Journal
CHEM
Volume 7, Issue 3, Pages 686-698Publisher
CELL PRESS
DOI: 10.1016/j.chempr.2020.11.023
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Funding
- NSFC [21725101, 21871244, 21673213, 21521001]
- Fundamental Research Funds for the Central Universities [WK2060030029]
- Fujian Institute of Innovation (CAS)
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The study encapsulated naked Pd nanoparticles in a metal-organic framework (MOF) to regulate Pd microenvironment and interactions with substrates, resulting in significantly improved activity and selectivity in organic silane dehydrogenation coupling and hydrogenation of halogenated nitrobenzenes. This approach surpasses traditional methods, indicating the potential of metal NPs@MOF composites for efficiently integrating well-accessible metal sites with engineered microenvironments.
Creating free-access active sites and regulating their interaction with substrates are crucial for efficient catalysis, yet remain a grand challenge. Herein, naked Pd nanoparticles (NPs) have been encapsulated in a metal-organic framework (MOF), MIL-101-NH2, to afford Pd@MIL-101-NH2. The hydrophobic perfluoroalkyls were post-synthetically modified onto -NH2 group to yield Pd@MIL-101-Fx (x = 3, 5, 7, 11, 15), which engineer the MOF pore walls to regulate Pd surrounding microenvironment and interaction with substrates. As a result, both the dehydrogenation coupling of organosilane and hydrogenation of halogenated nitrobenzenes show that their activity and selectivity can be greatly promoted upon hydrophobic modification due to the favorable substrate enrichment and regulated interactions between Pd and the modified MOF hosts, far surpassing the traditional supported or surfactant-protected Pd NPs. We envision metal NPs@MOF composites would be an ideal platform integrating the inherent activity of well-accessible metal sites with engineered microenvironment via readily tunable MOFs.
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