Efficient visible light initiated one-pot syntheses of secondary amines from nitro aromatics and benzyl alcohols over Pd@NH2-UiO-66(Zr)
Efficient visible light initiated one-pot syntheses of secondary amines from nitro aromatics and benzyl alcohols over Pd@NH2-UiO-66(Zr)
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高效可见光引发硝基芳烃和苯甲醇在 Pd@NH2-UiO-66(Zr) 上一锅法合成仲胺
DOI：
10.1016/j.apcatb.2021.121031
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Zhaohui Li
中科院分区：
文献类型：
--
作者：
Mingming Hao;Zhaohui Li
采用双溶剂浸渍法和光还原法制备了Pd@NH2-UiO-66（Zr）纳米粒子，并将其包裹在NH 2-UiO-66（Zr）纳米粒子的空腔内，该纳米粒子在可见光下催化硝基化合物和醇的加氢/脱氢反应合成仲胺中表现出良好的上级活性，胺和醛缩合成亚胺，以及亚胺的氢化。在硝基化合物光催化氢化成胺和醇脱氢成醛的反应中，光生电子/空穴的同时消耗促进了整个反应。由于腔体和小尺寸Pd纳米颗粒的限制效应，Pd@NH2-UiO-66（Zr）与其中较大的Pd纳米颗粒沉积在表面上的Pd/NH 2-UiO-66（Zr）相比显示出显著优越的上级性能。该研究为仲胺的制备提供了一种高效、绿色的策略，并强调了利用M/MOFs纳米复合材料作为光诱导一锅法串联反应的多功能催化剂的巨大潜力。
Pd@NH2-UiO-66(Zr), with small-sized Pd nanoparticles encapsulated inside the cavities of NH2-UiO-66(Zr), was obtained via a double-solvent impregnation followed by a photoreduction process, which shows superior activity for the visible light initiated syntheses of secondary amines from nitro compounds and alcohols, via a sequential photocatalytic hydrogenation of nitro compounds/dehydrogenation of alcohols, condensation of amines and aldehydes to imines, and the hydrogenation of imines. Simultaneous consumption of photogenerated electrons/holes in the photocatalytic hydrogenation of nitro compounds to amines and dehydrogenation of alcohols to aldehydes promotes the whole reaction. Due to the confinement effect of the cavity and the small-sized Pd nanoparticles, Pd@NH2-UiO-66(Zr) shows significantly superior performance as compared with Pd/NH2-UiO-66(Zr), in which larger Pd nanoparticles are deposited on the surface. This study provides an efficient and green strategy for the production of secondary amines and highlights the great potential of using M/MOFs nanocomposites as multifunctional catalysts for light induced one-pot tandem reactions.
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