Regioselective Gas-Phase n-Butane Transfer Dehydrogenation via Silica-Supported Pincer-Iridium Complexes

Boris Sheludko, Cristina F. Castro, Chaitanya A. Khalap, Thomas J. Emge, Alan S. Goldman, Fuat E. Celik

Research output: Contribution to journalArticlepeer-review

Abstract

The production of olefins via on-purpose dehydrogenation of alkanes allows for a more efficient, selective and lower cost alternative to processes such as steam cracking. Silica-supported pincer-iridium complexes of the form [(≡SiO−R4POCOP)Ir(CO)] (R4POCOP=κ3-C6H3-2,6-(OPR2)2) are effective for acceptorless alkane dehydrogenation, and have been shown stable up to 300 °C. However, while solution-phase analogues of such species have demonstrated high regioselectivity for terminal olefin production under transfer dehydrogenation conditions at or below 240 °C, in open systems at 300 °C, regioselectivity under acceptorless dehydrogenation conditions is consistently low. In this work, complexes [(≡SiO−tBu4POCOP)Ir(CO)] (1) and [(≡SiO−iPr4PCP)Ir(CO)] (2) were synthesized via immobilization of molecular precursors. These complexes were used for gas-phase butane transfer dehydrogenation using increasingly sterically demanding olefins, resulting in observed selectivities of up to 77 %. The results indicate that the active site is conserved upon immobilization.

Original languageEnglish (US)
Pages (from-to)407-415
Number of pages9
JournalChemCatChem
Volume13
Issue number1
DOIs
StatePublished - Jan 12 2021

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Physical and Theoretical Chemistry
  • Organic Chemistry
  • Inorganic Chemistry

Keywords

  • dehydrogenation
  • heterogeneous catalysis
  • hydrogen transfer
  • iridium
  • supported catalysts

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