Selective Reduction Mechanism of Graphene Oxide Driven by the Photon Mode versus the Thermal Mode
- Masaki Hada*Masaki Hada*E-mail: [email protected]Graduate School of Natural Science and Technology, , Okayama University, Okayama 700-8530, JapanTsukuba Research Center for Interdisciplinary Materials Science, Faculty of Pure and Applied Sciences, University of Tsukuba, Tsukuba 305-8573, JapanMore by Masaki Hada,
- Kiyoshi Miyata ,
- Satoshi OhmuraSatoshi OhmuraFaculty of Engineering, Hiroshima Institute of Technology, Hiroshima 731-5193, JapanMore by Satoshi Ohmura,
- Yusuke ArashidaYusuke ArashidaGraduate School of Engineering, Yokohama National University, Yokohama 240-8501, JapanMore by Yusuke Arashida,
- Kohei IchiyanagiKohei IchiyanagiHigh Energy Accelerator Research Organization, Tsukuba 305-0801, JapanMore by Kohei Ichiyanagi,
- Ikufumi KatayamaIkufumi KatayamaGraduate School of Engineering, Yokohama National University, Yokohama 240-8501, JapanMore by Ikufumi Katayama,
- Takayuki SuzukiTakayuki SuzukiGraduate School of Engineering, Yokohama National University, Yokohama 240-8501, JapanMore by Takayuki Suzuki,
- Wang ChenWang ChenResearch Core for Interdisciplinary Sciences, Okayama University, Okayama 700-8530, JapanMore by Wang Chen,
- Shota MizoteShota MizoteGraduate School of Natural Science and Technology, Okayama University, Okayama 700-8530, JapanMore by Shota Mizote,
- Takayoshi SawaTakayoshi SawaGraduate School of Natural Science and Technology, Okayama University, Okayama 700-8530, JapanMore by Takayoshi Sawa,
- Takayoshi YokoyaTakayoshi YokoyaGraduate School of Natural Science and Technology, Research Institute for Interdisciplinary Science, , Okayama University, Okayama 700-8530, JapanMore by Takayoshi Yokoya,
- Toshio SekiToshio SekiDepartment of Nuclear Engineering, Kyoto University, Uji 611-0011, JapanMore by Toshio Seki,
- Jiro MatsuoJiro MatsuoQuantum Science and Engineering Center, Kyoto University, Uji 611-0011, JapanMore by Jiro Matsuo,
- Tomoharu TokunagaTomoharu TokunagaGraduate School of Engineering, Nagoya University, Nagoya 464-0814, JapanMore by Tomoharu Tokunaga,
- Chihiro ItohChihiro ItohFaculty of System Engineering, Wakayama University, Wakayama 640-8510, JapanMore by Chihiro Itoh,
- Kenji TsurutaKenji TsurutaGraduate School of Natural Science and Technology, Okayama University, Okayama 700-8530, JapanMore by Kenji Tsuruta,
- Ryo Fukaya ,
- Shunsuke NozawaShunsuke NozawaHigh Energy Accelerator Research Organization, Tsukuba 305-0801, JapanMore by Shunsuke Nozawa,
- Shin-ichi AdachiShin-ichi AdachiHigh Energy Accelerator Research Organization, Tsukuba 305-0801, JapanMore by Shin-ichi Adachi,
- Jun TakedaJun TakedaGraduate School of Engineering, Yokohama National University, Yokohama 240-8501, JapanMore by Jun Takeda,
- Ken Onda*Ken Onda*E-mail: [email protected]Faculty of Science, Kyushu University, Fukuoka 819-0395, JapanMore by Ken Onda,
- Shin-ya KoshiharaShin-ya KoshiharaSchool of Science, Tokyo Institute of Technology, Tokyo 152-8551, JapanMore by Shin-ya Koshihara,
- Yasuhiko HayashiYasuhiko HayashiGraduate School of Natural Science and Technology, Okayama University, Okayama 700-8530, JapanMore by Yasuhiko Hayashi, and
- Yuta Nishina*Yuta Nishina*E-mail: [email protected]Graduate School of Natural Science and Technology, Research Core for Interdisciplinary Sciences, , Okayama University, Okayama 700-8530, JapanMore by Yuta Nishina
Abstract
A 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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