3 years ago

Catalytically Active Silicon Oxide Nanoclusters Stabilized in a Metal–Organic Framework

Catalytically Active Silicon Oxide Nanoclusters Stabilized in a Metal–Organic Framework
Martino Rimoldi, Leighanne C. Gallington, Karena W. Chapman, Omar K. Farha, Keith MacRenaris, Joseph T. Hupp
Post-synthetic modification of the zirconium-based metal–organic framework (MOF) NU-1000 by atomic layer deposition (ALD), using tetramethoxysilane (Si(OMe)4) as a precursor, led to the incorporation and stabilization of silicon oxide clusters composed of only a few silicon atoms in the framework's pores. The resulting SiOx functionalized material (Si-NU-1000) was found to be catalytically active despite the inactivity of related bulk silicon dioxide (SiO2), thus demonstrating the positive effects of having nanosized clusters of SiOx. Moreover, Si-NU-1000 showed activity greater than that found for aluminum oxide based catalysts—oxides known for their high acidity—such as an aluminum oxide functionalized MOF (Al-NU-1000) and bulk γ-Al2O3. X-ray photoelectron spectroscopy and infrared spectroscopy measurements unmasked the electron donating nature of Si-NU-1000, explaining the unusual electronic properties of the nanosized SiOx clusters and supporting their high catalytic activity. Post-synthetic modification: Low nuclearity silicon oxide clusters introduced into a zirconium metal–organic framework by atomic layer deposition enhance its activity as an acid catalyst.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/chem.201701902

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