Dramatic liquid-phase dehydrogenation rate enhancements using gas-phase hydrogen acceptors

Kenneth Hindle, Robbie Burch, Paul Crawford, Christopher Hardacre, Peijun Hu, B. Kalirai, David Rooney

Research output: Contribution to journalArticle

17 Citations (Scopus)

Abstract

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. (C) 2007 Elsevier Inc. All rights reserved.
Original languageEnglish
Pages (from-to)338-344
Number of pages7
JournalJournal of Catalysis
Volume251 (2)
Issue number2
DOIs
Publication statusPublished - 25 Oct 2007

ASJC Scopus subject areas

  • Catalysis
  • Process Chemistry and Technology

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