Chemical Modification of Graphene Oxide by Nitrogenation: An X-ray Absorption and Emission Spectroscopy Study
Abstract
Nitrogen-doped graphene oxides (GO:N x) were synthesized by a partial reduction of graphene oxide (GO) using urea [CO(NH 2) 2 ]. Their electronic/bonding structures were investigated using X-ray absorption near-edge structure (XANES), valence-band photoemission spectroscopy (VB-PES), X-ray emission spectroscopy (XES) and resonant inelastic X-ray scattering (RIXS). During GO:N x synthesis, different nitrogen-bonding species, such as pyrrolic/graphitic-nitrogen, were formed by replacing of oxygen-containing functional groups. At lower N-content (2.7 at%), pyrrolic-N, owing to surface and subsurface diffusion of C, N and NH is deduced from various X-ray spectroscopies. In contrast, at higher N-content (5.0 at%) graphitic nitrogen was formed in which each N-atom trigonally bonds to three distinct sp 2 -hybridized carbons with substitution of the N-atoms for C atoms in the graphite layer. Upon nitrogen substitution, the total density of state close to Fermi level is increased to raise the valence-band maximum, as revealed by VB-PES spectra, indicating an electron donation from nitrogen, molecular bonding C/N/O coordination or/and lattice structure reorganization in GO:N x . The well-ordered chemical environments induced by nitrogen dopant are revealed by XANES and RIXS measurements.
- Authors:
-
- Tamkang Univ., Taipei (Taiwan). Dept. of Physics
- Univ. of South Afric, Johannesburg (South Africa). Dept. of Physics
- Ulster Univ., Newtownabbey (United Kingdom). Engineering Research Inst.
- National Univ. of Kaohsiung (Taiwan). Dept. of Applied Physics
- National Synchrotron Radiation Research Center, Hsinchu (Taiwan)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source; Univ. of California, Santa Cruz, CA (United States). Dept. of Chemistry and Biochemistry
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1379732
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 7; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electronic properties and devices
Citation Formats
Chuang, Cheng-Hao, Ray, Sekhar C., Mazumder, Debarati, Sharma, Surbhi, Ganguly, Abhijit, Papakonstantinou, Pagona, Chiou, Jau-Wern, Tsai, Huang-Ming, Shiu, Hung-Wei, Chen, Chia-Hao, Lin, Hong-Ji, Guo, Jinghua, and Pong, Way-Faung. Chemical Modification of Graphene Oxide by Nitrogenation: An X-ray Absorption and Emission Spectroscopy Study. United States: N. p., 2017.
Web. doi:10.1038/srep42235.
Chuang, Cheng-Hao, Ray, Sekhar C., Mazumder, Debarati, Sharma, Surbhi, Ganguly, Abhijit, Papakonstantinou, Pagona, Chiou, Jau-Wern, Tsai, Huang-Ming, Shiu, Hung-Wei, Chen, Chia-Hao, Lin, Hong-Ji, Guo, Jinghua, & Pong, Way-Faung. Chemical Modification of Graphene Oxide by Nitrogenation: An X-ray Absorption and Emission Spectroscopy Study. United States. https://doi.org/10.1038/srep42235
Chuang, Cheng-Hao, Ray, Sekhar C., Mazumder, Debarati, Sharma, Surbhi, Ganguly, Abhijit, Papakonstantinou, Pagona, Chiou, Jau-Wern, Tsai, Huang-Ming, Shiu, Hung-Wei, Chen, Chia-Hao, Lin, Hong-Ji, Guo, Jinghua, and Pong, Way-Faung. Fri .
"Chemical Modification of Graphene Oxide by Nitrogenation: An X-ray Absorption and Emission Spectroscopy Study". United States. https://doi.org/10.1038/srep42235. https://www.osti.gov/servlets/purl/1379732.
@article{osti_1379732,
title = {Chemical Modification of Graphene Oxide by Nitrogenation: An X-ray Absorption and Emission Spectroscopy Study},
author = {Chuang, Cheng-Hao and Ray, Sekhar C. and Mazumder, Debarati and Sharma, Surbhi and Ganguly, Abhijit and Papakonstantinou, Pagona and Chiou, Jau-Wern and Tsai, Huang-Ming and Shiu, Hung-Wei and Chen, Chia-Hao and Lin, Hong-Ji and Guo, Jinghua and Pong, Way-Faung},
abstractNote = {Nitrogen-doped graphene oxides (GO:N x) were synthesized by a partial reduction of graphene oxide (GO) using urea [CO(NH 2) 2 ]. Their electronic/bonding structures were investigated using X-ray absorption near-edge structure (XANES), valence-band photoemission spectroscopy (VB-PES), X-ray emission spectroscopy (XES) and resonant inelastic X-ray scattering (RIXS). During GO:N x synthesis, different nitrogen-bonding species, such as pyrrolic/graphitic-nitrogen, were formed by replacing of oxygen-containing functional groups. At lower N-content (2.7 at%), pyrrolic-N, owing to surface and subsurface diffusion of C, N and NH is deduced from various X-ray spectroscopies. In contrast, at higher N-content (5.0 at%) graphitic nitrogen was formed in which each N-atom trigonally bonds to three distinct sp 2 -hybridized carbons with substitution of the N-atoms for C atoms in the graphite layer. Upon nitrogen substitution, the total density of state close to Fermi level is increased to raise the valence-band maximum, as revealed by VB-PES spectra, indicating an electron donation from nitrogen, molecular bonding C/N/O coordination or/and lattice structure reorganization in GO:N x . The well-ordered chemical environments induced by nitrogen dopant are revealed by XANES and RIXS measurements.},
doi = {10.1038/srep42235},
journal = {Scientific Reports},
number = ,
volume = 7,
place = {United States},
year = {2017},
month = {2}
}
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