Abstract
The massive use of petroleum and its possible exhaustion are driving the current research trend to study alternative raw materials from biomass for organic reactions. In this context, the present article presents a study of the catalytic esterification of levulinic acid, a platform molecule, with ethanol. Metal-organic framework (MOF) type compounds UiO-66-NH2 have been synthesized. Zirconium was incorporated, using zirconium chloride as a metal precursor, together with 2-aminoterephthalic acid as an organic binding agent. An alternative route of synthesis was proposed using more favorable conditions from an economic and environmental point of view, replacing dimethylformamide by 50 and 75% acetone as substitute solvent. The physicochemical properties of the materials were evaluated by X-ray diffraction (XRD), Infrared Spectrometry with Fourier Transform (FTIR), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), microwave plasma atomic emission spectroscopy (MP-AES) and N2 adsorption to understand their morphology, crystalline, chemical and pore structure. The progress of the reaction was followed by gas chromatography and mass spectroscopy. The catalytic activity result of MOF25% in autoclave reactor, showed 100% of selectivity to ethyl levulinate and a turnover number (TON) of 66.18 moles of product/moles of Zr. This good catalytic performance obtained by partial solvent replacement in the synthetic material provides a more economical and eco-friendly process for ethyl levulinate generation.
Highlights
The massive use of petroleum and its possible exhaustion are driving the current research trend to study alternative raw materials from biomass for organic reactions
It was observed that all the materials present a good order and crystallinity, except the MOF50% sample that presents a lower peak intensity, which is related to the crystalline defects of the material that provide its acidity
The synthesis of the Metal-organic framework (MOF) UiO-66-NH2 was achieved under mild solvothermal conditions, replacing up to 75% v/v of the traditional dimethylformamide with acetone
Summary
The massive use of petroleum and its possible exhaustion are driving the current research trend to study alternative raw materials from biomass for organic reactions. In this context, the present article presents a study of the catalytic esterification of levulinic acid, a platform molecule, with ethanol. The increasing demand for chemicals and energy, together with the decline in oil resources, has led to great efforts to develop renewable replacements for fossil raw materials. The intensive use of fossil-fuel means that future energy demand, associated with increasing world populations, economic development and modernization cannot to be met [1,2,3]
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