10.1021/acs.jpcc.9b08662.s001
Hongbo Wu
Hongbo
Wu
Jonathan E. Sutton
Jonathan E.
Sutton
Wei Guo
Wei
Guo
Dionisios G. Vlachos
Dionisios G.
Vlachos
Volcano Curves for in Silico Prediction of Mono- and
Bifunctional Catalysts: Application to Ammonia Decomposition
American Chemical Society
2019
FP
Monte Carlo
KMC method
microstructure
monofunctional materials
volcano curve
Ammonia Decomposition Computational screening
bimetallic facets
materials exhibit
SR-MKM
Volcano Curves
Silico Prediction
KMC calculations
Bifunctional Catalysts
SR-KMC volcanos
Dual site
ammonia decomposition
multifunctional catalysts
model
2019-10-28 15:38:21
Journal contribution
https://acs.figshare.com/articles/journal_contribution/Volcano_Curves_for_in_Silico_Prediction_of_Mono-_and_Bifunctional_Catalysts_Application_to_Ammonia_Decomposition/10060157
Computational
screening of catalysts with complex microstructures
and/or multiple interacting sites is challenging. Here, we evaluate
the ammonia decomposition on perfect and patched core–shell
bimetallic facets using a hierarchy of kinetic models, namely, scaling
relations (SRs)-based mean-field microkinetic models (SR-MKM), and
first-principles (FP) and SR-based spatially resolved kinetic Monte
Carlo (FP- and SR-KMC) simulations. SR-KMC volcanos possess a double-peak
on perfect facets and a single peak on patched bimetallic facets.
When lateral interactions of the most abundant surface intermediate
are strong, only the KMC method predicts the volcano accurately. Dual
site (bifunctional) materials exhibit a considerably different volcano
curve from monofunctional materials and thus, multifunctional materials’
property prediction requires KMC calculations. Our computational screening
highlights the importance of the microstructure of multifunctional
catalysts.