A reusable zirconium-based catalyst for the cycloaddition of CO2 to propylene oxide (PO) was prepared by the surface organometallic chemistry (SOMC) methodology. Accordingly, well-defined amounts of the ZrCl4.(OEt2)(2) precursor were grafted on the surface of silica dehydroxylated at 700 degrees C (SiO2-700) and at 200 degrees C (SiO2-200) in order to afford surface coordination compounds with different podality and chemical environment. The identity of the surface complexes was thoroughly investigated by FT-IR, elemental microanalysis and solid state NMR and applied as a recoverable and reusable heterogeneous catalyst for the title reaction using pure CO2 and flue gas samples from a cement factory. The observed catalytic activity for the isolated zirconium complexes is rationalized by means of systematic DFT calculations.

Conversion of actual flue gas CO2 via cycloaddition to propylene oxide catalyzed by a single-site, recyclable zirconium catalyst

Cavallo, Luigi;
2017

Abstract

A reusable zirconium-based catalyst for the cycloaddition of CO2 to propylene oxide (PO) was prepared by the surface organometallic chemistry (SOMC) methodology. Accordingly, well-defined amounts of the ZrCl4.(OEt2)(2) precursor were grafted on the surface of silica dehydroxylated at 700 degrees C (SiO2-700) and at 200 degrees C (SiO2-200) in order to afford surface coordination compounds with different podality and chemical environment. The identity of the surface complexes was thoroughly investigated by FT-IR, elemental microanalysis and solid state NMR and applied as a recoverable and reusable heterogeneous catalyst for the title reaction using pure CO2 and flue gas samples from a cement factory. The observed catalytic activity for the isolated zirconium complexes is rationalized by means of systematic DFT calculations.
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/11386/4701946
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