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A study of ethanol dehydrogenation to acetaldehyde over supported copper catalysts: Catalytic activity, deactivation and regeneration
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2020-06-20 , DOI: 10.1016/j.apcata.2020.117710
Giovanni Pampararo , Gabriella Garbarino , Paola Riani , Maria Villa García , Vicente Sánchez Escribano , Guido Busca

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.



中文翻译:

负载型铜催化剂上乙醇脱氢制乙醛的研究:催化活性,失活和再生

10%和30%wt。通过湿浸渍从商业载体(Sasol)开始制备CuO / wt载体CuO / Al 2 O 3,CuO / ZnAl 2 O 4和CuO / MgAl 2 O 4。在XRD,IR和UV可见光谱,SEM和能量色散X射线光谱,表面积和孔隙率测量中,对催化剂进行了表征。新鲜的含CuO粉末在乙醇/氮气流中转化为负载型Cu金属催化剂,并作为有效的脱氢催化剂,在500-650 K下产生的乙醛收率范围为65-90%。在Cu / ZnAl上观察到的最佳选择性2 Ø图4显然与在二乙醚和乙烯的脱水反应中未覆盖的载体表面的低活性有关。这些催化剂已经在623 K处通过在铜位上的碳沉积而逐渐失活,这几乎保留了未覆盖的载体表面用于脱水反应的活性。通过在约650 K的氧气中燃烧,可以轻松逆转这种影响。增加铜负载量只会使乙醛选择性有所提高。在较高温度下,也观察到了Cu颗粒烧结,但不一定会导致明显的失活。

更新日期:2020-07-05
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