The Diffusion and Clustering Formation of Gold Atoms on Alpha-Graphyne

Motivated by the experiment, high mobility of gold atoms on two-dimensional carbon sheets, we examine the ground-state structures, mobility, and clustering formations of small gold clusters (Au_n, n = 1-4) on monolayer alpha-graphyne using first-principles DFT calculations and finite temperature MD simulations. We reveal that Au_n cluster prefers to locate at the center of a hexagon in alpha-graphyne. The binding energy of Au_n on alpha-graphyne increases with increasing the number (n) of gold atoms. Moreover, we predict the step-wise formation of Au_2 out of two pre-adsorbed Au_1 ad-atoms. Likewise, the formation of Au_3 and Au_4 is also considered in the same way. The diffusion energy barrier of Au_1 on alpha-graphyne is found to be only 0.26 eV, indicating the high mobility of gold atoms on alpha-graphyne. Remarkably, the energy required for the cluster formation of gold atoms on alpha-graphyne is about less than 0.2 eV. According to our MD simulations at room temperature (RT), the Au_n cluster is subsequently formed on alpha-graphyne. Considering the high mobility of a single gold atom, the strong binding energy of small gold clusters, and the easy clustering of Au_n at RT on alpha-graphyne, we suggest that alpha-graphyne is a suitable substrate for gold cluster formation.

Keywords:

Clustering formation, diffusion, gold adsorption, graphyne two-dimensional materials,

