Predicting the Electric Field Effect on the Lateral Interactions Between Adsorbates: O/Fe(100) from First Principles
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A density functional theory parameterized lattice gas cluster expansion of oxygen on an Fe(100) surface is developed in the presence and absence of an applied positive and negative external electric field, characterizing the heterogeneity in oxygen’s surface distribution and the effect of an external electric field on the lateral interactions between the adsorbates. We show that the presence of a negative electric field tends to weaken both attractive and repulsive interactions while the positive electric field tends to strengthen these interactions, altering surface distributions and ground state configurations. Since lateral interactions have been shown to play a critical role in defining catalytic behavior, the application of an applied electric field has the potential to be a useful tool in adjusting critical chemical properties of Fe-based hydrodeoxygenation catalysts, by decreasing the repulsive interactions between the adspecies in the presence of a negative field and thereby mitigating the formation of an oxide.
KeywordsLattice gas model Electric field Mean field model Hydrodeoxygenation Iron Oxygen
J.B. and J.-S.M. were primarily funded by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences (DE-SC0014560). G.C., NSF Graduate Research Fellow, gratefully acknowledges financial support from the National Science Foundation Graduate Research Fellowship Program. G.C. also acknowledges the NSF EAPSI fellowship program under award number 1613890. J.B., Seattle Chapter ARCS Fellow, gratefully acknowledges financial support from the Achievement Rewards for College Scientists Foundation. The Pacific Northwest National Laboratory is operated by Battelle for the U.S. DOE.
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