Reduction and covalent modification of graphene-oxide by nitrogen in glow discharge plasma

Research output: Contribution to journalArticle

Abstract

In this work, we performed plasma treatment of thin layers of graphene oxide samples in various nitrogen containing gases (mainly NH3 and N2). Experiments were performed in the preparation chamber of the X-ray photoelectron spectrometer, allowing "in situ" characterization of the treated surface. Introduction of nitrogen into the top surface was intensified by applying negative voltage on the sample between 0 and 300 V accelerating the positive plasma ions towards the sample. Significant amount of nitrogen (≈10 atomic %) was built into the top atomic layers of the graphene oxide samples at application of the 2 types of plasma gases for 10-minute reaction time. When comparing the NH3 and N2 plasma treatments, more complete reduction and closely similar amount of nitrogen was found at applying NH3 plasma. When increasing the bias, the N-content increased, together with decrease of the O content. The high-resolution C1s, O1s, and N1s spectra are broad, representing different chemical states. The peak envelopes of the O1s and N1s lines could be decomposed essentially to 3, while the C1s spectrum to 5 different, well-separated peaks, being identical for all samples. The component peaks were assigned to specific chemical bonding states (N1s: 398.3 eV sp2 pyridine N, 399.7 eV sp2 pyrrole, diazine or triazine N, 401.0 eV N in graphite plane; O1s: 530.8 eV carbonyl, 532.2 eV ether, epoxy, alcohol, ester C(box drawings double horizontal)O, 533.6 eV ester C-O-C, carboxyl OH). The relative amounts of C-O and C-N bonding states changed significantly with advancement of the treatment performed at increasing biases.

Original languageEnglish
JournalSurface and Interface Analysis
DOIs
Publication statusAccepted/In press - Jan 1 2018

Fingerprint

Graphite
Glow discharges
glow discharges
Graphene
graphene
Nitric Oxide
Nitrogen
Plasmas
nitrogen
Oxides
oxides
Plasma Gases
esters
Esters
Triazines
Pyrroles
Photoelectrons
Ether
Spectrometers
pyrroles

Keywords

  • Glow discharge NH plasma
  • Graphene oxide reduction
  • N-modified graphene oxide
  • XPS quantification

ASJC Scopus subject areas

  • Chemistry(all)
  • Condensed Matter Physics
  • Surfaces and Interfaces
  • Surfaces, Coatings and Films
  • Materials Chemistry

Cite this

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title = "Reduction and covalent modification of graphene-oxide by nitrogen in glow discharge plasma",
abstract = "In this work, we performed plasma treatment of thin layers of graphene oxide samples in various nitrogen containing gases (mainly NH3 and N2). Experiments were performed in the preparation chamber of the X-ray photoelectron spectrometer, allowing {"}in situ{"} characterization of the treated surface. Introduction of nitrogen into the top surface was intensified by applying negative voltage on the sample between 0 and 300 V accelerating the positive plasma ions towards the sample. Significant amount of nitrogen (≈10 atomic {\%}) was built into the top atomic layers of the graphene oxide samples at application of the 2 types of plasma gases for 10-minute reaction time. When comparing the NH3 and N2 plasma treatments, more complete reduction and closely similar amount of nitrogen was found at applying NH3 plasma. When increasing the bias, the N-content increased, together with decrease of the O content. The high-resolution C1s, O1s, and N1s spectra are broad, representing different chemical states. The peak envelopes of the O1s and N1s lines could be decomposed essentially to 3, while the C1s spectrum to 5 different, well-separated peaks, being identical for all samples. The component peaks were assigned to specific chemical bonding states (N1s: 398.3 eV sp2 pyridine N, 399.7 eV sp2 pyrrole, diazine or triazine N, 401.0 eV N in graphite plane; O1s: 530.8 eV carbonyl, 532.2 eV ether, epoxy, alcohol, ester C(box drawings double horizontal)O, 533.6 eV ester C-O-C, carboxyl OH). The relative amounts of C-O and C-N bonding states changed significantly with advancement of the treatment performed at increasing biases.",
keywords = "Glow discharge NH plasma, Graphene oxide reduction, N-modified graphene oxide, XPS quantification",
author = "M. Mohai and K. L{\'a}szl{\'o} and I. Bert{\'o}ti",
year = "2018",
month = "1",
day = "1",
doi = "10.1002/sia.6411",
language = "English",
journal = "Surface and Interface Analysis",
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T1 - Reduction and covalent modification of graphene-oxide by nitrogen in glow discharge plasma

