TY - JOUR
T1 - Predicting Monolayer Oxide Stability over Low-Index Surfaces of TiO2 Polymorphs Using ab Initio Thermodynamics
AU - Jonayat, A. S.M.
AU - Chen, Siqi
AU - Van Duin, Adri C.T.
AU - Janik, Michael
N1 - Funding Information:
This work used the Extreme Science and Engineering Discovery Environment (XSEDE),77 which is supported by the National Science Foundation under grant no. ACI-1548562. A.S.M.J. acknowledges training provided by the Computational Materials Education and Training (CoMET) NSF Research Traineeship (grant number DGE-1449785).
Funding Information:
This material is based upon work supported by the National Science Foundation under grant no. 1505607. This work used the Extreme Science and Engineering Discovery Environment (XSEDE),77 which is supported by the National Science Foundation under grant no. ACI-1548562. A.S.M.J. acknowledges training provided by the Computational Materials Education and Training (CoMET) NSF Research Traineeship (grant number DGE-1449785).
Publisher Copyright:
© Copyright 2018 American Chemical Society.
PY - 2018/10/2
Y1 - 2018/10/2
N2 - Monolayer metal oxide coatings on metal oxide supports have the possibility of tuning the surface chemical properties of the coated systems. However, the (meta)stability of these structures makes experimental discovery challenging. A computational approach can help to determine properties that make a coating/substrate system stable and evaluate the stability of a variety of combinations. Herein, we use density functional theory (DFT) to study the stability of monolayer transitional metal oxides over different facets of anatase, brookite, and rutile phase of TiO2. We find that coatings that have a stable polymorph matching that of the support, as well as substrates with higher surface energies, are more likely to form monolayer-coated systems. DFT calculations recommend a number of coating/TiO2 surface facet combinations that may be stable. Despite these predictive observations, we did not find a significant correlation between monolayer stability and a single atomic, surface, or structural property of the coating/support metal/metal oxide and coating oxide monolayer stability. More complex predictive relationships need future study.
AB - Monolayer metal oxide coatings on metal oxide supports have the possibility of tuning the surface chemical properties of the coated systems. However, the (meta)stability of these structures makes experimental discovery challenging. A computational approach can help to determine properties that make a coating/substrate system stable and evaluate the stability of a variety of combinations. Herein, we use density functional theory (DFT) to study the stability of monolayer transitional metal oxides over different facets of anatase, brookite, and rutile phase of TiO2. We find that coatings that have a stable polymorph matching that of the support, as well as substrates with higher surface energies, are more likely to form monolayer-coated systems. DFT calculations recommend a number of coating/TiO2 surface facet combinations that may be stable. Despite these predictive observations, we did not find a significant correlation between monolayer stability and a single atomic, surface, or structural property of the coating/support metal/metal oxide and coating oxide monolayer stability. More complex predictive relationships need future study.
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U2 - 10.1021/acs.langmuir.8b02426
DO - 10.1021/acs.langmuir.8b02426
M3 - Article
C2 - 30168723
AN - SCOPUS:85053710820
SN - 0743-7463
VL - 34
SP - 11685
EP - 11694
JO - Langmuir
JF - Langmuir
IS - 39
ER -