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

preprint
submitted on 28.08.2020 and posted on 28.08.2020 by Boris Sheludko, Cristina Castro, Chaitanya Khalap, Thomas Emge, Alan Goldman, Fuat E. Celik
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.

Funding

First-Principles Design of Coke-Resistant Dehydrogenation Catalysts for Valorization of Light Hydrocarbon Feedstocks

Directorate for Engineering

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Alkane Transformations based on Dehydrogenation and Related Reactions: A Tandem Approach

Basic Energy Sciences

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History

Email Address of Submitting Author

fuat.celik@rutgers.edu

Institution

Rutgers, The State University of New Jersey

Country

USA

ORCID For Submitting Author

0000-0002-5891-6375

Declaration of Conflict of Interest

The authors declare no competing interests.

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