Atomic Hydrogen Diffusion on Doped and Chemically Modified Graphene
To explore hydrogen mobility on graphene, density functional calculations are used to determine the magnitude of binding energy versus the diffusion barrier for graphene, considering the effects of hole and electron doping, B and N substitutional dopants, and oxygen heteroatoms. Although C-H binding energy and the barrier for chemical diffusion are not correlated, the binding energy of H in the lowest energy site on top of a C atom correlates with the binding energy of H over a "bridge" C-C bond, which is the transition state for chemical diffusion. Using this framework, we demonstrate that both B substitutionally doped graphene and hydoxylated graphene have the potential to simultaneously meet thermodynamic and kinetic constraints for reversible room-temperature hydrogenation. The constraints demonstrate that reversible room-temperature hydrogenation is possible only when H diffuses in a chemically bound state.
A. D. Lueking et al., "Atomic Hydrogen Diffusion on Doped and Chemically Modified Graphene," Journal of Physical Chemistry C, vol. 117, no. 12, pp. 6312-6319, American Chemical Society (ACS), Feb 2013.
The definitive version is available at https://doi.org/10.1021/jp4007763
Chemical and Biochemical Engineering
Marie Curie International Incoming Fellowship Marie Curie International Reintegration FellowshipUnited States.Department of Energy. Office of Basic Energy SciencesEuropean UnionGreek National Funds
Keywords and Phrases
Atomic hydrogen; Chemical diffusion; Chemically-modified graphene; Electron-doping; Hydrogen mobility; Kinetic constraints; Room temperature; Transition state; Binding energy; Density functional theory; Diffusion in solids; Doping (additives); Hole mobility; Hydrogenation; Graphene
International Standard Serial Number (ISSN)
Article - Journal
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