Ethanol conversion over GaO-ZrO solid solution: empirical evidence of the reaction pathway, the surface acid-base properties, and the role of gallium ions
Ethanol conversion over Ga 2 O 3 -ZrO 2 solid solution was examined in the temperature range of 573-773 K, and acetone/isobutene formation was confirmed under cofeeding of H 2 O vapor. The reaction pathway was empirically investigated with the contact time dependency and reactivity of the five possi...
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Veröffentlicht in: | Catalysis science & technology 2021-03, Vol.11 (6), p.247-256 |
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Zusammenfassung: | Ethanol conversion over Ga
2
O
3
-ZrO
2
solid solution was examined in the temperature range of 573-773 K, and acetone/isobutene formation was confirmed under cofeeding of H
2
O vapor. The reaction pathway was empirically investigated with the contact time dependency and reactivity of the five possible intermediates. The surface acid-base properties were discussed with 1-butene isomerization, 2-butanol decomposition and the poisoning experiment, the dehydration/dehydrogenation selectivity of C3-C4 primary and secondary alcohols, and CO
2
-TPD. The Ga
2
O
3
-ZrO
2
catalyst was less basic than ZrO
2
itself and exhibited a stronger dehydrogenation property. Alcohol dehydrogenation over Ga
2
O
3
-ZrO
2
was suggested to be promoted by the specific dehydrogenation property of isolated Ga
3+
species. Acetaldehyde formed by ethanol dehydrogenation was converted into acetone, mainly
via
acetate species in the presence of H
2
O. Coexistence of ZrO
2
, doped elements with dehydrogenation capability, surface acid-base properties, and H
2
O vapor is important for ethanol to acetone/isobutene reaction.
The reaction pathway of ethanol conversion to acetone/isobutene over Ga
2
O
3
-ZrO
2
solid solution was investigated. Acetaldehyde formation is promoted at the atomically dispersed Ga
3+
species due to its dehydrogenation capability rather than solid basicity of a catalyst. |
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ISSN: | 2044-4753 2044-4761 |
DOI: | 10.1039/d0cy02271c |