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在双金属有机框架中相互包裹不同的金属有机框架以制备独特的复合催化剂。

Interwrapping Distinct Metal-Organic Frameworks in Dual-MOFs for the Creation of Unique Composite Catalysts.

作者信息

Ling Jia-Long, Chen Kai, Wu Chuan-De

机构信息

State Key Laboratory of Silicon Materials, Department of Chemistry, Zhejiang University, Hangzhou 310027, China.

出版信息

Research (Wash D C). 2021 Jul 9;2021:9835935. doi: 10.34133/2021/9835935. eCollection 2021.

Abstract

Incorporating metal nanoparticles (MNPs) inside metal-organic frameworks (MOFs) demonstrates superior catalytic properties in numerous reactions; however, the size and distribution of MNPs could not be well controlled, resulting in low product selectivity in catalysis by undergoing different catalytic reaction pathways. We report herein a facile strategy for integrating lattice-mismatched MOFs together to fabricate homogeneously distributed "dual-MOFs," which are the ideal precursors for the preparation of MNPs@MOFs with unique catalytic properties. As a proof of concept, we successfully synthesize a dual-MOF HKUST-1/ZIF-8 for in situ creation of redox-active Cu NPs inside hierarchical porous ZIF-8 under controlled pyrolytic conditions. Combining the advantages of size-tunable Cu NPs in the molecular sieving matrix of ZIF-8, Cu@ZIF-8 demonstrates high activity and selectivity for transformation of alkynes into alkenes without overhydrogenation, which surpasses most of the catalysts in the literature. Therefore, this work paves a new pathway for developing highly efficient and selective heterogeneous catalysts to produce highly value-added chemicals.

摘要

将金属纳米颗粒(MNPs)掺入金属有机框架(MOFs)中在众多反应中展现出卓越的催化性能;然而,MNPs的尺寸和分布无法得到很好的控制,导致在催化过程中通过不同的催化反应途径时产物选择性较低。我们在此报告一种简便的策略,即将晶格不匹配的MOFs整合在一起以制备均匀分布的“双MOFs”,它们是制备具有独特催化性能的MNPs@MOFs的理想前驱体。作为概念验证,我们成功合成了双MOF HKUST-1/ZIF-8,用于在可控热解条件下在分级多孔ZIF-8内部原位生成具有氧化还原活性的铜纳米颗粒。结合ZIF-8分子筛基质中尺寸可调的铜纳米颗粒的优势,Cu@ZIF-8在炔烃转化为烯烃且无过度氢化的反应中表现出高活性和选择性,这超过了文献中的大多数催化剂。因此,这项工作为开发高效、选择性的多相催化剂以生产高附加值化学品开辟了一条新途径。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3e40/8286356/55374dd49bca/RESEARCH2021-9835935.sch.001.jpg

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