Photocatalytic acceptorless alkane dehydrogenation: Scope, mechanism, and conquering deactivation with carbon dioxide

Abhishek Dutta Chowdhury, J. J. Jennifer Julis, Kathleen Grabow, Bernd Hannebauer, Ursula Bentrup, Martin Adam, Robert Franke, Ralf Jackstell, Matthias Beller

Research output: Contribution to journalArticlepeer-review

20 Scopus citations

Abstract

Alkane dehydrogenation is of special interest for basic science but also offers interesting opportunities for industry. The existing dehydrogenation methodologies make use of heterogeneous catalysts, which suffer from harsh reaction conditions and a lack of selectivity, whereas homogeneous methodologies rely mostly on unsolicited waste generation from hydrogen acceptors. Conversely, acceptorless photochemical alkane dehydrogenation in the presence of trans-Rh(PMe3 )2(CO)Cl can be regarded as a more benign and atom efficient alternative. However, this methodology suffers from catalyst deactivation over time. Herein, we provide a detailed investigation of the trans -Rh(PMe3)2(CO)Cl-photocatalyzed alkane dehydrogenation using spectroscopic and theoretical investigations. These studies inspired us to utilize CO2 to prevent catalyst deactivation, which leads eventually to improved catalyst turnover numbers in the dehydrogenation of alkanes that include liquid organic hydrogen carriers.

Original languageEnglish
Pages (from-to)323-330
Number of pages8
JournalChemSusChem
Volume8
Issue number2
DOIs
StatePublished - Jan 2015
Externally publishedYes

Keywords

  • Alkanes
  • Dehydrogenation
  • Homogeneous catalysis
  • Photochemistry
  • Rhodium

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