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.


Chemical and Biochemical Engineering


Marie Curie International Incoming Fellowship
Marie Curie International Reintegration Fellowship
United States. Department of Energy. Office of Basic Energy Sciences
European Union
Greek National Funds


This work was supported through a Marie Curie International Incoming Fellowship (AL) and a Marie Curie International Reintegration Fellowship (GP). The ideas for this work were drawn, in part, from AL's work supported by the U.S.Department of Energy, Basic Energy Sciences Awards DEFG02-09ER466556and DE-SC0002157. This research has been also cofinanced by the European Union (European SocialFund - ESF) and Greek national funds through the Operational Program "Education and Lifelong Learning" of the National Strategic Reference Framework (NSRF) -Research Funding Program: THALES.

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

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Article - Journal

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© 2013 American Chemical Society (ACS), All rights reserved.

Publication Date

01 Feb 2013