与仅沉积在SBA-15上的铜相比,树突中形成的颗粒的铜浸出显示的不那么明显。较大的树枝状分子由于抗扩散性而导致速率降低,G1,G2和G3的三唑产量从8.9降低至5.2 mol /(mol Cu-hour)。红外光谱用于实时监测反应,并提供有关形成的各种表面中间体的信息。

更新日期:2018-07-04
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