期刊
ACS APPLIED MATERIALS & INTERFACES
卷 9, 期 11, 页码 9772-9777出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.7b00562
关键词
metal-organic frameworks; hydrogenation; biomimetic catalyst; Bronsted acid; Hantzsch ester; imine
资金
- MOST [2016YFA0202900]
- National Natural Science Foundation of China [21376212, 21436010]
- Natural Science Foundation of Zhejiang Province, People's Republic of China [LY13B060001]
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.
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