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

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 site...

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Bibliographic Details
Published in:Nature communications 2022-12, Vol.13 (1), p.7407-7407, Article 7407
Main Authors: DeJong, M., Price, A. J. A., Mårsell, E., Tom, G., Nguyen, G. D., Johnson, E. R., Burke, S. A.
Format: Article
Language:English
Subjects:
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Atomic force microscopy
Catalysts
Density functional theory
Humanities and Social Sciences
Intermediates
Iron
Low temperature
Microscopy
multidisciplinary
Reaction mechanisms
Scanning tunneling microscopy
Science
Science (multidisciplinary)
Silver
Spectroscopy
Substrates
Transition metals
Ultrahigh temperature
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Summary: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 C 2 H 4 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. Surface-supported metalorganics promise the best of homogenous and heterogeneous catalysts. Here the authors show that small molecules bind to an iron-terpyridine site on silver via surface bound intermediates by following molecules one at a time.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-022-35193-6