jp9b08662_si_001.pdf (1.19 MB)
Volcano Curves for in Silico Prediction of Mono- and Bifunctional Catalysts: Application to Ammonia Decomposition
journal contribution
posted on 2019-10-28, 15:38 authored by Hongbo Wu, Jonathan E. Sutton, Wei Guo, Dionisios G. VlachosComputational
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.
History
Usage metrics
Categories
Keywords
FPMonte CarloKMC methodmicrostructuremonofunctional materialsvolcano curveAmmonia Decomposition Computational screeningbimetallic facetsmaterials exhibitSR-MKMVolcano CurvesSilico PredictionKMC calculationsBifunctional CatalystsSR-KMC volcanosDual siteammonia decompositionmultifunctional catalystsmodel
Licence
Exports
RefWorks
BibTeX
Ref. manager
Endnote
DataCite
NLM
DC