Continuous catalytic process for the selective dehydration of glycerol over Cu-based mixed oxide
[Display omitted] •Cu-Mg-Al oxide catalyzes selectively glycerol dehydration to acetol in a continuous flow system.•10.0%Cu-HT-4 catalyst offers the best glycerol conversion and acetol selectivity.•Cu-catalysts remain active after several re-uses by introducing regeneration cycles.•Cu is essential f...
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| Published in: | Journal of catalysis Vol. 385; pp. 160 - 175 |
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| Format: | Journal Article |
| Language: | English |
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01-05-2020
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| Abstract | [Display omitted]
•Cu-Mg-Al oxide catalyzes selectively glycerol dehydration to acetol in a continuous flow system.•10.0%Cu-HT-4 catalyst offers the best glycerol conversion and acetol selectivity.•Cu-catalysts remain active after several re-uses by introducing regeneration cycles.•Cu is essential for acetol production with high reaction rate and more selective than Ni or Co.•In situ spectroscopic studies evidence Cu1+ as the most active Cu species in the catalyst.
The selective dehydration of glycerol to hydroxyacetone (acetol) was studied with Cu-based mixed oxides derived from hydrotalcite as catalysts in a continuous flow fix-bed reactor. Catalysts were prepared by co-precipitation and characterized by ICP, N2 adsorption, XRD, NH3-TPD, CO2-TPD, TPR and TEM. Different parameters were investigated to develop the most appropriate material as well as to determine the function of every metallic species. The optimized Cu-Mg-AlOx offered ≈60% acetol selectivity at >90% glycerol conversion (≈80% liquid yield, up to TOS = 9 h). The catalyst could be regenerated by calcination, achieving full activity recovery after five re-cycles. “In-situ” FTIR and XPS measurements evidenced that the presence of Cu, specially the most active Cu1+ species, was essential to carry out the dehydration to acetol with high reaction rates, and to form the preferred intermediate (with CO group); although a minor contribution from Cu0 and Cu2+ species could not be discarded. |
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| AbstractList | [Display omitted]
•Cu-Mg-Al oxide catalyzes selectively glycerol dehydration to acetol in a continuous flow system.•10.0%Cu-HT-4 catalyst offers the best glycerol conversion and acetol selectivity.•Cu-catalysts remain active after several re-uses by introducing regeneration cycles.•Cu is essential for acetol production with high reaction rate and more selective than Ni or Co.•In situ spectroscopic studies evidence Cu1+ as the most active Cu species in the catalyst.
The selective dehydration of glycerol to hydroxyacetone (acetol) was studied with Cu-based mixed oxides derived from hydrotalcite as catalysts in a continuous flow fix-bed reactor. Catalysts were prepared by co-precipitation and characterized by ICP, N2 adsorption, XRD, NH3-TPD, CO2-TPD, TPR and TEM. Different parameters were investigated to develop the most appropriate material as well as to determine the function of every metallic species. The optimized Cu-Mg-AlOx offered ≈60% acetol selectivity at >90% glycerol conversion (≈80% liquid yield, up to TOS = 9 h). The catalyst could be regenerated by calcination, achieving full activity recovery after five re-cycles. “In-situ” FTIR and XPS measurements evidenced that the presence of Cu, specially the most active Cu1+ species, was essential to carry out the dehydration to acetol with high reaction rates, and to form the preferred intermediate (with CO group); although a minor contribution from Cu0 and Cu2+ species could not be discarded. |
| Author | Domine, Marcelo E. Ventura, María Concepción, Patricia Mazarío, Jaime |
| Author_xml | – sequence: 1 givenname: Jaime surname: Mazarío fullname: Mazarío, Jaime – sequence: 2 givenname: Patricia surname: Concepción fullname: Concepción, Patricia – sequence: 3 givenname: María orcidid: 0000-0002-7173-3995 surname: Ventura fullname: Ventura, María – sequence: 4 givenname: Marcelo E. surname: Domine fullname: Domine, Marcelo E. email: mdomine@itq.upv.es |
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•Cu-Mg-Al oxide catalyzes selectively glycerol dehydration to acetol in a continuous flow system.•10.0%Cu-HT-4 catalyst offers the best... |
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| SubjectTerms | Acetol Copper catalyst Glycerol Glycerol dehydration Mixed oxides |
| Title | Continuous catalytic process for the selective dehydration of glycerol over Cu-based mixed oxide |
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