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Amft M, Sanyal B, Eriksson O, Skorodumova NV, 2011. Small Gold Clusters on Graphene, their Mobility and Clustering: a DFT Study. Journal of Physics: Condensed Matter, 23: 205301.
Azizi E, Tehrani ZA, Jamshidi Z, Interactions of Small Gold Clusters, Aun (n=1–3), with Graphyne: Theoretical Investigation, 2014. Journal of Molecular Graphics and Modelling, 54: 80.
Baughman RH, Eckhardt H, Kertesz M, 1987. Structure‐Property Predictions for New Planar Forms of Carbon: Layered Phases Containing s p 2 and s p Atoms. The Journal of Chemical Physics, 87: 6687.
Blochl PE, 1994. Projector Augmented-Wave Method. Physical Review B, 50: 17953.
Carara SS, Batista RJC, Chacham H, 2009. Modifications in Graphene Electron States Due to a Deposited Lattice of Au Nanoparticles: Density Functional Calculations. Physical Review B, 80: 115435.
Chen D, Tang J, Zhang X, Cui H, Li Y, 2018. Sulfur Dioxide Adsorbed on Pristine and Au Dimer Decorated γ-Graphyne: A Density Functional Theory Study, Applied Surface Science, 458: 781. Cranford SW, Buehler MJ, 2012. Selective Hydrogen Purification Through Graphdiyne under Ambient Temperature and Pressure. Nanoscale, 4: 4587.
Foiles SM, Baskes MI, Daw MS, 1986. Embedded-Atom-Method Functions for the Fcc Metals Cu, Ag, Au, Ni, Pd, Pt, and their Alloys. Physical Review B, 33: 7983.
Grimme S, 2006. Semiempirical GGA-Type Density Functional Constructed with a Long-Range Dispersion Correction. Journal of Computational Chemistry, 27: 1787.
Guo Y, Jiang K, Xu B, Xia Y, Yin J, Liu Z, 2012. Remarkable Hydrogen Storage Capacity in Li-Decorated Graphyne: Theoretical Predication, The Journal of Physical Chemistry C, 116: 13837.
Haley MM, Brand SC, Pak JJ, 1997. Carbon Networks Based on Dehydrobenzoannulenes: Synthesis of Graphdiyne Substructures. Angewandte Chemie International Edition, 36: 836.
Henkelman G, Uberuaga BP, Jonsson HA, 2000. Climbing Image Nudged Elastic Band Method for Finding Saddle Points and Minimum Energy Paths. The Journal of Chemical Physics, 113: 9901.
Hoover WG, 1985. Canonical Dynamics: Equilibrium Phase-Space Distributions. Physical Review A, 31: 1695.
Ipek S, Kilic ME, Mogulkoc A, Cahangirov S, Durgun E, 2018. Semiconducting Defect-Free Polymorph of Borophene: Peierls Distortion in Two-Dimensions. Physical Review B, 98: 241408.
Jensen P, Blase X, Ordejon P, 2004. First-Principles Study of Gold Adsorption and Diffusion on Graphite. Surfice Science, 564: 173.
Johnson CA, Lu Y, Haley MM, 2007. Carbon Networks Based on Benzocyclynes. 6. Synthesis of Graphyne Substructures via Directed Alkyne Metathesis. Organic Letters, 9: 3725.
Kilic ME, Erkoc S, 2016. Structural Properties of Pristine and Defected ZnO Nanosheets under Biaxial Strain: Molecular Dynamics Simulations. Journal of Nanoscience and Nanotechnology, 16: 1506.
Kilic ME, Lee K-R, 2020. Tuning the Electronic, Mechanical, Thermal, and Optical Properties of Tetrahexcarbon via Hydrogenation, Carbon, 161: 71.
Kilic ME, Lee K-R, 2020. First-principles Study of Fluorinated Tetrahexcarbon: Stable Configurations, Thermal, Mechanical, and Electronic Properties, The Journal of Physical Chemistry C, 124: 8225
Kilic ME, Lee K-R, 2021. Tetrahex Carbides: Two-dimensional Group-IV Materials for Nanoelectronics and Photocatalytic Water Splitting, Carbon, 174: 368.
Kaner RB, 2005. Material Science: Designing Superhard Materials. Science, 308: 1268.
Kim BG, Choi HJ, 2012. Graphyne: Hexagonal Network of Carbon with Versatile Dirac Cones. Physical Review B, 86: 115435.
Kresse G, Hafner J, 1994. Norm-Conserving and Ultrasoft Pseudopotentials for First-Row and Transition Elements, Journal of Physics: Condensed Matter, 6: 8245.
Kresse G, Joubert D, 1999. From Ultrasoft Pseudopotentials to the Projector Augmented-Wave Method. Physical Review B, 59: 1758.
Kong X, Huang Y, Liu Q, 2017. Two-Dimensional Boron-Doped Graphyne Nanosheet: A New Metal-Free Catalyst for Oxygen Evolution Reaction. Carbon, 123: 558.
Kou J, Zhou X, Lu H, Wu F, Fan J, 2014. Graphyne as the Membrane for Water Desalination, Nanoscale, 6: 1865.
Li C, Li J, Wu F, Li S-S, Xia J-B, Wang L-W, 2011. High Capacity Hydrogen Storage in Ca Decorated Graphyne: a First-Principles Study. The Journal of Physical Chemistry C, 115: 23221.
Li G, Li Y, Liu H, Guo Y, Li Y, Zhu D, 2010. Architecture of Graphdiyne Nanoscale Films. Chemical Communications, 46: 3256.
Luedtke WD, Landman U, 1999. Slip Diffusion and Lévy Flights of an Adsorbed Gold Nanocluster. Physical Review Letter, 82: 3835.
Ma DW, Li T, Wang Q, Yang G, He C, Ma B, Lu Z, 2015. Graphyne As a Promising Substrate for the Noble-Metal Single-Atom Catalysts. Carbon, 95: 756.
McCreary KM, Pi K, Swartz AG, Han W, Bao W, Lau CN, Guinea F, Katsnelson MI, Kawakami RK, 2010. Effect of Cluster Formation on Graphene Mobility. Physical Review B, 81: 115453.
Monkhorst HJ, Pack JD, 1976. Special Points for Brillouin-Zone Integrations. Physical Review B, 13: 5188.
Morshedloo T, Roknabadi MR, Behdani M, Modarresi M, Kazempour A, 2016. First Principle Study of Inducing Superconductivity in α-Graphyne by Hole-Doping and Biaxial Tensile Strain. Computational Material Science, 124: 183.
Nose S, 1984. A Unified Formulation of the Constant Temperature Molecular Dynamics Methods. The Journal of Chemical Physics, 81: 511.
Nose S, 1984, A Molecular Dynamics Method for Simulations in the Canonical Ensemble. Molecular Physics, 52: 255.
Novoselov KS, 2004. Electric Field Effect in Atomically Thin Carbon Films. Science, 306: 666.
Novoselov KS, Geim AK, Morozov S, Jiang D, Katsnelson MI, Grigorieva IV, Dubonos SV, Firsov AA, 2005. Two-Dimensional Gas of Massless Dirac Fermions in Graphene. Nature, 438: 197.
Okamoto H, Kumai Y, Sugiyama Y, Mitsuoka T, Nakanishi K, Ohta T, Nozaki H, Yamaguchi S, Shirai S, Nakano H, 2010. Silicon Nanosheets and their Self-Assembled Regular Stacking Structure. Journal of the American Chemical Society, 132: 2710.
Pekoz R, Konuk M, Kilic ME, Durgun E, 2018. Two-Dimensional Fluorinated Boron Sheets: Mechanical, Electronic, and Thermal Properties. ACS Omega, 3: 1815.
Perdew JP, Burke K, Ernzerhof M, 1996. Generalized Gradient Approximation Made Simple, Physical Review Letter, 77: 3865.
Plimpton S, 1995. Fast Parallel Algorithms for Short-Range Molecular Dynamics. Journal of Computational Physics, 117: 1.
Stuart SJ, Tutein AB, Harrison JA, 2000. A Reactive Potential for Hydrocarbons with Intermolecular Interactions. The Journal of Chemical Physics., 112: 6472.
Togo A, Chaput L, Tanaka I, 2015. Distributions of Phonon Lifetimes in Brillouin Zones. Physical Review B, 91, 094306.
Wang GM, BelBruno JJ, Kenny SD, Smith R, 2004. Gold Adatoms and Dimers on Relaxed Graphite Surfaces. Physical Review B, 69: 195412.
Wang GM, BelBruno JJ, Kenny SD, Smith R, 2005. Density Functional Study of Aun (n=3–5) Clusters on Relaxed Graphite Surfaces. Surface Science, 576: 107.
Wang T, Huang J, Lv H, Fan Q, Feng L, Tao Z, Ju H, Wu X, Tait SL, Zhu J, 2018. Kinetic Strategies for the Formation of Graphyne Nanowires via Sonogashira Coupling on Ag (111). Journal of the American Chemical Society, 140: 13421.
Yan J-A, Ruan WY, Chou MY, 2008. Phonon Dispersions and Vibrational Properties of Monolayer, Bilayer, and Trilayer Graphene: Density-Functional Perturbation Theory. Physical Review B, 77: 125401.
Zhang Y, Tan Y-W, Stormer HL, Kim P, 2005. Experimental Observation of the Quantum Hall Effect and Berry’s Phase in Graphene. Nature, 438: 201.