Chemical structures of hydrazine-treated graphene oxide and generation of aromatic nitrogen doping

Sungjin Park; Yichen Hu; Jin Ok Hwang; Eui Sup Lee; Leah B. Casabianca; Weiwei Cai; Jeffrey R. Potts; Hyung Wook Ha; Shanshan Chen; Junghoon Oh; Sang Ouk Kim; Yong Hyun Kim; Yoshitaka Ishii; Rodney S. Ruoff

doi:10.1038/ncomms1643

Chemical structures of hydrazine-treated graphene oxide and generation of aromatic nitrogen doping

Sungjin Park, Yichen Hu, Jin Ok Hwang, Eui Sup Lee, Leah B. Casabianca, Weiwei Cai, Jeffrey R. Potts, Hyung Wook Ha, Shanshan Chen, Junghoon Oh, Sang Ouk Kim, Yong Hyun Kim, Yoshitaka Ishii, Rodney S. Ruoff

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Abstract

Chemically modified graphene platelets, produced via graphene oxide, show great promise in a variety of applications due to their electrical, thermal, barrier and mechanical properties. Understanding the chemical structures of chemically modified graphene platelets will aid in the understanding of their physical properties and facilitate development of chemically modified graphene platelet chemistry. Here we use ¹³C and ¹⁵N solid-state nuclear magnetic resonance spectroscopy and X-ray photoelectron spectroscopy to study the chemical structure of ¹⁵ N-labelled hydrazine-treated ¹³C-labelled graphite oxide and unlabelled hydrazine-treated graphene oxide, respectively. These experiments suggest that hydrazine treatment of graphene oxide causes insertion of an aromatic N₂ moiety in a five-membered ring at the platelet edges and also restores graphitic networks on the basal planes. Furthermore, density-functional theory calculations support the formation of such N₂ structures at the edges and help to elucidate the influence of the aromatic N₂ moieties on the electronic structure of chemically modified graphene platelets.

Original language	English
Article number	638
Journal	Nature Communications
Volume	3
DOIs	https://doi.org/10.1038/ncomms1643
State	Published - 2012

Bibliographical note

Funding Information:
S.P. and J.O. were supported by Global Frontier Research Center for Advanced Soft Electronics. This study was supported in part by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Award DESC001951 (R.S.R and Y.I.). The SSNMR methodology development in this work was also supported by the NSF (CHE 449952, CHE 957793) and the Dreyfus Foundation Teacher-Scholar Award program for Y.I. L.B.C. held an American Fellowship from the American Association of University Women during the course of this work. J.O.H and S.O.K. were supported by the NRL (R0A-2008-000-20057-0) and WCU (R32-2008-000-10051-0) programs funded by the Korean government. E.-S.L and Y.-H.K were supported by the WCU (R31-2008-000-10071-0) and Basic Science Research (2010-0006922) programs through the NRF of Korea.

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@article{54c8cc3b29784d40a08dc7589b2b1364,

title = "Chemical structures of hydrazine-treated graphene oxide and generation of aromatic nitrogen doping",

abstract = "Chemically modified graphene platelets, produced via graphene oxide, show great promise in a variety of applications due to their electrical, thermal, barrier and mechanical properties. Understanding the chemical structures of chemically modified graphene platelets will aid in the understanding of their physical properties and facilitate development of chemically modified graphene platelet chemistry. Here we use 13C and 15N solid-state nuclear magnetic resonance spectroscopy and X-ray photoelectron spectroscopy to study the chemical structure of 15 N-labelled hydrazine-treated 13C-labelled graphite oxide and unlabelled hydrazine-treated graphene oxide, respectively. These experiments suggest that hydrazine treatment of graphene oxide causes insertion of an aromatic N2 moiety in a five-membered ring at the platelet edges and also restores graphitic networks on the basal planes. Furthermore, density-functional theory calculations support the formation of such N2 structures at the edges and help to elucidate the influence of the aromatic N2 moieties on the electronic structure of chemically modified graphene platelets.",

author = "Sungjin Park and Yichen Hu and Hwang, {Jin Ok} and Lee, {Eui Sup} and Casabianca, {Leah B.} and Weiwei Cai and Potts, {Jeffrey R.} and Ha, {Hyung Wook} and Shanshan Chen and Junghoon Oh and Kim, {Sang Ouk} and Kim, {Yong Hyun} and Yoshitaka Ishii and Ruoff, {Rodney S.}",

