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Sheludko, Boris ; Castro, Cristina F. ; Goldman, Alan S. ; Celik, Fuat E. ( , ACS Catalysis)null (Ed.)
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Sheludko, Boris ; Castro, Cristina F. ; Khalap, Chaitanya A. ; Emge, Thomas J. ; Goldman, Alan S. ; Celik, Fuat E. ( , ChemCatChem)
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−
t Bu4POCOP)Ir(CO)] (1 ) and [(≡SiO−i Pr4PCP)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.