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Small molecule binding to surface-supported single-site transition-metal reaction centres

Author

Listed:
  • M. DeJong

    (University of British Columbia
    University of British Columbia)

  • A. J. A. Price

    (Dalhousie University)

  • E. Mårsell

    (University of British Columbia)

  • G. Tom

    (University of British Columbia
    University of British Columbia)

  • G. D. Nguyen

    (University of British Columbia)

  • E. R. Johnson

    (Dalhousie University)

  • S. A. Burke

    (University of British Columbia
    University of British Columbia
    University of British Columbia)

Abstract

Despite dominating industrial processes, heterogeneous catalysts remain challenging to characterize and control. This is largely attributable to the diversity of potentially active sites at the catalyst-reactant interface and the complex behaviour that can arise from interactions between active sites. Surface-supported, single-site molecular catalysts aim to bring together benefits of both heterogeneous and homogeneous catalysts, offering easy separability while exploiting molecular design of reactivity, though the presence of a surface is likely to influence reaction mechanisms. Here, we use metal-organic coordination to build reactive Fe-terpyridine sites on the Ag(111) surface and study their activity towards CO and C2H4 gaseous reactants using low-temperature ultrahigh-vacuum scanning tunnelling microscopy, scanning tunnelling spectroscopy, and atomic force microscopy supported by density-functional theory models. Using a site-by-site approach at low temperature to visualize the reaction pathway, we find that reactants bond to the Fe-tpy active sites via surface-bound intermediates, and investigate the role of the substrate in understanding and designing single-site catalysts on metallic supports.

Suggested Citation

  • M. DeJong & A. J. A. Price & E. Mårsell & G. Tom & G. D. Nguyen & E. R. Johnson & S. A. Burke, 2022. "Small molecule binding to surface-supported single-site transition-metal reaction centres," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-35193-6
    DOI: 10.1038/s41467-022-35193-6
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    References listed on IDEAS

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    1. Prokop Hapala & Martin Švec & Oleksandr Stetsovych & Nadine J. van der Heijden & Martin Ondráček & Joost van der Lit & Pingo Mutombo & Ingmar Swart & Pavel Jelínek, 2016. "Mapping the electrostatic force field of single molecules from high-resolution scanning probe images," Nature Communications, Nature, vol. 7(1), pages 1-8, September.
    2. Johannes V. Barth & Giovanni Costantini & Klaus Kern, 2005. "Engineering atomic and molecular nanostructures at surfaces," Nature, Nature, vol. 437(7059), pages 671-679, September.
    3. Cornelius Krull & Marina Castelli & Prokop Hapala & Dhaneesh Kumar & Anton Tadich & Martina Capsoni & Mark T. Edmonds & Jack Hellerstedt & Sarah A. Burke & Pavel Jelinek & Agustin Schiffrin, 2018. "Iron-based trinuclear metal-organic nanostructures on a surface with local charge accumulation," Nature Communications, Nature, vol. 9(1), pages 1-7, December.
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