Understanding Defect-Stabilized Noncovalent Functionalization of Graphene

Hua Zhou, Ahmet Uysal, Daniela M. Anjos, Yu Cai, Steven H. Overbury, Matthew Neurock, John K. McDonough, Yury Gogotsi, Paul Fenter

Research output: Contribution to journalArticlepeer-review

11 Scopus citations

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.

Original languageEnglish (US)
Article number1500277
JournalAdvanced Materials Interfaces
Volume2
Issue number17
DOIs
StatePublished - Nov 23 2015

Keywords

  • X-ray reflectivity
  • functionalization
  • graphene
  • proton-coupled electron transfer
  • quinone

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