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Exciting H2 Molecules for Graphene Functionalization

Abstract : Hydrogen functionalization of graphene by exposure to vibrationally excited H2 molecules is investigated by combined scanning tunneling microscopy, high resolution electron energy loss spectroscopy, x-ray photoemission spectroscopy measurements and density functional theory calculations. The measurements reveal that vibrationally excited H2 molecules dissociatively adsorb on graphene on Ir(111) resulting in nano-patterned hydrogen functionalization structures. Calculations demonstrate that the presence of the Ir surface below the graphene lowersthe H2 dissociative adsorption barrier and allows for the adsorption reaction at energies well below the dissociation threshold of the H-H bond. The first reacting H2 molecule must contain considerable vibrational energy to overcome the dissociative adsorption barrier. However, this initial adsorption further activates the surface resulting in reduced barriers for dissociative adsorption of subsequent H2 molecules. This enables functionalization by H2 molecules with lower vibrational energy, yielding an avalanche effect for the hydrogenation reaction. These results provide an example of a catalytically active graphene coated surface and additionally set the stage for a reinterpretation of previous experimental work involving elevated H2 background gas pressures in the presence of hot filaments.
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Submitted on : Wednesday, December 12, 2018 - 4:13:44 PM
Last modification on : Wednesday, December 11, 2019 - 1:12:01 PM
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Line Kyhl, Régis Bisson, Richard Balog, Michael Groves, Esben Leonhard Kolsbjerg, et al.. Exciting H2 Molecules for Graphene Functionalization. ACS Nano, American Chemical Society, 2018, 12 (1), pp.513 - 520. ⟨10.1021/acsnano.7b07079⟩. ⟨hal-01690707⟩

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