note = "Funding Information: S.P. and J.O. were supported by Global Frontier Research Center for Advanced Soft Electronics. This study was supported in part by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Award DESC001951 (R.S.R and Y.I.). The SSNMR methodology development in this work was also supported by the NSF (CHE 449952, CHE 957793) and the Dreyfus Foundation Teacher-Scholar Award program for Y.I. L.B.C. held an American Fellowship from the American Association of University Women during the course of this work. J.O.H and S.O.K. were supported by the NRL (R0A-2008-000-20057-0) and WCU (R32-2008-000-10051-0) programs funded by the Korean government. E.-S.L and Y.-H.K were supported by the WCU (R31-2008-000-10071-0) and Basic Science Research (2010-0006922) programs through the NRF of Korea.",

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doi = "10.1038/ncomms1643",

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T1 - Chemical structures of hydrazine-treated graphene oxide and generation of aromatic nitrogen doping

AU - Park, Sungjin

AU - Hu, Yichen

AU - Hwang, Jin Ok

AU - Lee, Eui Sup

AU - Casabianca, Leah B.

AU - Cai, Weiwei

AU - Potts, Jeffrey R.

AU - Ha, Hyung Wook

AU - Chen, Shanshan

AU - Oh, Junghoon

AU - Kim, Sang Ouk

AU - Kim, Yong Hyun

AU - Ishii, Yoshitaka

AU - Ruoff, Rodney S.

N1 - Funding Information: S.P. and J.O. were supported by Global Frontier Research Center for Advanced Soft Electronics. This study was supported in part by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Award DESC001951 (R.S.R and Y.I.). The SSNMR methodology development in this work was also supported by the NSF (CHE 449952, CHE 957793) and the Dreyfus Foundation Teacher-Scholar Award program for Y.I. L.B.C. held an American Fellowship from the American Association of University Women during the course of this work. J.O.H and S.O.K. were supported by the NRL (R0A-2008-000-20057-0) and WCU (R32-2008-000-10051-0) programs funded by the Korean government. E.-S.L and Y.-H.K were supported by the WCU (R31-2008-000-10071-0) and Basic Science Research (2010-0006922) programs through the NRF of Korea.

PY - 2012

Y1 - 2012

N2 - Chemically modified graphene platelets, produced via graphene oxide, show great promise in a variety of applications due to their electrical, thermal, barrier and mechanical properties. Understanding the chemical structures of chemically modified graphene platelets will aid in the understanding of their physical properties and facilitate development of chemically modified graphene platelet chemistry. Here we use 13C and 15N solid-state nuclear magnetic resonance spectroscopy and X-ray photoelectron spectroscopy to study the chemical structure of 15 N-labelled hydrazine-treated 13C-labelled graphite oxide and unlabelled hydrazine-treated graphene oxide, respectively. These experiments suggest that hydrazine treatment of graphene oxide causes insertion of an aromatic N2 moiety in a five-membered ring at the platelet edges and also restores graphitic networks on the basal planes. Furthermore, density-functional theory calculations support the formation of such N2 structures at the edges and help to elucidate the influence of the aromatic N2 moieties on the electronic structure of chemically modified graphene platelets.

AB - Chemically modified graphene platelets, produced via graphene oxide, show great promise in a variety of applications due to their electrical, thermal, barrier and mechanical properties. Understanding the chemical structures of chemically modified graphene platelets will aid in the understanding of their physical properties and facilitate development of chemically modified graphene platelet chemistry. Here we use 13C and 15N solid-state nuclear magnetic resonance spectroscopy and X-ray photoelectron spectroscopy to study the chemical structure of 15 N-labelled hydrazine-treated 13C-labelled graphite oxide and unlabelled hydrazine-treated graphene oxide, respectively. These experiments suggest that hydrazine treatment of graphene oxide causes insertion of an aromatic N2 moiety in a five-membered ring at the platelet edges and also restores graphitic networks on the basal planes. Furthermore, density-functional theory calculations support the formation of such N2 structures at the edges and help to elucidate the influence of the aromatic N2 moieties on the electronic structure of chemically modified graphene platelets.

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DO - 10.1038/ncomms1643

M3 - Article

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SN - 2041-1723

VL - 3

JO - Nature Communications

JF - Nature Communications

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ER -

Chemical structures of hydrazine-treated graphene oxide and generation of aromatic nitrogen doping

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