Chemical Modification of Graphene Oxide by Nitrogenation: An X-ray Absorption and Emission Spectroscopy Study

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

doi:10.1038/srep42235

Chemical Modification of Graphene Oxide by Nitrogenation: An X-ray Absorption and Emission Spectroscopy Study

Journal Article · Fri Feb 10 00:00:00 EST 2017 · Scientific Reports

DOI:https://doi.org/10.1038/srep42235· OSTI ID:1379732

Chuang, Cheng-Hao ^[1]; Ray, Sekhar C. ^[2]; Mazumder, Debarati ^[2]; Sharma, Surbhi ^[3]; Ganguly, Abhijit ^[3]; Papakonstantinou, Pagona ^[3]; Chiou, Jau-Wern ^[4]; Tsai, Huang-Ming ^[5]; Shiu, Hung-Wei ^[5]; Chen, Chia-Hao ^[5]; Lin, Hong-Ji ^[5]; Guo, Jinghua ^[6]; Pong, Way-Faung ^[1]

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

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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1379732

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Vol. 7; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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