Exciting H2 Molecules for Graphene Functionalization

Line Kyhl; Regis Bisson; Richard Balog; Michael N Groves; Esben Leonhard Kolsbjerg; Andrew Martin Cassidy; Jakob Holm Jørgensen; Susanne Halkjær; Jill A Miwa; Antonija Grubišić Čabo; Thierry Angot; Philip Hofmann; Mohammad Alif Arman; Samuli Urpelainen; Paolo Lacovig; Luca Bignardi; Hendrik Bluhm; Jan Knudsen; Bjørk Hammer; Liv Hornekaer

doi:10.1021/acsnano.7b07079

Exciting H2 Molecules for Graphene Functionalization

Line Kyhl, Regis Bisson, Richard Balog, Michael N Groves, Esben Leonhard Kolsbjerg, Andrew Martin Cassidy, Jakob Holm Jørgensen, Susanne Halkjær, Jill A Miwa, Antonija Grubišić Čabo, Thierry Angot, Philip Hofmann, Mohammad Alif Arman, Samuli Urpelainen, Paolo Lacovig, Luca Bignardi, Hendrik Bluhm, Jan Knudsen, Bjørk Hammer, Liv Hornekaer

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Abstract

Hydrogen functionalization of graphene by exposure to vibrationally excited H ₂ molecules is investigated by combined scanning tunneling microscopy, highresolution 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 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 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.

Original language	English
Journal	ACS Nano
Volume	12
Issue	1
Pages (from-to)	513-520
Number of pages	8
ISSN	1936-0851
DOIs	https://doi.org/10.1021/acsnano.7b07079
Publication status	Published - 2018

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10.1021/acsnano.7b07079

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Kyhl, L., Bisson, R., Balog, R., Groves, M. N., Kolsbjerg, E. L., Cassidy, A. M., Jørgensen, J. H., Halkjær, S., Miwa, J. A., Čabo, A. G., Angot, T., Hofmann, P., Arman, M. A., Urpelainen, S., Lacovig, P., Bignardi, L., Bluhm, H., Knudsen, J., Hammer, B., & Hornekaer, L. (2018). Exciting H2 Molecules for Graphene Functionalization. ACS Nano, 12(1), 513-520. https://doi.org/10.1021/acsnano.7b07079

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title = "Exciting H2 Molecules for Graphene Functionalization",

abstract = "Hydrogen functionalization of graphene by exposure to vibrationally excited H 2 molecules is investigated by combined scanning tunneling microscopy, highresolution 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 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 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.",

keywords = "Journal Article",

author = "Line Kyhl and Regis Bisson and Richard Balog and Groves, {Michael N} and Kolsbjerg, {Esben Leonhard} and Cassidy, {Andrew Martin} and J{\o}rgensen, {Jakob Holm} and Susanne Halkj{\ae}r and Miwa, {Jill A} and {\v C}abo, {Antonija Grubi{\v s}i{\'c}} and Thierry Angot and Philip Hofmann and Arman, {Mohammad Alif} and Samuli Urpelainen and Paolo Lacovig and Luca Bignardi and Hendrik Bluhm and Jan Knudsen and Bj{\o}rk Hammer and Liv Hornekaer",

year = "2018",

doi = "10.1021/acsnano.7b07079",

language = "English",

volume = "12",

pages = "513--520",

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Kyhl, L, Bisson, R, Balog, R, Groves, MN, Kolsbjerg, EL, Cassidy, AM, Jørgensen, JH, Halkjær, S, Miwa, JA, Čabo, AG, Angot, T, Hofmann, P, Arman, MA, Urpelainen, S, Lacovig, P, Bignardi, L, Bluhm, H, Knudsen, J, Hammer, B & Hornekaer, L 2018, 'Exciting H2 Molecules for Graphene Functionalization', ACS Nano, vol. 12, no. 1, pp. 513-520. https://doi.org/10.1021/acsnano.7b07079

TY - JOUR

T1 - Exciting H2 Molecules for Graphene Functionalization

AU - Kyhl, Line

AU - Bisson, Regis

AU - Balog, Richard

AU - Groves, Michael N

AU - Kolsbjerg, Esben Leonhard

AU - Cassidy, Andrew Martin

AU - Jørgensen, Jakob Holm

AU - Halkjær, Susanne

AU - Miwa, Jill A

AU - Čabo, Antonija Grubišić

AU - Angot, Thierry

AU - Hofmann, Philip

AU - Arman, Mohammad Alif

AU - Urpelainen, Samuli

AU - Lacovig, Paolo

AU - Bignardi, Luca

AU - Bluhm, Hendrik

AU - Knudsen, Jan

AU - Hammer, Bjørk

AU - Hornekaer, Liv

PY - 2018

Y1 - 2018

N2 - Hydrogen functionalization of graphene by exposure to vibrationally excited H 2 molecules is investigated by combined scanning tunneling microscopy, highresolution 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 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 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.

AB - Hydrogen functionalization of graphene by exposure to vibrationally excited H 2 molecules is investigated by combined scanning tunneling microscopy, highresolution 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 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 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.

KW - Journal Article

UR - http://www.scopus.com/inward/record.url?scp=85041131756&partnerID=8YFLogxK

U2 - 10.1021/acsnano.7b07079

DO - 10.1021/acsnano.7b07079

M3 - Journal article

C2 - 29253339

SN - 1936-0851

VL - 12

SP - 513

EP - 520

JO - ACS Nano

JF - ACS Nano

IS - 1

ER -

Exciting H2 Molecules for Graphene Functionalization

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