脱氢
化学
丙烯
催化作用
氢
光化学
气相
无机化学
有机化学
作者
Kenneth T. Hindle,R. Burch,P.C. Crawford,Christopher Hardacre,P. Hu,B. Kalirai,David W. Rooney
标识
DOI:10.1016/j.jcat.2007.07.032
摘要
The dehydrogenation of 1,2,3,4-tetrahydrocarbazole (THCZ) to form carbazole (CZ) over supported palladium catalysts was examined in the presence of hydrogen acceptors. As expected, liquid hydrogen acceptors increased the rate of reaction but, importantly, gaseous hydrogen acceptors also have been used. Ethene, propene, and but-1-ene showed up to a fivefold increase in the rate of dehydrogenation. Moreover, compared with the analogous liquid systems, the gaseous alternatives are a potentially more economic method of enhancing the activity and provide a simpler workup. The mechanism for the increase in rate was examined by density functional theory calculations, which showed that the propene hydrogenation competes effectively with the back-hydrogenation of the intermediates formed during the THCZ dehydrogenation, resulting in a shift in the equilibrium toward to the formation of CZ.
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