Quantum studies of Eley–Rideal reactions between H atoms on a graphite surface

Sha, Xuejun; Jackson, Bret; Lemoine, Didier

doi:10.1063/1.1463399

Cited by 142 publications

(198 citation statements)

References 43 publications

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“…As expected, and in agreement with many previous DFT GGA studies, the barrier between the gas phase and the chemisorbed state is about 200 meV. 16,19,[32][33][34][35] The chemisorption well is 800 meV with a H−C bond length of 1.13 Å and puckering of the top site carbon atom away from the surface by ∼ 0.4 Å. With PBE there is no physisorption state, which is again consistent with previous work and understandable given the lack of a long-range correlation term in GGA exchange-correlation functionals.…”

Section: Hydrogen At Graphenesupporting

confidence: 92%

“…This barrier -which includes vdW, ZPE effects, quantum tunneling and finite temperature effects -is approximately half the height of barriers typically predicted for H atom chemisorption at graphene using traditional DFT-GGA methods. 16,19,[32][33][34][35] Although the barrier is substantially reduced the physisorption well remains relatively unperturbed, being a similar depth and shifted towards the gas phase by just ∼ 0.1 Å.…”

Section: Hydrogen At Graphenementioning

confidence: 99%

See 1 more Smart Citation

Cooperative Interplay of van der Waals Forces and Quantum Nuclear Effects on Adsorption: H at Graphene and at Coronene

et al. 2014

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The energetic barriers that atoms and molecules often experience when binding to surfaces are incredibly important to a myriad of chemical and physical processes. However these barriers are difficult to describe accurately with current computer simulation approaches. Two prominent contemporary challenges faced by simulation are the role of van der Waals forces and nuclear quantum effects. Here we examine the widely studied model systems of hydrogen

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Section: Hydrogen At Graphenesupporting

confidence: 92%

Section: Hydrogen At Graphenementioning

confidence: 99%

Cooperative Interplay of van der Waals Forces and Quantum Nuclear Effects on Adsorption: H at Graphene and at Coronene

et al. 2014

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“…1,2 The predominance of molecular hydrogen in interstellar media has been explained by the interplay between chemisorption and physisorption modes of hydrogen atoms onto graphene. 3,4 Hydrogen-induced defects in graphene have been investigated with respect to metal-free magnetism and band-gap engineering. 5,6 Even greater interest comes from the field of hydrogen storage.…”

Section: Introductionmentioning

confidence: 99%

Stability of hydrogenation states of graphene and conditions for hydrogen spillover

Han

Jung

et al. 2012

Phys. Rev. B

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The hydrogen spillover mechanism has been discussed in the field of hydrogen storage and is believed to have particular advantage over the storage as metal or chemical hydrides. We investigate conditions for practicality realizing the hydrogen spillover mechanism onto carbon surfaces, using first-principles methods. Our results show that contrary to common belief, types of hydrogenation configurations of graphene (the aggregated all-paired configurations) can satisfy the thermodynamic requirement for room-temperature hydrogen storage. However, the peculiarity of the paired adsorption modes gives rise to a large kinetic barrier against hydrogen migration and desorption. It means that an extremely high pressure is required to induce the migration-derived hydrogenation. However, if mobile catalytic particles are present inside the graphitic interstitials, hydrogen migration channels can open and the spillover phenomena can be realized. We suggest a molecular model for such a mobile catalyst which can exchange hydrogen atoms with the wall of graphene.

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“…Several theoretical studies have been performed in the past on the Eley-Rideal [128][129][130][131][132][133][134] and LangmuirHinshelwood [135,136] reactions. On the experimental side, chemisorption of hydrogen atoms has been studied [137] in conditions of relevance for photo-dissociation regions and good agreement was found with theoretical predictions [138].…”

Section: Quantum Studies Of Dynamical Processes At Surfacesmentioning

confidence: 99%

“…4 we consider some aspects of hydrogen dynamics on graphite, an important issue for understanding formation of hydrogen molecules in the interstellar medium (ISM). In this case we used the previously derived density functional theory (DFT) potential energy surface of Jackson and coworkers [23,24] in a quantum study of collision induced processes involving hydrogen atoms. In Sect.…”

Section: Introductionmentioning

confidence: 99%

Chemistry at surfaces: from ab initio structures to quantum dynamics

et al. 2007

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Recent years have witnessed an ever growing interest in theoretically studying chemical processes at surfaces. Apart from the interest in catalysis, electrochemistry, hydrogen economy, green chemistry, atmospheric and interstellar chemistry, theoretical understanding of the molecule-surface chemical bonding and of the microscopic dynamics of adsorption and reaction of adsorbates are of fundamental importance for modeling known processes, understanding new experimental data, predicting new phenomena, controlling reaction pathways. In this work, we review the efforts we have made in the last few years in this exciting field. We first consider the energetics and the structural properties of some adsorbates on metal surfaces, as deduced by converged, first-principles, plane-wave calculations within the slab-supercell approach. These studies comprise water adsorption on Ru(0001), a subject of very intense debate in the past few years, and oxygen adsorption on aluminum, the prototypical example of metal passivation. Next, we address dynamical processes at surfaces with classical and quantum methods. Here the main interest is in hydrogen dynamics on metallic and semi-metallic surfaces, because of its importance for hydrogen storage and interstellar chem- istry. Hydrogen sticking is studied with classical and quasi-classical means, with particular emphasis on the relaxation of hot-atoms following dissociative chemisorption. Hot atoms dynamics on metal surfaces is investigated in the reverse, hydrogen recombination process and compared to Eley-Rideal dynamics. Finally, Eley-Rideal, collision-induced desorption, and adsorbate-induced trapping are studied quantum mechanically on a graphite surface, and unexpected quantum effects are observed.

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Quantum studies of Eley–Rideal reactions between H atoms on a graphite surface

Cited by 142 publications

References 43 publications

Cooperative Interplay of van der Waals Forces and Quantum Nuclear Effects on Adsorption: H at Graphene and at Coronene

Cooperative Interplay of van der Waals Forces and Quantum Nuclear Effects on Adsorption: H at Graphene and at Coronene

Stability of hydrogenation states of graphene and conditions for hydrogen spillover

Chemistry at surfaces: from ab initio structures to quantum dynamics

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