Journal article
Understanding Defect‐Stabilized Noncovalent Functionalization of Graphene
Advanced materials interfaces, Vol.2(17), pp.1500277-n/a
23 Nov 2015
Abstract
The noncovalent functionalization of graphene by small molecule aromatic adsorbates, phenanthrenequinone (PQ), is investigated systematically by combining electrochemical characterization, high‐resolution interfacial X‐ray scattering, and ab initio density functional theory calculations. The findings in this study reveal that while PQ deposited on pristine graphene is unstable to electrochemical cycling, the prior introduction of defects and oxygen functionality (hydroxyl and epoxide groups) to the basal plane by exposure to atomic radicals (i.e., oxygen plasma) effectively stabilizes its noncovalent functionalization by PQ adsorption. The structure of adsorbed PQ molecules resembles the graphene layer stacking and is further stabilized by hydrogen bonding with terminal hydroxyl groups that form at defect sites within the graphene basal plane. The stabilized PQ/graphene interface demonstrates persistent redox activity associated with proton‐coupled‐electron‐transfer reactions. The resultant PQ adsorbed structure is essentially independent of electrochemical potentials. These results highlight a facile approach to enhance functionalities of the otherwise chemically inert graphene using noncovalent interactions.
A defect‐mediated stabilization mechanism of the adsorption of small‐molecule aromatics for the noncovalent functionalization of graphene is understood by an investigation combining electrochemical characterization, high‐resolution interfacial X‐ray scattering, and ab initio density functional theory calculations. A stabilized quinone/graphene interface demonstrates persistent redox activity associated with the proton‐coupled‐electron‐transfer reaction.
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Details
- Title
- Understanding Defect‐Stabilized Noncovalent Functionalization of Graphene
- Creators
- Hua Zhou - Argonne National LaboratoryAhmet Uysal - Argonne National LaboratoryDaniela M Anjos - Oak Ridge National LaboratoryYu Cai - University of VirginiaSteven H Overbury - Oak Ridge National LaboratoryMatthew Neurock - University of VirginiaJohn K McDonough - Drexel UniversityYury Gogotsi - Drexel UniversityPaul Fenter - Argonne National Laboratory
- Publication Details
- Advanced materials interfaces, Vol.2(17), pp.1500277-n/a
- Publisher
- Wiley
- Number of pages
- 8
- Grant note
- DOE‐SC‐BES (DEAC02–06CH11357) U. Department of Energy, Office of Science, Office of Basic Energy Sciences Office of Science of the US Department of Energy (DE‐AC02‐05CH11231)
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Materials Science and Engineering
- Identifiers
- 991014969854204721
InCites Highlights
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- Collaboration types
- Domestic collaboration
- Web of Science research areas
- Chemistry, Multidisciplinary
- Materials Science, Multidisciplinary