Descriptor-Based Analysis Applied to HCN Synthesis from NH3 and CH4

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The design of solid metal catalysts using theoretical methods has been a long-standing goal in heterogeneous catalysis. Recent developments in methodology and computer technology as well as the establishment of a descriptor-based approach for the analysis of reaction mechanisms and trends across the periodic table allow for the fast screening for new catalytic materials and have lead to first examples of computational discoveries of new materials. The underlying principles of the descriptor-based approach are the existence of relations between the surface electronic structure, adsorption energies and activation barriers that result in volcano-shaped activity plots as function of simple descriptors, such ... continued below

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Grabow, L August 18, 2011.

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The design of solid metal catalysts using theoretical methods has been a long-standing goal in heterogeneous catalysis. Recent developments in methodology and computer technology as well as the establishment of a descriptor-based approach for the analysis of reaction mechanisms and trends across the periodic table allow for the fast screening for new catalytic materials and have lead to first examples of computational discoveries of new materials. The underlying principles of the descriptor-based approach are the existence of relations between the surface electronic structure, adsorption energies and activation barriers that result in volcano-shaped activity plots as function of simple descriptors, such as atomic binding energies or the d-band center. Linear scaling relations have been established between the adsorption energies of hydrogen-containing molecules such as CH{sub x}, NH{sub x}, OH{sub x} and SH{sub x} and the C, N O and S adsorption energies on transition-metal surfaces. Transition-state energies have also been shown to scale linearly with adsorption energies in a similar fashion. Recently, a single transition state scaling relation has been identified for a large number of C-C, C-O, C-N, N-O, N-N, and O-O coupling reactions. The scaling relations provide a powerful tool for the investigation of reaction mechanisms and the prediction of potential energy surfaces. They limit the number of independent variables to a few, typically adsorption energies of key atoms. Using this information as input to a microkinetic model provides an understanding of trends in catalytic activity across the transition metals. In most cases a volcano-shaped relation between activity and the key variables, the descriptors, is observed. In the present paper we will provide an example of the approach outlined above and show how one can obtain an understanding of activity/selectivity trends of a reaction with just a few new calculations.

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  • Journal Name: Submitted to Angewandte Chemie Int. Ed.; Journal Volume: 123; Journal Issue: 20

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  • Report No.: SLAC-PUB-14385
  • Grant Number: AC02-76SF00515
  • DOI: 10.1002/ange.201100353 | External Link
  • Office of Scientific & Technical Information Report Number: 1022511
  • Archival Resource Key: ark:/67531/metadc834191

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  • August 18, 2011

Added to The UNT Digital Library

  • May 19, 2016, 3:16 p.m.

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  • Nov. 23, 2016, 12:43 p.m.

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Grabow, L. Descriptor-Based Analysis Applied to HCN Synthesis from NH3 and CH4, article, August 18, 2011; United States. (digital.library.unt.edu/ark:/67531/metadc834191/: accessed May 23, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.