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

Author

Listed:
  • 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
    Dalian University of Technology)

  • Jeffrey T. Miller

    (Purdue University)

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.

Suggested Citation

  • 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 & Jeffre, 2021. "Olefin oligomerization by main group Ga3+ and Zn2+ single site catalysts on SiO2," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-22512-6
    DOI: 10.1038/s41467-021-22512-6
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    Cited by:

    1. Zijun Huang & Dedong He & Weihua Deng & Guowu Jin & Ke Li & Yongming Luo, 2023. "Illustrating new understanding of adsorbed water on silica for inducing tetrahedral cobalt(II) for propane dehydrogenation," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Qiyuan Zhao & Yinan Xu & Jeffrey Greeley & Brett M. Savoie, 2022. "Deep reaction network exploration at a heterogeneous catalytic interface," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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