Escaping scaling relationships for water dissociation at interfacial sites of zirconia-supported Rh and Pt clusters
Kauppinen, M. M., Korpelin, V., Verma, M. A., Melander, M. M., & Honkala, K. (2019). Escaping scaling relationships for water dissociation at interfacial sites of zirconia-supported Rh and Pt clusters. Journal of Chemical Physics, 151(16), Article 164302. https://doi.org/10.1063/1.5126261
Published inJournal of Chemical Physics
© 2019 Author(s)
Water dissociation is an important reaction involved in many industrial processes. In this computational study, the dissociation of water is used as a model reaction for probing the activity of interfacial sites of globally optimized ZrO2 supported Pt and Rh clusters under the framework of density functional theory. Our findings demonstrate that the perimeter sites of these small clusters can activate water, but the dissociation behavior varies considerably between sites. It is shown that the studied clusters break scaling relationships for water dissociation, suggesting that these catalysts may achieve activities beyond the maximum imposed by such relations. Furthermore, we observed large differences in the thermodynamics of the water dissociation reaction between global minimum and near-global minimum isomers of the clusters. Overall, our results highlight the uniqueness of interfacial sites in catalytic reactions and the need for developing new concepts and tools to deal with the associated complexity. ...
PublisherAmerican Institute of Physics
Publication in research information system
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Related funder(s)Academy of Finland
Funding program(s)Postdoctoral Researcher, AoF; Academy Project, AoF
Additional information about fundingThe work was funded by the Academy of Finland, Project Nos. 307853 and 317739, and the University of Jyväskylä. The electronic structure calculations were made possible by the computational resources provided by the CSC—IT Center for Science, Espoo, Finland (https://www.csc.fi/en/). V.K. thanks Mr. Lauri Himanen from Aalto University for fruitful discussions on SOAP.
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