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Answers
Step-by-step explanation:
Hua Zhou+*, Ahmet Uysal+, Daniela M. Anjos‡, Yu Cai§, Steven H. Overbury‡, Matthew
Neurock§, John K. McDonough¶, Yury Gogotsi¶, and Paul Fenter+*
+ Chemical Science and Engineering Division, Argonne National Laboratory, Argonne, IL
60439
‡ Chemical Science Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831
§ Departments of Chemical Engineering and Chemistry, University of Virginia,
Charlottesville, VA 22904
¶ Department of Materials Science and Engineering & A.J. Drexel Nanomaterials Institute,
Drexel University, Philadelphia, PA 19104
Keywords: Graphene; Functionalization; Quinone; X-ray reflectivity; Proton-Coupled-
Electron-Transfer
Abstract: The non-covalent functionalization of graphene by small molecule aromatic
adsorbates, phenanthrenequinone (PQ), was investigated systematically by combining
electrochemical characterization, high-resolution interfacial X-ray scattering and ab-initio
density functional theory calculations. Our findings 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 non-covalent functionalization by PQ adsorption.
The structure of adsorbed PQ molecules resemble the graphene layer stacking and are 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 (PCET) 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