Alkane activation over acidic zeolites: the first step.

Chemistry

Laboratoire des Matériaux Surfaces et Procédés pour la Catalyse, Member of ELCASS (European Laboratory for Catalysis and Surface Sciences), UMR 7515 CNRS, 25 rue Becquerel 67087 Strasbourg Cedex 2, France.

Published: January 2010

AI Article Synopsis

  • The activation of alkanes through heterogeneous acid catalysis has been debated for a long time, particularly regarding the formation of reaction intermediates like carbocations and alkoxies.
  • Recent experiments using gas chromatography and online mass spectrometry show that H(2) and methane are produced when using H-zeolites, while D-zeolites yield HD and CH(3)D as primary products, specifically when reacting with isobutane.
  • The findings suggest that sigma-bond protolysis by strong acid sites is the initial step in hydrocarbon activation on these catalysts at mild temperatures, similar to the processes that happen in liquid superacid conditions.

Article Abstract

The heterogeneous acid-catalyzed activation step of alkanes leading to the reaction intermediates (carbocationic or alkoxy species) was up to now the matter of a longstanding controversy. Gas chromatography and online mass spectroscopy measurements show that H(2) and methane are formed over H-zeolites, whereas HD and CH(3)D are formed over D-zeolites as the primary products in the reaction with isobutane. These results indicate that sigma-bond protolysis by strong acid sites is the first step for hydrocarbon activation on these catalysts at mild temperatures (473 K), in analogy to the activation path occurring in liquid superacid media.

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Source
http://dx.doi.org/10.1002/chem.200901737DOI Listing

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