Chemical Makeup and Hydrophilic Behavior of Graphene Oxide Nanoribbons after Low-Temperature Fluorination

Rebeca Romero Aburto, Lawrence B. Alemany, Thomas K. Weldeghiorghis, Sehmus Ozden, Zhiwei Peng, Aurélien Lherbier, Andrés Rafael Botello Méndez, Chandra Sekhar Tiwary, Jaime Taha-Tijerina, Zheng Yan, Mika Tabata, Jean Christophe Charlier, James M. Tour, Pulickel M. Ajayan

Research output: Contribution to journalArticle

23 Citations (Scopus)

Abstract

© 2015 American Chemical Society. Here we investigated the fluorination of graphene oxide nanoribbons (GONRs) using H<inf>2</inf> and F<inf>2</inf> gases at low temperature, below 200°C, with the purpose of elucidating their structure and predicting a fluorination mechanism. The importance of this study is the understanding of how fluorine functional groups are incorporated in complex structures, such as GONRs, as a function of temperature. The insight provided herein can potentially help engineer application-oriented materials for several research and industrial sectors. Direct <sup>13</sup>C pulse magic angle spinning (MAS) nuclear magnetic resonance (NMR) confirmed the presence of epoxy, hydroxyl, ester and ketone carbonyl, tertiary alkyl fluorides, as well as graphitic sp<sup>2</sup>-hybridized carbon. Moreover, <sup>19</sup>F-<sup>13</sup>C cross-polarization MAS NMR with <sup>1</sup>H and <sup>19</sup>F decoupling confirmed the presence of secondary alkyl fluoride (CF<inf>2</inf>) groups in the fluorinated graphene oxide nanoribbon (FGONR) structures fluorinated above 50°C. First-principles density functional theory calculations gained insight into the atomic arrangement of the most dominant chemical groups. The fluorinated GONRs present atomic fluorine percentages in the range of 6-35. Interestingly, the FGONRs synthesized up to 100°C, with 6-19% of atomic fluorine, exhibit colloidal similar stability in aqueous environments when compared to GONRs. This colloidal stability is important because it is not common for materials with up to 19% fluorine to have a high degree of hydrophilicity.
Original languageEnglish
Pages (from-to)7009-7018
Number of pages10
JournalACS Nano
DOIs
Publication statusPublished - 28 Jul 2015
Externally publishedYes

Fingerprint

Nanoribbons
Fluorination
Carbon Nanotubes
fluorination
Graphite
Fluorine
Oxides
Graphene
graphene
fluorine
oxides
Magic angle spinning
Fluorides
metal spinning
fluorides
Temperature
Nuclear magnetic resonance
nuclear magnetic resonance
cross polarization
Hydrophilicity

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Engineering(all)
  • Physics and Astronomy(all)

Cite this

Romero Aburto, R., Alemany, L. B., Weldeghiorghis, T. K., Ozden, S., Peng, Z., Lherbier, A., ... Ajayan, P. M. (2015). Chemical Makeup and Hydrophilic Behavior of Graphene Oxide Nanoribbons after Low-Temperature Fluorination. ACS Nano, 7009-7018. https://doi.org/10.1021/acsnano.5b01330
Romero Aburto, Rebeca ; Alemany, Lawrence B. ; Weldeghiorghis, Thomas K. ; Ozden, Sehmus ; Peng, Zhiwei ; Lherbier, Aurélien ; Botello Méndez, Andrés Rafael ; Tiwary, Chandra Sekhar ; Taha-Tijerina, Jaime ; Yan, Zheng ; Tabata, Mika ; Charlier, Jean Christophe ; Tour, James M. ; Ajayan, Pulickel M. / Chemical Makeup and Hydrophilic Behavior of Graphene Oxide Nanoribbons after Low-Temperature Fluorination. In: ACS Nano. 2015 ; pp. 7009-7018.
@article{33dbcc2fc9bc4c0ca3b5d5f75f204416,
title = "Chemical Makeup and Hydrophilic Behavior of Graphene Oxide Nanoribbons after Low-Temperature Fluorination",
abstract = "{\circledC} 2015 American Chemical Society. Here we investigated the fluorination of graphene oxide nanoribbons (GONRs) using H2 and F2 gases at low temperature, below 200°C, with the purpose of elucidating their structure and predicting a fluorination mechanism. The importance of this study is the understanding of how fluorine functional groups are incorporated in complex structures, such as GONRs, as a function of temperature. The insight provided herein can potentially help engineer application-oriented materials for several research and industrial sectors. Direct 13C pulse magic angle spinning (MAS) nuclear magnetic resonance (NMR) confirmed the presence of epoxy, hydroxyl, ester and ketone carbonyl, tertiary alkyl fluorides, as well as graphitic sp2-hybridized carbon. Moreover, 19F-13C cross-polarization MAS NMR with 1H and 19F decoupling confirmed the presence of secondary alkyl fluoride (CF2) groups in the fluorinated graphene oxide nanoribbon (FGONR) structures fluorinated above 50°C. First-principles density functional theory calculations gained insight into the atomic arrangement of the most dominant chemical groups. The fluorinated GONRs present atomic fluorine percentages in the range of 6-35. Interestingly, the FGONRs synthesized up to 100°C, with 6-19{\%} of atomic fluorine, exhibit colloidal similar stability in aqueous environments when compared to GONRs. This colloidal stability is important because it is not common for materials with up to 19{\%} fluorine to have a high degree of hydrophilicity.",
author = "{Romero Aburto}, Rebeca and Alemany, {Lawrence B.} and Weldeghiorghis, {Thomas K.} and Sehmus Ozden and Zhiwei Peng and Aur{\'e}lien Lherbier and {Botello M{\'e}ndez}, {Andr{\'e}s Rafael} and Tiwary, {Chandra Sekhar} and Jaime Taha-Tijerina and Zheng Yan and Mika Tabata and Charlier, {Jean Christophe} and Tour, {James M.} and Ajayan, {Pulickel M.}",
year = "2015",
month = "7",
day = "28",
doi = "10.1021/acsnano.5b01330",
language = "English",
pages = "7009--7018",
journal = "ACS Nano",
issn = "1936-0851",
publisher = "American Chemical Society",

