TY - JOUR
T1 - Effect of Oxidation Level on the Interfacial Water at the Graphene Oxide-Water Interface
T2 - From Spectroscopic Signatures to Hydrogen-Bonding Environment
AU - David, Rolf
AU - Tuladhar, Aashish
AU - Zhang, Le
AU - Arges, Christopher
AU - Kumar, Revati
N1 - Publisher Copyright:
Copyright © 2020 American Chemical Society.
PY - 2020/9/17
Y1 - 2020/9/17
N2 - The interfacial region of the graphene oxide (GO)-water system is nonhomogenous due to the presence of two distinct domains: an oxygen-rich surface and a graphene-like region. The experimental vibrational sum-frequency generation (vSFG) spectra are distinctly different for the fully oxidized GO-water interface as compared to the reduced GO-water case. Computational investigations using ab initio molecular dynamics were performed to determine the molecular origins of the different spectroscopic features. The simulations were first validated by comparing the simulated vSFG spectra to those from the experiment, and the contributions to the spectra from different hydrogen bonding environments and interfacial water orientations were determined as a function of the oxidation level of the GO sheet. The ab initio simulations also revealed the reactive nature of the GO-water interface.
AB - The interfacial region of the graphene oxide (GO)-water system is nonhomogenous due to the presence of two distinct domains: an oxygen-rich surface and a graphene-like region. The experimental vibrational sum-frequency generation (vSFG) spectra are distinctly different for the fully oxidized GO-water interface as compared to the reduced GO-water case. Computational investigations using ab initio molecular dynamics were performed to determine the molecular origins of the different spectroscopic features. The simulations were first validated by comparing the simulated vSFG spectra to those from the experiment, and the contributions to the spectra from different hydrogen bonding environments and interfacial water orientations were determined as a function of the oxidation level of the GO sheet. The ab initio simulations also revealed the reactive nature of the GO-water interface.
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U2 - 10.1021/acs.jpcb.0c05282
DO - 10.1021/acs.jpcb.0c05282
M3 - Article
C2 - 32804501
AN - SCOPUS:85091191558
SN - 1520-6106
VL - 124
SP - 8167
EP - 8178
JO - Journal of Physical Chemistry B
JF - Journal of Physical Chemistry B
IS - 37
ER -