skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

This content will become publicly available on August 29, 2020

Title: Kinetic Monte Carlo Simulations Unveil Synergic Effects at Work on Bifunctional Catalysts

Abstract

The interaction among metal particles and the support in heterogeneous catalysis has been the subject of a large number of studies. Although strong metal–support interactions can lead to deleterious catalyst deactivation and the underlying mechanism is well understood, in other cases the effect may beneficially enhance the catalytic activity and/or selectivity with no clear picture of the chemistry involved. Strong metal–support interactions make Au nanoparticles dispersed on MoC a highly active catalyst for the low-temperature water-gas shift reaction (WGSR). In this work, by using kinetic Monte Carlo (kMC) simulations, we unravel the origin of the experimentally observed high WGSR activity of Au/MoC. The kMC simulations provide strong evidence for a cooperative effect between the different regions of the catalyst: the clean MoC regions are responsible for adsorbing and dissociating water molecules, and the vicinity of the Au adclusters contributes to COOH formation. The information thus obtained goes beyond that obtained solely from free-energy landscapes and constitutes a step forward toward the rational design of catalysts. Importantly, the simulations and analysis described here are general and can be applied to other complex systems involving different catalytic regions and a large number of surface processes.

Authors:
 [1];  [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Universitat de Barcelona (Spain)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1566288
Report Number(s):
BNL-212097-2019-JAAM
Journal ID: ISSN 2155-5435
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 9; Journal Issue: 10; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; kMC; synergic effects; bifunctional catalysts; WGSR; reaction mechanisms; transition-metal carbides

Citation Formats

Prats, Hèctor, Posada-Pérez, Sergio, Rodriguez, José A., Sayós, Ramón, and Illas, Francesc. Kinetic Monte Carlo Simulations Unveil Synergic Effects at Work on Bifunctional Catalysts. United States: N. p., 2019. Web. doi:10.1021/acscatal.9b02813.
Prats, Hèctor, Posada-Pérez, Sergio, Rodriguez, José A., Sayós, Ramón, & Illas, Francesc. Kinetic Monte Carlo Simulations Unveil Synergic Effects at Work on Bifunctional Catalysts. United States. doi:10.1021/acscatal.9b02813.
Prats, Hèctor, Posada-Pérez, Sergio, Rodriguez, José A., Sayós, Ramón, and Illas, Francesc. Thu . "Kinetic Monte Carlo Simulations Unveil Synergic Effects at Work on Bifunctional Catalysts". United States. doi:10.1021/acscatal.9b02813.
@article{osti_1566288,
title = {Kinetic Monte Carlo Simulations Unveil Synergic Effects at Work on Bifunctional Catalysts},
author = {Prats, Hèctor and Posada-Pérez, Sergio and Rodriguez, José A. and Sayós, Ramón and Illas, Francesc},
abstractNote = {The interaction among metal particles and the support in heterogeneous catalysis has been the subject of a large number of studies. Although strong metal–support interactions can lead to deleterious catalyst deactivation and the underlying mechanism is well understood, in other cases the effect may beneficially enhance the catalytic activity and/or selectivity with no clear picture of the chemistry involved. Strong metal–support interactions make Au nanoparticles dispersed on MoC a highly active catalyst for the low-temperature water-gas shift reaction (WGSR). In this work, by using kinetic Monte Carlo (kMC) simulations, we unravel the origin of the experimentally observed high WGSR activity of Au/MoC. The kMC simulations provide strong evidence for a cooperative effect between the different regions of the catalyst: the clean MoC regions are responsible for adsorbing and dissociating water molecules, and the vicinity of the Au adclusters contributes to COOH formation. The information thus obtained goes beyond that obtained solely from free-energy landscapes and constitutes a step forward toward the rational design of catalysts. Importantly, the simulations and analysis described here are general and can be applied to other complex systems involving different catalytic regions and a large number of surface processes.},
doi = {10.1021/acscatal.9b02813},
journal = {ACS Catalysis},
number = 10,
volume = 9,
place = {United States},
year = {2019},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on August 29, 2020
Publisher's Version of Record

Save / Share: