Olefin oligomerization by main group Ga3+ and Zn2+ single site catalysts on SiO2

Nicole J. LiBretto, Yinan Xu, Aubrey Quigley, Ethan Edwards, Rhea Nargund, Juan Carlos Vega-Vila, Richard Caulkins, Arunima Saxena, Rajamani Gounder, Jeffrey Greeley, Guanghui Zhang () and Jeffrey T. Miller ()
Additional contact information
Nicole J. LiBretto: Purdue University
Yinan Xu: Purdue University
Aubrey Quigley: Purdue University
Ethan Edwards: Purdue University
Rhea Nargund: Purdue University
Juan Carlos Vega-Vila: Purdue University
Richard Caulkins: Purdue University
Arunima Saxena: Purdue University
Rajamani Gounder: Purdue University
Jeffrey Greeley: Purdue University
Guanghui Zhang: Purdue University
Jeffrey T. Miller: Purdue University

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract In heterogeneous catalysis, olefin oligomerization is typically performed on immobilized transition metal ions, such as Ni2+ and Cr3+. Here we report that silica-supported, single site catalysts containing immobilized, main group Zn2+ and Ga3+ ion sites catalyze ethylene and propylene oligomerization to an equilibrium distribution of linear olefins with rates similar to that of Ni2+. The molecular weight distribution of products formed on Zn2+ is similar to Ni2+, while Ga3+ forms higher molecular weight olefins. In situ spectroscopic and computational studies suggest that oligomerization unexpectedly occurs by the Cossee-Arlman mechanism via metal hydride and metal alkyl intermediates formed during olefin insertion and β-hydride elimination elementary steps. Initiation of the catalytic cycle is proposed to occur by heterolytic C-H dissociation of ethylene, which occurs at about 250 °C where oligomerization is catalytically relevant. This work illuminates new chemistry for main group metal catalysts with potential for development of new oligomerization processes.

Date: 2021
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DOI: 10.1038/s41467-021-22512-6

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