期刊
ACS NANO
卷 12, 期 1, 页码 513-520出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.7b07079
关键词
graphene; vibrational excitation; nanostructured functionalization; band gap engineering molecular hydrogen; catalysis
类别
资金
- Danish Council for Independent Research [0602-02566B, 0602-02265B]
- Innovation Fund Denmark (NIAGRA)
- European Research Council (CoG GRANN)
- Villum Foundation via Villum Centre of Excellence for Dirac Materials [11744]
- Division of Chemical Sciences, Geosciences and Biosciences of the U.S. Department of Energy at LBNL [DE-AC02-05CH11231]
- Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy at LBNL [DE-AC02-05CH11231]
Hydrogen functionalization of graphene by exposure to vibrationally excited H-2 molecules is investigated by combined scanning tunneling microscopy, high resolution electron energy loss spectroscopy, X-ray photoelectron spectroscopy measurements, and density functional theory calculations. The measurements reveal that vibrationally excited H-2 molecules dissociatively adsorb on graphene on Ir(111) resulting in nanopatterned hydrogen functionalization structures. Calculations demonstrate that the presence of the Ir surface below the graphene lowers the H-2 dissociative adsorption barrier and allows for the adsorption reaction at energies well below the dissociation threshold of the H-H bond. The first reacting H-2 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 H-2 molecules. This enables functionalization by H-2 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 re-interpretation of previous experimental work involving elevated H-2 background gas pressures in the presence of hot filaments.
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