nn9b03060_si_001.pdf (2.55 MB)
Selective Reduction Mechanism of Graphene Oxide Driven by the Photon Mode versus the Thermal Mode
journal contribution
posted on 2019-08-23, 11:05 authored by Masaki Hada, Kiyoshi Miyata, Satoshi Ohmura, Yusuke Arashida, Kohei Ichiyanagi, Ikufumi Katayama, Takayuki Suzuki, Wang Chen, Shota Mizote, Takayoshi Sawa, Takayoshi Yokoya, Toshio Seki, Jiro Matsuo, Tomoharu Tokunaga, Chihiro Itoh, Kenji Tsuruta, Ryo Fukaya, Shunsuke Nozawa, Shin-ichi Adachi, Jun Takeda, Ken Onda, Shin-ya Koshihara, Yasuhiko Hayashi, Yuta NishinaA two-dimensional
nanocarbon, graphene, has attracted substantial
interest due to its excellent properties. The reduction of graphene
oxide (GO) has been investigated for the mass production of graphene
used in practical applications. Different reduction processes produce
different properties in graphene, affecting the performance of the
final materials or devices. Therefore, an understanding of the mechanisms
of GO reduction is important for controlling the properties of functional
two-dimensional systems. Here, we determined the average structure
of reduced GO prepared via heating and photoexcitation
and clearly distinguished their reduction mechanisms using ultrafast
time-resolved electron diffraction, time-resolved infrared vibrational
spectroscopy, and time-dependent density functional theory calculations.
The oxygen atoms of epoxy groups are selectively removed from the
basal plane of GO by photoexcitation (photon mode), in stark contrast
to the behavior observed for the thermal reduction of hydroxyl and
epoxy groups (thermal mode). The difference originates from the selective
excitation of epoxy bonds via an electronic transition
due to their antibonding character. This work will enable the preparation
of the optimum GO for the intended applications and expands the application
scope of two-dimensional systems.
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vibrational spectroscopybasal planetheory calculationsapplication scopePhoton ModeThermal Modereduction mechanismstime-dependent densitygraphene oxideDifferent reduction processesoxygen atomsultrafast time-resolved electron diffractionphotoexcitationSelective Reduction Mechanismmass productionantibonding characterGraphene Oxidemode
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