caa a22 4500 606173846 CHVBK 20210128100735.0 cr unu---uuuuu 210128e20150501xx s 000 0 eng 10.1007/s11244-015-0380-2 doi (NATIONALLICENCE)springer-10.1007/s11244-015-0380-2 Upgrading Light Hydrocarbons: A Tandem Catalytic System for Alkane/Alkene Coupling [Elektronische Daten] [Jay Labinger, David Leitch, John Bercaw, Mark Deimund, Mark Davis] Light hydrocarbons, with relatively low fuel value, are abundant from several sources, including mixed alkane/alkene refinery byproduct streams. A tandem system consisting of a compatible combination of a homogeneous alkane dehydrogenation catalyst (known to be kinetically efficient but thermodynamically disfavored at low temperatures) with an olefin dimerization catalyst could effect the coupling of an alkane and alkene to produce a heavier, more valuable fuel molecule (CnH2n+2+CnH2n=C2nH4n+2), a reaction that is thermodynamically favorable below 250°C. We have demonstrated that coupling with a tandem homogeneous catalyst, consisting of a pincer-ligated iridium alkane dehydrogenation catalyst and an organometallic tantalum alkene dimerization catalyst; the combination couples 1-hexene/n-heptane to C13/C14 products at temperatures ranging from 100 to 150°C, operating with up to 90% cooperativity. This particular combination generates alkene products rather than the desired alkanes, however, because the regioselectivity of the dimerization catalyst preferentially yields highly substituted alkenes that are not reactive towards hydrogen transfer. A complete cycle should be attainable by combining the dehydrogenation catalyst with an alternate dimerization catalyst that gives mostly linear and monosubstituted alkenes; we have synthesized a novel class of nickel-exchanged zincosilicates that exhibit the desired dimerization catalytic behavior. Springer Science+Business Media New York, 2015 Alkane/alkene coupling nationallicence Tandem catalysis nationallicence Alkane dehydrogenation nationallicence Alkene oligomerization nationallicence Light hydrocarbon upgrading nationallicence Labinger Jay Division of Chemistry and Chemical Engineering, California Institute of Technology, 91125, Pasadena, CA, USA aut Leitch David Division of Chemistry and Chemical Engineering, California Institute of Technology, 91125, Pasadena, CA, USA aut Bercaw John Division of Chemistry and Chemical Engineering, California Institute of Technology, 91125, Pasadena, CA, USA aut Deimund Mark Division of Chemistry and Chemical Engineering, California Institute of Technology, 91125, Pasadena, CA, USA aut Davis Mark Division of Chemistry and Chemical Engineering, California Institute of Technology, 91125, Pasadena, CA, USA aut Topics in Catalysis Springer US; http://www.springer-ny.com 58/7-9(2015-05-01), 494-501 1022-5528 58:7-9<494 2015 58 11244 https://doi.org/10.1007/s11244-015-0380-2 text/html Onlinezugriff via DOI BK010053 XK010053 XK010000 Metadata rights reserved Springer special CC-BY-NC licence nationallicence 1 research-article jats NATIONALLICENCE NATIONALLICENCE NL-springer NATIONALLICENCE 856 40 https://doi.org/10.1007/s11244-015-0380-2 text/html Onlinezugriff via DOI NATIONALLICENCE 700 1- Labinger Jay Division of Chemistry and Chemical Engineering, California Institute of Technology, 91125, Pasadena, CA, USA aut NATIONALLICENCE 700 1- Leitch David Division of Chemistry and Chemical Engineering, California Institute of Technology, 91125, Pasadena, CA, USA aut NATIONALLICENCE 700 1- Bercaw John Division of Chemistry and Chemical Engineering, California Institute of Technology, 91125, Pasadena, CA, USA aut NATIONALLICENCE 700 1- Deimund Mark Division of Chemistry and Chemical Engineering, California Institute of Technology, 91125, Pasadena, CA, USA aut NATIONALLICENCE 700 1- Davis Mark Division of Chemistry and Chemical Engineering, California Institute of Technology, 91125, Pasadena, CA, USA aut NATIONALLICENCE 773 0- Topics in Catalysis Springer US; http://www.springer-ny.com 58/7-9(2015-05-01), 494-501 1022-5528 58:7-9<494 2015 58 11244