One-pot tandem synthesis of imines from alcohols and amines is regarded as an effective, economic and green approach under mild conditions. In this work, Au nanoparticles (NPs) dispersed on MIL-101 (Au/MIL-101) were demonstrated as highly active and selective bifunctional heterogeneous catalyst for production of various imine derivatives with excellent yields, via amine-alcohol cross-coupling reaction at 343 K in an open flask under an Ar atmosphere. Various physicochemical techniques, including inductively coupled plasma optical emission spectroscopy (ICP-OES), powder X-ray diffraction (P-XRD), X-ray photoelectron spectroscopy (XPS) transmission electron microscopy (TEM) and N₂ adsorption-desorption, were used to characterize of the Au/MIL-101 catalyst. The obtained bifunctional catalyst is highly active and selective towards one-pot imine formation and exhibited the highest TOF (30.15-51.47 h⁻¹) among all the ever-reported MOF-supported Au catalysts. The reaction mechanism of the imine formation from alcohol and amine over Au/MIL-101 catalyst was proposed. Mechanism experiment results demonstrate that Au NPs highly effective in activating oxidation of benzyl alcohol to benzaldehyde while the Lewis acid sites on MIL-101 catalyzed the second condensation step without interfering with the oxidation step. As a result, the excellent catalytic performance of Au/MIL-101 can be ascribed to the synergistic effect between Au NPs with Lewis acid sites in MIL-101.

在醇和胺的条件下，一锅串联合成亚胺是一种有效，经济和绿色的方法。在这项工作中，分散在MIL-101（Au / MIL-101）上的Au纳米颗粒（NPs）被证明是高活性和选择性的双功能非均相催化剂，可通过胺-醇交叉偶合反应在70℃下以优异的产率生产各种亚胺衍生物。 343 K在Ar气氛下的开放式烧瓶中。各种物理化学技术，包括电感耦合等离子体发射光谱（ICP-OES），粉末X射线衍射（P-XRD），X射线光电子能谱（XPS）透射电子显微镜（TEM）和N ₂吸附-解吸用于表征Au / MIL-101催化剂。所获得的双功能催化剂具有高活性，并且对一锅亚胺的形成具有选择性，并且在所有有史以来的MOF负载的Au催化剂中，TOF最高（30.15-51.47 h ^-1）。提出了在Au / MIL-101催化剂上由醇和胺形成亚胺的反应机理。机理实验结果表明，Au NPs在激活苯甲醇氧化为苯甲醛方面非常有效，而MIL-101上的Lewis酸位催化第二步缩合步骤，而不会干扰氧化步骤。结果，Au / MIL-101优异的催化性能可以归因于MIL-101中具有路易斯酸位的Au NP之间的协同作用。