Abstract
The influence of excess Fe3+ in ZnFe2O4 for the catalytic oxidative dehydrogenation of 1-butene to 1, 3-butadiene was investigated to try to clarify inconsistencies in the existing literature. A series of nanoscale zinc ferrite powders were produced with increasing Fe: Zn ratios. The materials were characterized by a range of techniques, which showed the presence of α-Fe2O3 as a distinct phase with an increasing excess of Fe3+ and SEM highlighted the increased presence of surface structures on the ferrites at higher Fe: Zn ratios. Reaction testing showed α-Fe2O3to be virtually inactive for the oxidative dehydrogenation of 1-butene. Results for the ferrite catalysts showed a significant decrease in both conversion and yield with an increasing excess of Fe3+. Therefore an excess of Fe3+ has a negative effect on catalytic activity and selectivity of zinc ferrite for the oxidative dehydrogenation of 1-butene, but acts as a promoter for competing hydrogenation and combustion side reactions.
Highlights
Armstrong & Miller [1] discovered 1,3-butadiene in 1886 as a product of his high temperature treatment of petroleum [1], since 1,3-butadiene has been used for the production of a wide variety of synthetic rubbers and elastomers, in particular styrene-butadiene rubber and polybutadienes, which make up approximately 54% of the global 1,3-butadiene demand [2]
The aim of this work was to determine the effect of increasing the Fe: Zn ratio of ZnFe2O4 on its catalytic activity for 1-butene Oxidative dehydrogenation (ODH)
We have clearly shown that as the Fe: Zn ratio was increased the catalytic activity and 1, 3-butadiene selectivity were significantly reduced
Summary
Armstrong & Miller [1] discovered 1,3-butadiene in 1886 as a product of his high temperature treatment of petroleum [1], since 1,3-butadiene has been used for the production of a wide variety of synthetic rubbers and elastomers, in particular styrene-butadiene rubber and polybutadienes, which make up approximately 54% of the global 1,3-butadiene demand [2]. 1, 3-butadiene is almost solely produced from crude oil as a by-product of the steam cracking of naphtha and higher crude oil fractions for the production of ethylene. Butadiene yields from steam cracking vary widely with the composition of the refinery feed and are significantly lower for light hydrocarbon feeds derived from shale gas, because of this there is uncertainty about future 1,3-butadiene supply and pricing has driven a considerable amount of interest in alternative methods for producing it by on-purpose through chemical catalysis. A variety of other processes have been investigated for the on-purpose production of 1,3-butadiene, such as the Lebedev reaction from ethanol and dehydration routes from butanediols [4], routes employing dehydrogenation of alternative hydrocarbon feeds are the most highly developed. Oxidative dehydrogenation (ODH) of 1-butene has been shown to be a promising alternative method for 1,3-butadiene production [5,6] and has been practised commercially when economically viable to do so
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