Introducing structural sensitivity into adsorption–energy scaling relations by means of coordination numbers
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- 6 April 2015
- journal article
- research article
- Published by Springer Nature in Nature Chemistry
- Vol. 7 (5), 403-410
- https://doi.org/10.1038/nchem.2226
Abstract
The search for improved heterogeneous catalysts is an important but difficult task. Scaling relations between the adsorption energies of reaction intermediates greatly facilitate the computational design of catalysts. However, this methodology does not currently incorporate structure sensitivity and hence cannot describe adequately the overall activity of realistic catalyst particles and extended surfaces with several facets, edges and apices. Here, we generalize scaling relations by examining twelve different low-index, stepped and kinked surfaces of nine transition metals. This allows us to quantify the effect of the adsorption-site geometry on these relations, ensures a full prediction of their parameters, and helps in identifying intrinsic thermodynamic restrictions to the performance of catalysts. The resulting fully predictable, structure-sensitive scaling relations are a step towards the long-sought rational design of multifaceted catalytic particles. Such a design can now target not only the chemical nature of active materials but also the actual geometry of their active sites.Keywords
This publication has 53 references indexed in Scilit:
- Theoretical Considerations on the Electroreduction of CO to C2 Species on Cu(100) ElectrodesAngewandte Chemie International Edition, 2013
- Selectivity of CO2 Reduction on Copper Electrodes: The Role of the Kinetics of Elementary StepsAngewandte Chemie International Edition, 2013
- Understanding Trends in the Electrocatalytic Activity of Metals and Enzymes for CO2 Reduction to COThe Journal of Physical Chemistry Letters, 2013
- Number of outer electrons as descriptor for adsorption processes on transition metals and their oxidesChemical Science, 2013
- Understanding the electrocatalysis of oxygen reduction on platinum and its alloysEnergy & Environmental Science, 2012
- CatApp: A Web Application for Surface Chemistry and Heterogeneous CatalysisAngewandte Chemie International Edition, 2011
- Universal transition state scaling relations for (de)hydrogenation over transition metalsPhysical Chemistry Chemical Physics, 2011
- Theory of the Kinetics of Chemical Potentials in Heterogeneous CatalysisAngewandte Chemie International Edition, 2011
- Thermodynamic theory of multi-electron transfer reactions: Implications for electrocatalysisJournal of Electroanalytical Chemistry, 2010
- Ammonia Selective Oxidation on Pt(100) Sites in an Alkaline MediumThe Journal of Physical Chemistry B, 2005