Pandey, J.K. (2016) Nobel metal free, oxidant free, solvent free catalytic transformation of alcohol to aldehyde over ZnO-CeO2 mixed oxide catalyst. Applied Catalysis A: General , 523. pp. 21-30. ISSN 0926-860X

PDF Restricted to Registered users only Download (2612Kb) | Request a copy

Abstract

The catalytic transformation of alcohols to aldehydes under oxidant-free condition has drawn significant attention from the perspective of green chemistry. In this work, we designed noble metal free ZnO-CeO2 mixed oxide catalyst in four different ratios and tested for vapor phase benzyl alcohol dehydrogenation reaction as a model reaction under oxidant free condition. The ZnO-CeO2 mixed oxide catalyst having ratio Zn/Ce = 30/70 composition showed highest selectivity towards formation of benzaldehyde. Interestingly in addition to benzaldehyde, toluene was formed in the reaction due to hydrogenolysis of benzyl alcohol. The lowest Ce3+/Ce4+ ratio was observed from the XPS analysis of Ce(3d) core electron for the catalyst having Zn/Ce = 30/70 composition compared to others. CO2-TPD results proved that mostly the medium strength basic sites were responsible for hydrogen abstraction from benzyl alcohol producing benzaldehyde. H2-TPR results showed that ZnO-CeO2 catalyst (Zn/Ce = 30:70) had lowest reduction temperature which is in the 673 K to 573 K temperature range. The amount of toluene was higher for the ZnO-CeO2 catalyst having Zn/Ce = 40:60 ratio which had less basic sites and higher fraction of Ce3+ ion. The ZnO-CeO2 catalyst (Zn/Ce = 30:70) did not deactivate for a reaction time up to 2 h. While successive regenerations of the catalyst, toluene selectivity were increased. This may be due to the reduction of Ce4+ to Ce3+ by adsorbed hydrogen species. Also the ZnO-CeO2catalyst (Zn/Ce = 30/70) showed activity for the formation of ethanal, propanal, butanal and octanal along with corresponding alkanes from ethanol, 1-propanol, 1-butanol and 1-octanol in oxidant free condition demonstrating the in-situ generation of hydrogen. The micro kinetic analysis showed that there is no external and internal mass transfer limitation in the present case.

Item Type:	Article
Uncontrolled Keywords:	Dehydrogenation; Benzyl alcohol; Propane; Zinc; Ceria; Toluene
Subjects:	Non Coal Ventilation, Fire Gallery and Metallurgy
Divisions:	UNSPECIFIED
Depositing User:	Mr. B. R. Panduranga
Date Deposited:	06 Jan 2017 03:45
Last Modified:	30 Apr 2017 06:04
URI:	http://cimfr.csircentral.net/id/eprint/1648

Actions (login required)

View Item