Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 7, Pages 8344-8352Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c20437
Keywords
metal-organic framework; postsynthetic functionalization; carbon dioxide fixation; cycloaddition; heterogeneous catalysis
Funding
- National Science Centre, Poland [UMO-2014/14/E/ST5/00652]
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A tandem postsynthetic modification strategy was developed for Zr-based metal-organic framework (MOF) materials, resulting in well-defined 2-in-1 heterogeneous catalysts with high catalytic activity in the synthesis of cyclic carbonates. Experimental measurements, including DRIFT and solid-state NMR, helped elucidate the role of each component in the catalytic reaction, especially the cooperative effect between Lewis acid sites and the co-catalyst in the heterogeneous system.
We have devised a straightforward tandem postsynthetic modification strategy for Zr-based metal-organic framework (MOF) materials, which resulted in a series of well-defined 2-in-1 heterogeneous catalysts, cat1-cat8, exhibiting high catalytic activity in the synthesis of cyclic carbonates under solvent-free and co-catalyst-free conditions. The materials feature precisely located co-catalyst moieties decorating the metal nodes throughout the bulk of the MOF and yield cyclic carbonates with up to 99% efficiency at room temperature. We use diffuse reflectance infrared Fourier transform (DRIFT) and solid-state nuclear magnetic resonance (NMR) measurements to elucidate the role of each component in this model catalytic reaction. Establishing a method to precisely control the co-catalyst loading allowed us to observe the cooperativity between Lewis acid sites and the co-catalyst in the 2-in-1 heterogeneous system.
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