催化作用
化学
羟醛缩合
水溶液
惰性气体
酮
烯烃纤维
有机化学
作者
Vanessa Lebarbier Dagle,Robert A. Dagle,Libor Kovařík,Frederick G. Baddour,Susan E. Habas,Richard T. Elander
出处
期刊:Chemcatchem
[Wiley]
日期:2019-06-03
卷期号:11 (15): 3393-3400
被引量:9
标识
DOI:10.1002/cctc.201900292
摘要
Abstract In this study we investigated the conversion of aqueous methyl‐ethyl‐ketone (MEK) to olefin fuel precursors over Zn x Zr y O z mixed oxide catalysts. Experiments were carried out in water as MEK is intended to be produced from the dehydration of 2,3‐butanediol in fermentation broth which is highly diluted in water. We demonstrated that Zn x Zr y O z catalysts are highly effective for converting aqueous MEK to C 4 −C 5 olefins. High selectivity to olefins equal to 85 % was reached at 92 % per pass conversion when under H 2 atmosphere. Catalyst stability was demonstrated for 60 hours’ time on stream, highlighting the potential for upgrading 2,3‐butanediol contained in fermentation broth without the need for energy‐intensive water separation. Increased concentration of MEK in the aqueous feed results in increased activity towards olefin production. However, water inhibits catalyst deactivation from coking. A mechanistic investigation revealed the impact of the reaction environment (inert or reducing atmosphere) on the reaction pathways. In an inert environment, the mechanism involves consecutive aldol condensation of MEK and 3‐pentanone intermediate. Under reducing conditions two reaction pathways compete with each other as MEK hydrogenation to butenes occurs concurrently with the aldol condensation/decomposition.
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