}

Romero Aburto, R, Alemany, LB, Weldeghiorghis, TK, Ozden, S, Peng, Z, Lherbier, A, Botello Méndez, AR, Tiwary, CS, Taha-Tijerina, J, Yan, Z, Tabata, M, Charlier, JC, Tour, JM & Ajayan, PM 2015, 'Chemical Makeup and Hydrophilic Behavior of Graphene Oxide Nanoribbons after Low-Temperature Fluorination', ACS Nano, pp. 7009-7018. https://doi.org/10.1021/acsnano.5b01330

Chemical Makeup and Hydrophilic Behavior of Graphene Oxide Nanoribbons after Low-Temperature Fluorination. / Romero Aburto, Rebeca; Alemany, Lawrence B.; Weldeghiorghis, Thomas K.; Ozden, Sehmus; Peng, Zhiwei; Lherbier, Aurélien; Botello Méndez, Andrés Rafael; Tiwary, Chandra Sekhar; Taha-Tijerina, Jaime; Yan, Zheng; Tabata, Mika; Charlier, Jean Christophe; Tour, James M.; Ajayan, Pulickel M.

In: ACS Nano, 28.07.2015, p. 7009-7018.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Chemical Makeup and Hydrophilic Behavior of Graphene Oxide Nanoribbons after Low-Temperature Fluorination

AU - Romero Aburto, Rebeca

AU - Alemany, Lawrence B.

AU - Weldeghiorghis, Thomas K.

AU - Ozden, Sehmus

AU - Peng, Zhiwei

AU - Lherbier, Aurélien

AU - Botello Méndez, Andrés Rafael

AU - Tiwary, Chandra Sekhar

AU - Taha-Tijerina, Jaime

AU - Yan, Zheng

AU - Tabata, Mika

AU - Charlier, Jean Christophe

AU - Tour, James M.

AU - Ajayan, Pulickel M.

PY - 2015/7/28

Y1 - 2015/7/28

N2 - © 2015 American Chemical Society. Here we investigated the fluorination of graphene oxide nanoribbons (GONRs) using H2 and F2 gases at low temperature, below 200°C, with the purpose of elucidating their structure and predicting a fluorination mechanism. The importance of this study is the understanding of how fluorine functional groups are incorporated in complex structures, such as GONRs, as a function of temperature. The insight provided herein can potentially help engineer application-oriented materials for several research and industrial sectors. Direct 13C pulse magic angle spinning (MAS) nuclear magnetic resonance (NMR) confirmed the presence of epoxy, hydroxyl, ester and ketone carbonyl, tertiary alkyl fluorides, as well as graphitic sp2-hybridized carbon. Moreover, 19F-13C cross-polarization MAS NMR with 1H and 19F decoupling confirmed the presence of secondary alkyl fluoride (CF2) groups in the fluorinated graphene oxide nanoribbon (FGONR) structures fluorinated above 50°C. First-principles density functional theory calculations gained insight into the atomic arrangement of the most dominant chemical groups. The fluorinated GONRs present atomic fluorine percentages in the range of 6-35. Interestingly, the FGONRs synthesized up to 100°C, with 6-19% of atomic fluorine, exhibit colloidal similar stability in aqueous environments when compared to GONRs. This colloidal stability is important because it is not common for materials with up to 19% fluorine to have a high degree of hydrophilicity.

AB - © 2015 American Chemical Society. Here we investigated the fluorination of graphene oxide nanoribbons (GONRs) using H2 and F2 gases at low temperature, below 200°C, with the purpose of elucidating their structure and predicting a fluorination mechanism. The importance of this study is the understanding of how fluorine functional groups are incorporated in complex structures, such as GONRs, as a function of temperature. The insight provided herein can potentially help engineer application-oriented materials for several research and industrial sectors. Direct 13C pulse magic angle spinning (MAS) nuclear magnetic resonance (NMR) confirmed the presence of epoxy, hydroxyl, ester and ketone carbonyl, tertiary alkyl fluorides, as well as graphitic sp2-hybridized carbon. Moreover, 19F-13C cross-polarization MAS NMR with 1H and 19F decoupling confirmed the presence of secondary alkyl fluoride (CF2) groups in the fluorinated graphene oxide nanoribbon (FGONR) structures fluorinated above 50°C. First-principles density functional theory calculations gained insight into the atomic arrangement of the most dominant chemical groups. The fluorinated GONRs present atomic fluorine percentages in the range of 6-35. Interestingly, the FGONRs synthesized up to 100°C, with 6-19% of atomic fluorine, exhibit colloidal similar stability in aqueous environments when compared to GONRs. This colloidal stability is important because it is not common for materials with up to 19% fluorine to have a high degree of hydrophilicity.

U2 - 10.1021/acsnano.5b01330

DO - 10.1021/acsnano.5b01330

M3 - Article

SP - 7009

EP - 7018

JO - ACS Nano

JF - ACS Nano

SN - 1936-0851

ER -

Romero Aburto R, Alemany LB, Weldeghiorghis TK, Ozden S, Peng Z, Lherbier A et al. Chemical Makeup and Hydrophilic Behavior of Graphene Oxide Nanoribbons after Low-Temperature Fluorination. ACS Nano. 2015 Jul 28;7009-7018. https://doi.org/10.1021/acsnano.5b01330