Carbon monoxide-induced adatom sintering in a Pd-Fe3O4 model catalyst

G.S. Parkinson, Z. Novotny, G. Argentero, M. Schmid, J. Pavelec, R. Kosak, P. Blaha, U. Diebold

Institut für Angewandte Physik, Technische Universität Wien, 1040 Wien, Austria
Institute of Materials Chemistry, Technische Universität Wien, 1060 Wien, Austria

Nature Mater. 12 (2013) 724-728

The coarsening of catalytically-active metal clusters is often accelerated by the presence of gases, but the role played by gas molecules is difficult to ascertain and varies from system to system. We use scanning tunneling microscopy (STM) to follow the CO-induced coalescence of Pd adatoms supported on the Fe3O4(001) surface at room temperature, and find Pd-carbonyl species to be responsible for mobility in this system. Once these reach a critical density, clusters nucleate; subsequent coarsening occurs through cluster diffusion and coalescence. Whereas CO induces the mobility in the Pd/Fe3O4 system, surface hydroxyls have the opposite effect. Pd atoms transported to surface OH groups are no longer susceptible to carbonyl formation and remain isolated. Following the evolution from well-dispersed metal adatoms into clusters, atom-by-atom, allows identification of the key processes that underlie gas-induced mass transport.

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A preprint of the paper is available at cond-mat/1303.0664.

Reprints available from G.S. Parkinson (parkinson< encoded email address >).