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J Am Chem Soc. 2018 Jul 5;140(26):8198-8205. doi: 10.1021/jacs.8b03235. Epub 2018 Jun 26.

Electrochemically Scalable Production of Fluorine-Modified Graphene for Flexible and High-Energy Ionogel-Based Microsupercapacitors.

Zhou F1, Huang H1, Xiao C1,2, Zheng S1,2,3, Shi X1,2,4, Qin J1,3, Fu Q1,2, Bao X1,2, Feng X5, Müllen K6, Wu ZS1.

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Dalian National Laboratory for Clean Energy , Dalian Institute of Chemical Physics, Chinese Academy of Sciences , 457 Zhongshan Road , Dalian 116023 , China.
State Key Laboratory of Catalysis , Dalian Institute of Chemical Physics, Chinese Academy of Sciences , 457 Zhongshan Road , Dalian 116023 , China.
University of Chinese Academy of Sciences , 19 A Yuquan Road , Shijingshan District , Beijing 100049 , China.
Department of Chemical Physics , University of Science and Technology of China , 96 JinZhai Road , Hefei 230026 , P. R. China.
Center for Advancing Electronics Dresden (cfaed) & Department of Chemistry and Food Chemistry , Technische Universität Dresden , Mommsenstraβe 4 , 01062 Dresden , Germany.
Max-Planck-Institut für Polymerforschung , Ackermannweg 10 , 55128 Mainz , Germany.


Scalable production of high-quality heteroatom-modified graphene is critical for microscale supercapacitors but remains a great challenge. Herein, we demonstrate a scalable, single-step electrochemical exfoliation of graphite into highly solution-processable fluorine-modified graphene (FG), achieved in an aqueous fluorine-containing neutral electrolyte, for flexible and high-energy-density ionogel-based microsupercapacitors (FG-MSCs). The electrochemically exfoliated FG nanosheets are characterized by atomic thinness, large lateral size (up to 12 μm), a high yield of >70% with ≤3 layers, and a fluorine doping of 3 at%, allowing for large-scale production of FG-MSCs. Our ionogel-based FG-MSCs deliver high energy density of 56 mWh cm-3, by far outperforming the most reported MSCs. Furthermore, the all-solid-state microdevices offer exceptional cyclability with ∼93% after 5000 cycles, robust mechanical flexibility with 100% of capacitance retention bended at 180°, and outstanding serial and parallel integration without the requirement of metal-based interconnects for high-voltage and high-capacitance output. Therefore, these FG-MSCs represent remarkable potential for electronics.


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