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Reaction cycles and poisoning in catalysis by gold clusters: a thermodynamics approach

MPG-Autoren
http://pubman.mpdl.mpg.de/cone/persons/resource/persons21355

Beret,  Elizabeth C.
Theory, Fritz Haber Institute, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons22193

Wijk,  Merel van
Theory, Fritz Haber Institute, Max Planck Society;
Radboud University;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons21549

Ghiringhelli,  Luca M.
Theory, Fritz Haber Institute, Max Planck Society;

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Zitation

Beret, E. C., Wijk, M. v., & Ghiringhelli, L. M. (2014). Reaction cycles and poisoning in catalysis by gold clusters: a thermodynamics approach. International Journal of Quantum Chemistry, 114(1), 57-65. doi:10.1002/qua.24503.


Zitierlink: http://hdl.handle.net/11858/00-001M-0000-0013-F74F-B
Zusammenfassung
In heterogeneous catalysis, a catalytic process takes place at nite temperature and at nite pressure of the atmosphere of the reactant gases. By applying ab initio atom- istic thermodynamics to the model case of free Au2 and Au-2 clusters in an atmosphere of O2 and CO, we derive all the thermodynamically possible reaction paths for the ox- idation of CO to COV. This analysis lets us explain how gold clusters enable oxidation reactions without breaking the spin-conservation rule. Furthermore, we identify special cluster+ligands compositions such as reaction intermediates and poisoned species. In particular, a thermodynamically driven poisoning is identied for the catalytic system containing free Au2 , and the experimental (p; T) conditions that avoid its formation are suggested. This implies that for some systems a catalytic cycle can be established, on thermodynamics grounds, only in a dened range of temperatures and pressures. In addition, our predictions for Au-2 provide the so far most complete interpretation of the available experimental data [Socaciu et al, J. Am. Chem. Soc. 125, 10437 (2003)].