Ab Initio Study of Graphene Functionalized with Carboxyl Groups and Tetracyanoethylene Oxide

ORAL

Abstract

The electronic and structural properties of carbon nanomaterials can be affected by chemical functionalization. We applied {\it ab initio} computational methods based on density functional theory to study the covalent functionalization of graphene with carboxyl (COOH) groups and tetracyanoethylene oxide (TCNEO). Our calculations were carried out using the SIESTA and Quantum Espresso electronic structure codes combined with the generalized gradient approximation and local density approximation for the exchange correlation functional. The calculated binding energies and vibrational spectra of functionalized graphene surface and H-terminated graphene edge were compared with the available experimental data. Our calculation showed that the reaction of cycloaddition of TCNEO to graphene was endothermic for the surface of pristine graphene and exothermic for the edge of H-terminated graphene sheet. The simulated Raman and IR spectra of graphene functionalized with TCNEO were consistent with the experimental results. The computed vibrational spectra of graphene functionalized with COOH groups showed that the presence of point defects near the functionalization site affects the Raman and IR spectroscopic signatures of functionalized graphene.

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Authors

  • Sanjiv Jha

    New Mexico State University

  • Igor Vasiliev

    New Mexico State Univ, New Mexico State University

  • John Colton

    Brigham Young University Dept. of Physics and Astronomy, Brigham Young University, None, The College of William and Mary/Jefferson Lab, Brigham Young University-Idaho, Blue Ridge Research and Consulting LLC, Air Force Research Laboratory - Wright Patterson Air Force Base, Brigham Young Univ - Provo, Blue Ridge Research and Consulting, University of Utah, SRI International, Utah State University, Utah Valley University, Los Alamos National Laboratory, Professor, Graduate, United States Air Force Academy, Arizona State Univ, SiO2 NanoTech, Entrepix Inc, AFRL, Advisor, Brigham Young University- Provo, University of New Mexico, Univ of Utah, University of Wisconsin -- Madison, New Mexico Tech Physics Dept., Retired, Department of Physics and Astronomy, University of Utah, Department of Physics \& Astronomy, University of Hawai'i, JILA and University of Colorado, Boulder, National Institute of Standards and Technology, Boulder, University of Colorado, Boulder, Lawrence Berkeley National Laboratory, National Institute of Standards and Technology, Space Dynamics Lab, New Mexico Tech, BYU Professor, Brigham Young University -- Provo, Northern Arizona University, University of Colorado Boulder, Colorado State University, University of Utah, Department of Physics, New Mexico State University

  • John Colton

    Brigham Young University Dept. of Physics and Astronomy, Brigham Young University, None, The College of William and Mary/Jefferson Lab, Brigham Young University-Idaho, Blue Ridge Research and Consulting LLC, Air Force Research Laboratory - Wright Patterson Air Force Base, Brigham Young Univ - Provo, Blue Ridge Research and Consulting, University of Utah, SRI International, Utah State University, Utah Valley University, Los Alamos National Laboratory, Professor, Graduate, United States Air Force Academy, Arizona State Univ, SiO2 NanoTech, Entrepix Inc, AFRL, Advisor, Brigham Young University- Provo, University of New Mexico, Univ of Utah, University of Wisconsin -- Madison, New Mexico Tech Physics Dept., Retired, Department of Physics and Astronomy, University of Utah, Department of Physics \& Astronomy, University of Hawai'i, JILA and University of Colorado, Boulder, National Institute of Standards and Technology, Boulder, University of Colorado, Boulder, Lawrence Berkeley National Laboratory, National Institute of Standards and Technology, Space Dynamics Lab, New Mexico Tech, BYU Professor, Brigham Young University -- Provo, Northern Arizona University, University of Colorado Boulder, Colorado State University, University of Utah, Department of Physics, New Mexico State University

  • John Colton

    Brigham Young University Dept. of Physics and Astronomy, Brigham Young University, None, The College of William and Mary/Jefferson Lab, Brigham Young University-Idaho, Blue Ridge Research and Consulting LLC, Air Force Research Laboratory - Wright Patterson Air Force Base, Brigham Young Univ - Provo, Blue Ridge Research and Consulting, University of Utah, SRI International, Utah State University, Utah Valley University, Los Alamos National Laboratory, Professor, Graduate, United States Air Force Academy, Arizona State Univ, SiO2 NanoTech, Entrepix Inc, AFRL, Advisor, Brigham Young University- Provo, University of New Mexico, Univ of Utah, University of Wisconsin -- Madison, New Mexico Tech Physics Dept., Retired, Department of Physics and Astronomy, University of Utah, Department of Physics \& Astronomy, University of Hawai'i, JILA and University of Colorado, Boulder, National Institute of Standards and Technology, Boulder, University of Colorado, Boulder, Lawrence Berkeley National Laboratory, National Institute of Standards and Technology, Space Dynamics Lab, New Mexico Tech, BYU Professor, Brigham Young University -- Provo, Northern Arizona University, University of Colorado Boulder, Colorado State University, University of Utah, Department of Physics, New Mexico State University