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A Space-Confined Polymerization Templated by Ice Enables Large-Scale Synthesis of Two-Dimensional Polymer Sheets
Authors:Xiaomeng Peng  Jie Zhang  Ji Zhou  Shang Chen  Yuncan Jia  Xinyi Han  Dr. Xiaodong Meng  Prof. Christopher W. Bielawski  Prof. Jianxin Geng
Affiliation:1. State Key Laboratory of Separation Membranes and Membrane Processes, Tianjin Key Laboratory of Advanced Fibers and Energy Storage, School of Material Science and Engineering, Tiangong University, No. 399 BinShuiXi Road, XiQing District, Tianjin, 300387 China

State Key Laboratory of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, No. 15 North Third Ring Road East, Chaoyang District, Beijing, 100029 China;2. State Key Laboratory of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, No. 15 North Third Ring Road East, Chaoyang District, Beijing, 100029 China;3. State Key Laboratory of Separation Membranes and Membrane Processes, Tianjin Key Laboratory of Advanced Fibers and Energy Storage, School of Material Science and Engineering, Tiangong University, No. 399 BinShuiXi Road, XiQing District, Tianjin, 300387 China;4. Center for Multidimensional Carbon Materials (CMCM), Institute for Basic Science (IBS), Ulsan, 44919 Republic of Korea

Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 44919 Republic of Korea

Abstract:Despite significant progress in the preparation and characterization of two-dimensional (2D) materials, the synthesis of 2D organic materials remains challenging. Here, we report a novel space-confined polymerization method that enables the large-scale synthesis of 2D sheets of a functional conjugated polymer, namely, poly(3,4-ethylenedioxythiophene) (PEDOT). A key step in this method is the confinement of monomer to the boundaries of ice crystals using micelles. This spatial confinement directs the polymerization to form 2D PEDOT sheets with high crystallinity and controlled morphology. Supercapacitors prepared from the 2D PEDOT sheets exhibit outstanding performance metrics. In aqueous electrolyte, a high areal specific capacitance of 898 mF cm−2 at 0.2 mA cm−2 along with an excellent rate capability is achieved (e.g., capacitance retention of 67.6 % at a 50-fold higher current). Moreover, the 2D PEDOT-based supercapacitors exhibit outstanding cycling stability (capacitance retention of 98.5 % after 30,000 cycles). Device performance is further improved when an organic electrolyte is used.
Keywords:Conjugated Polymers  Micelles  Space-Confined Polymerization  Supercapacitors  Two-Dimensional
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