AU - Mohai, M.

AU - László, K.

AU - Bertóti, I.

PY - 2018/1/1

Y1 - 2018/1/1

N2 - In this work, we performed plasma treatment of thin layers of graphene oxide samples in various nitrogen containing gases (mainly NH3 and N2). Experiments were performed in the preparation chamber of the X-ray photoelectron spectrometer, allowing "in situ" characterization of the treated surface. Introduction of nitrogen into the top surface was intensified by applying negative voltage on the sample between 0 and 300 V accelerating the positive plasma ions towards the sample. Significant amount of nitrogen (≈10 atomic %) was built into the top atomic layers of the graphene oxide samples at application of the 2 types of plasma gases for 10-minute reaction time. When comparing the NH3 and N2 plasma treatments, more complete reduction and closely similar amount of nitrogen was found at applying NH3 plasma. When increasing the bias, the N-content increased, together with decrease of the O content. The high-resolution C1s, O1s, and N1s spectra are broad, representing different chemical states. The peak envelopes of the O1s and N1s lines could be decomposed essentially to 3, while the C1s spectrum to 5 different, well-separated peaks, being identical for all samples. The component peaks were assigned to specific chemical bonding states (N1s: 398.3 eV sp2 pyridine N, 399.7 eV sp2 pyrrole, diazine or triazine N, 401.0 eV N in graphite plane; O1s: 530.8 eV carbonyl, 532.2 eV ether, epoxy, alcohol, ester C(box drawings double horizontal)O, 533.6 eV ester C-O-C, carboxyl OH). The relative amounts of C-O and C-N bonding states changed significantly with advancement of the treatment performed at increasing biases.

AB - In this work, we performed plasma treatment of thin layers of graphene oxide samples in various nitrogen containing gases (mainly NH3 and N2). Experiments were performed in the preparation chamber of the X-ray photoelectron spectrometer, allowing "in situ" characterization of the treated surface. Introduction of nitrogen into the top surface was intensified by applying negative voltage on the sample between 0 and 300 V accelerating the positive plasma ions towards the sample. Significant amount of nitrogen (≈10 atomic %) was built into the top atomic layers of the graphene oxide samples at application of the 2 types of plasma gases for 10-minute reaction time. When comparing the NH3 and N2 plasma treatments, more complete reduction and closely similar amount of nitrogen was found at applying NH3 plasma. When increasing the bias, the N-content increased, together with decrease of the O content. The high-resolution C1s, O1s, and N1s spectra are broad, representing different chemical states. The peak envelopes of the O1s and N1s lines could be decomposed essentially to 3, while the C1s spectrum to 5 different, well-separated peaks, being identical for all samples. The component peaks were assigned to specific chemical bonding states (N1s: 398.3 eV sp2 pyridine N, 399.7 eV sp2 pyrrole, diazine or triazine N, 401.0 eV N in graphite plane; O1s: 530.8 eV carbonyl, 532.2 eV ether, epoxy, alcohol, ester C(box drawings double horizontal)O, 533.6 eV ester C-O-C, carboxyl OH). The relative amounts of C-O and C-N bonding states changed significantly with advancement of the treatment performed at increasing biases.

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KW - N-modified graphene oxide

KW - XPS quantification

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