A study of ethanol dehydrogenation to acetaldehyde over supported copper catalysts: Catalytic activity, deactivation and regeneration

[Display omitted] •10−30 % CuO on Al2O3-, ZnAl2O4- and MgAl2O4- were tested in ethanol conversion.•Up to 90 % yield in acetaldehyde was obtained over 10 % and 30 % Cu/ZnAl2O4 at 623 K.•Al2O3 support is too active in ethanol dehydration limiting acetaldehyde selectivity.•Moderate deactivation at 623−...

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Veröffentlicht in:Applied catalysis. A, General General, 2020-07, Vol.602, p.117710, Article 117710
Hauptverfasser: Pampararo, Giovanni, Garbarino, Gabriella, Riani, Paola, Villa García, Maria, Sánchez Escribano, Vicente, Busca, Guido
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Sprache:eng
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Zusammenfassung:[Display omitted] •10−30 % CuO on Al2O3-, ZnAl2O4- and MgAl2O4- were tested in ethanol conversion.•Up to 90 % yield in acetaldehyde was obtained over 10 % and 30 % Cu/ZnAl2O4 at 623 K.•Al2O3 support is too active in ethanol dehydration limiting acetaldehyde selectivity.•Moderate deactivation at 623−673 K on stream occurs, due to carbon deposition.•Cu/ZnAl2O4 catalysts are regenerated by burning carbon deposits at 673 K with O2. 10 % and 30 % wt.CuO/wtsupport CuO/Al2O3, CuO/ZnAl2O4 and CuO/MgAl2O4 were prepared through wet impregnation, starting from commercial supports (Sasol). The catalysts were characterized, before and after catalytic runs, by XRD, IR and UV–vis spectroscopies, SEM and energy dispersive X-ray spectroscopy, surface area and porosity measurements. The fresh CuO-containing powders are converted into supported Cu metal catalysts in an ethanol/nitrogen stream, and act as efficient dehydrogenation catalysts producing acetaldehyde yields in the range 65–90 % at 500−650 K. The best selectivity observed on Cu/ZnAl2O4 is apparently mostly associated to the low activity of the uncovered support surface in the dehydration reactions to diethyl ether and ethylene. These catalysts are progressively deactivated already at 623 K by carbon deposition on copper sites, which leaves almost intact the activity of the uncovered support surface for dehydration reactions. This effect is easily reversed by burning in oxygen at around 650 K. Increasing copper loading only produces some increase in acetaldehyde selectivity. At higher temperature, Cu particle sintering is also observed, but it not necessarily causes evident deactivation.
ISSN:0926-860X
1873-3875
DOI:10.1016/j.apcata.2020.117710