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

M. DeJong, A. J. A. Price, E. Mårsell, G. Tom, G. D. Nguyen, E. R. Johnson () and S. A. Burke ()
Additional contact information
M. DeJong: University of British Columbia
A. J. A. Price: Dalhousie University
E. Mårsell: University of British Columbia
G. Tom: University of British Columbia
G. D. Nguyen: University of British Columbia
E. R. Johnson: Dalhousie University
S. A. Burke: University of British Columbia

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-35193-6

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