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Issue 16, 2016
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Catalytic transfer hydrogenation of ethyl levulinate to γ-valerolactone over zirconium-based metal–organic frameworks

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Abstract

A series of highly crystalline, porous, zirconium-based metal–organic frameworks (Zr-MOFs) with different ligand functionalities and porosities were applied for catalytic transfer hydrogenation of ethyl levulinate (EL) to form γ-valerolactone (GVL), using isopropanol as a hydrogen donor. The roles of the ligand functionality and the metal center of the Zr-MOFs were identified and reaction parameters optimized, for selective production of GVL. The maximum yield of GVL (up to 92.7%) was achieved in 2 h at 200 °C with UiO-66(Zr). Interestingly, zirconium trimesate (MOF-808) emerged as the most suitable candidate, with the highest GVL formation rate (94.4 μmol g−1 min−1) among the catalysts tested at 130 °C. It was also found to be effective in conversion of EL to GVL in an open system using the solvent refluxing method. Both the catalysts (UiO-66(Zr) and MOF-808) were recycled at least five times under their specified reaction conditions without a notable change in catalytic activity and product selectivity. Fresh and recycled catalysts were characterized in detail using X-ray powder diffraction (XRD), N2 adsorption–desorption, thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM) in order to understand the stability and structural changes that occurred in the catalysts. Finally, a plausible reaction mechanism was presented on the basis of active sites present in catalysts confirmed by characterization results.

Graphical abstract: Catalytic transfer hydrogenation of ethyl levulinate to γ-valerolactone over zirconium-based metal–organic frameworks

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Publication details

The article was received on 25 Feb 2016, accepted on 22 Jun 2016 and first published on 23 Jun 2016


Article type: Paper
DOI: 10.1039/C6GC00524A
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Green Chem., 2016,18, 4542-4552

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    Catalytic transfer hydrogenation of ethyl levulinate to γ-valerolactone over zirconium-based metal–organic frameworks

    A. H. Valekar, K. Cho, S. K. Chitale, D. Hong, G. Cha, U. Lee, D. W. Hwang, C. Serre, J. Chang and Y. K. Hwang, Green Chem., 2016, 18, 4542
    DOI: 10.1039/C6GC00524A

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