The production of DME via one-pot CO2 hydrogenation is a strategic way of recycling CO2 with the production of a high-value added product. This work aims to investigate the effect of the main zeolite features, e.g. structure or acidity, on the activity, selectivity and stability of the catalyst for DME production via both methanol dehydration and one-pot CO2 hydrogenation. Several zeolites (i.e. FER and MFI) were synthesized and deeply characterized with XRD, B.E.T, NH3-TPD and FTIR. Obtained crystals were used as catalysts for methanol dehydration as well as for one-pot CO2-to-DME process. Obtained results allow giving new insights about the role of the interaction between metals and acid sites for an efficient DME production via one-pot CO2 hydrogenation. In particular, zeolite acidity plays a crucial role in methanol dehydration step and Lewis acid sites seems to be more active than Brønsted sites. Furthermore, metal/acid proximity plays are a key factor in one-pot CO2 hydrogenation; in fact, the catalytic performances of multifunctional catalytic bed improve by increasing the metal/acid sites proximity. The findings of this research allow to highlight the main factors to be taken into account in terms of design and optimization of new catalytic systems for DME synthesis.

Direct CO2-to-dimethyl Ether Hydrogenation over CuZnZr/zeolite Hybrid Catalyst: New evidences on the interaction between acid and metal sites

Catizzone E.;Migliori M.;Giordano G.
2019

Abstract

The production of DME via one-pot CO2 hydrogenation is a strategic way of recycling CO2 with the production of a high-value added product. This work aims to investigate the effect of the main zeolite features, e.g. structure or acidity, on the activity, selectivity and stability of the catalyst for DME production via both methanol dehydration and one-pot CO2 hydrogenation. Several zeolites (i.e. FER and MFI) were synthesized and deeply characterized with XRD, B.E.T, NH3-TPD and FTIR. Obtained crystals were used as catalysts for methanol dehydration as well as for one-pot CO2-to-DME process. Obtained results allow giving new insights about the role of the interaction between metals and acid sites for an efficient DME production via one-pot CO2 hydrogenation. In particular, zeolite acidity plays a crucial role in methanol dehydration step and Lewis acid sites seems to be more active than Brønsted sites. Furthermore, metal/acid proximity plays are a key factor in one-pot CO2 hydrogenation; in fact, the catalytic performances of multifunctional catalytic bed improve by increasing the metal/acid sites proximity. The findings of this research allow to highlight the main factors to be taken into account in terms of design and optimization of new catalytic systems for DME synthesis.
CO2 recycling; Dimethyl ether; Heterogeneous catalysis; Industrial chemistry processes; Lewis/Brønsted acid sites; Nanostructured catalysts; Zeolites
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.11770/303568
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