Abstract
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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