Abstract
In this study, we used a combination of diffusion Monte Carlo and density functional theory calculations to investigate the stability and interlayer binding of various layered structures of Pt atoms adsorbed on graphene. Our findings show that vertically buckled Pt monolayer and bilayer with (111)-packing order are more energetically favorable than the corresponding buckled (100) or flat (100)-packing structures. This can be attributed to the significant lattice mismatch (>10%) between pristine graphene and a free-standing (100)-packing Pt layer. Additionally, our calculations reveal that among the (100)-packing Pt layers, an incommensurate structure with a Pt/C atomic ratio less than 1/2 may be more stable than the commensurate structures registered at the bridge sites, which aligns with recent experimental findings of incommensurate (100)-packing Pt layers on graphene. The interlayer binding between the Pt layer and graphene is found to be primarily driven by van der Waals interaction, except for the AA-stacked buckled-(100) Pt bilayer where the bottom Pt atoms show chemisorption to the graphene surface. This research offers a comprehensive examination of the stability and interlayer binding of metallic Pt layers, providing valuable insights for potential applications as a next-generation catalyst.
Original language | English |
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Pages (from-to) | 18630-18640 |
Number of pages | 11 |
Journal | Journal of Physical Chemistry C |
Volume | 127 |
Issue number | 37 |
DOIs | |
State | Published - Sep 21 2023 |
Funding
Initial work on this paper was supported by Konkuk University Researcher Fund in 2019. Y.K. was supported by the Basic Science Research Program (2018R1D1A1B07042443) through the National Research Foundation of Korea funded by the Ministry of Education. We also acknowledge the support from the Supercomputing Center/Korea Institute of Science and Technology Information with supercomputing resources including technical support (KSC-2020-CRE-0126). Final work (incommensurate calculations, manuscript writing) by J.A. and J.T.K. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, as part of the Computational Materials Sciences Program and Center for Predictive Simulation of Functional Materials. H.S. and A.B. (preparation of vdW-corrected DFT simulations, analysis and validation of results, editing and reviewing the manuscript) were also supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, as part of the Computational Materials Sciences Program and Center for Predictive Simulation of Functional Materials. An award of computer time was provided by the Innovative and Novel Computational Impact on Theory and Experiment (INCITE) program. This research used resources of the Argonne Leadership Computing Facility, which is a DOE Office of Science User Facility supported under contract DE-AC02-06CH11357. This research also used resources of the Oak Ridge Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract DE-AC05-00OR22725. This manuscript has been authored by UT-Battelle, LLC under contract no. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Initial work on this paper was supported by Konkuk University Researcher Fund in 2019. Y.K. was supported by the Basic Science Research Program (2018R1D1A1B07042443) through the National Research Foundation of Korea funded by the Ministry of Education. We also acknowledge the support from the Supercomputing Center/Korea Institute of Science and Technology Information with supercomputing resources including technical support (KSC-2020-CRE-0126). Final work (incommensurate calculations, manuscript writing) by J.A. and J.T.K. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, as part of the Computational Materials Sciences Program and Center for Predictive Simulation of Functional Materials. H.S. and A.B. (preparation of vdW-corrected DFT simulations, analysis and validation of results, editing and reviewing the manuscript) were also supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, as part of the Computational Materials Sciences Program and Center for Predictive Simulation of Functional Materials. An award of computer time was provided by the Innovative and Novel Computational Impact on Theory and Experiment (INCITE) program. This research used resources of the Argonne Leadership Computing Facility, which is a DOE Office of Science User Facility supported under contract DE-AC02-06CH11357. This research also used resources of the Oak Ridge Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract DE-AC05-00OR22725. This manuscript has been authored by UT-Battelle, LLC under contract no. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).