Ling Jia-Long, Chen Kai, Wu Chuan-De
State Key Laboratory of Silicon Materials, Department of Chemistry, Zhejiang University, Hangzhou 310027, China.
Research (Wash D C). 2021 Jul 9;2021:9835935. doi: 10.34133/2021/9835935. eCollection 2021.
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.
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。