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.
Angew Chem Int Ed Engl. 2023 Jun 12;62(24):e202301940. doi: 10.1002/anie.202301940. Epub 2023 May 8.
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 at 0.2 mA cm 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.
尽管在二维（2D）材料的制备和表征方面取得了重大进展，但 2D 有机材料的合成仍然具有挑战性。在这里，我们报告了一种新颖的空间限制聚合方法，该方法能够大规模合成功能共轭聚合物，即聚（3,4-亚乙基二氧噻吩）（PEDOT）的 2D 片材。该方法的关键步骤是使用胶束将单体限制在冰晶的边界内。这种空间限制促使聚合形成具有高结晶度和可控形态的 2D PEDOT 片材。由 2D PEDOT 片材制备的超级电容器表现出优异的性能指标。在水性电解质中，实现了 898 mF cm 的高比面积比电容，在 0.2 mA cm 时具有出色的倍率性能（例如，在电流增加 50 倍时，电容保持率为 67.6%）。此外，基于 2D PEDOT 的超级电容器具有出色的循环稳定性（在 30000 次循环后电容保持率为 98.5%）。当使用有机电解质时，器件性能进一步提高。
