Functionalized Metal-Organic Framework as a Biomimetic Heterogeneous Catalyst for Transfer Hydrogenation of Imines
Functionalized Metal-Organic Framework as a Biomimetic Heterogeneous Catalyst for Transfer Hydrogenation of Imines
复制标题
功能化金属有机框架作为亚胺转移氢化的仿生多相催化剂
DOI：
10.1021/acsami.7b00562
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发表时间：
2017-03-22
影响因子：
9.5
通讯作者：
Ren, Qilong
中科院分区：
文献类型：
--
作者：
Chen, Jingwen;Zhang, Zhiguo;Ren, Qilong
模拟生物催化体系已成为设计新颖有效的化学转化的流行策略之一。在酶催化的反应中，刘易斯和布朗斯台德酸性官能团在活性位点的协同相互作用代表了活化反应物的共同特征。以MIL-101（Cr）为仿生平台，在其多级孔道中引入磺酸基（SO 3 H），制备了以Hantzsch酯为还原剂的亚胺转移加氢多相催化剂。醛亚胺和酮亚胺都以类似于金属酶的方式有效地转化为它们的氢化对应物。包封在MOF笼中的Cr 3+节点和磺酸官能团在促进这种转化中协同工作，导致与其均质类似物相比的反应性。此外，MIL-101（Cr）-SO 3 H可以循环使用，而反应性没有明显损失。
Mimicking a biocatalytic system has been one of the prevalent strategies for the design of novel and efficient chemical transformations. Among the enzyme-catalyzed reactions, the cooperative interplay of Lewis- and Bronstedacidic functionalities at active sites represents a common feature in activating reactants. Employing MIL-101(Cr) as a biomimetic platform, we customize a sulfonic group (SO3H) into its hierarchical pores to generate a heterogeneous catalyst for transfer hydrogenation of imines by using Hantzsch ester as the reductant. Both aldimines and ketimines were efficiently converted to their hydrogenated counterparts in a manner similar to metal enzymes. The Cr3+ node and sulfonic acid functionality encapsulated in MOF cages worked cooperatively in promoting this transformation, resulting in an reactivity as compared to its homogeneous analogue. Furthermore, MIL-101(Cr)-SO3H could be recycled for many without considerable loss in reactivity.