Nitrogen-rich conjugated microporous polymers (CMPs) with tunable porosities and reversible redox properties have received increasing interest as electrode materials for supercapacitors. Herein, pyridyl building blocks with different substitutions are selected to synthesize four amine-linked conjugated microporous polytriphenylamine (PTPA) networks via Buchwald-Hartwig cross-coupling reaction engineering the redox activity of PTPAs. The structures, porosities, and redox activities of these four PTPAs are investigated. The electrochemical characterization results show that PTPA obtained using 2,5-diaminopyridine dihydrochloride (i.e., PTPA-25) displays the highest specific capacitances up to 335 F g-1 in 1.0 m H2 SO4 at a current density of 0.5 A g-1 . Upon 5000 cycles, PTPA-25 maintains good initial capacitances up to 65%, nearly 100% Coulombic efficiencies at a current density of 2 A g-1 , and high rate properties (remained a high capacitance of 250 F g-1 at 10 A g-1 ). The influence of different substitutions of pyridyl on the redox activities of the synthesized PTPA electrodes is further proposed, which would give insight into engineering the performance of CMPs-based supercapacitors.

中文翻译：

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使用吡啶基结构单元对高效超级电容器进行共轭微孔聚三苯胺网络中的工程氧化还原活性。

具有可调孔隙率和可逆氧化还原特性的富氮共轭微孔聚合物（CMP）作为超级电容器的电极材料受到越来越多的关注。在本文中，选择具有不同取代基的吡啶基结构单元，以通过Buchwald-Hartwig交叉偶联反应工程化PTPA的氧化还原活性来合成四个胺连接的共轭微孔聚三苯胺（PTPA）网络。研究了这四种PTPA的结构，孔隙率和氧化还原活性。电化学表征结果表明，使用2,5-二氨基吡啶二盐酸盐（即PTPA-25）制得的PTPA在1.0 m H2 SO4中以0.5 A g-1的电流密度显示最高的比电容，高达335 F g-1。经过5000次循环后，PTPA-25保持了高达65％的良好初始电容，在2 A g-1的电流密度下具有接近100％的库仑效率，并且具有高倍率特性（在10 A g-1时仍保持250 F g-1的高电容）。进一步提出了吡啶基的不同取代对合成的PTPA电极的氧化还原活性的影响，这将有助于工程设计基于CMP的超级电容器的性能。