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Electron transport shuttle mechanism via an Fe–N–C bond derived from a conjugated microporous polymer for a supercapacitor†
Dalton Transactions ( IF 3.5 ) Pub Date : 2017-12-04 00:00:00 , DOI: 10.1039/c7dt04094f
Alan Christian Lim 1, 2, 3, 4, 5 , Harsharaj S. Jadhav 1, 2, 3, 4, 5 , Jeong Gil Seo 1, 2, 3, 4, 5
Affiliation  

A new innovative electrode material (Fe-P800) consisting of a metal complex anchored on carbon via the utilization of iron-porphyrin conjugated microporous polymer (Fe-CMP) was prepared after pyrolyzing at 800 °C. The usage of the polymer with iron-porphyrin repeating units maximized the possible formation of Fe–Nx coordination within the bulk of the sample while the thermal treatment rendered the carbon framework to form a distinct arrangement between metal, nitrogen and carbon with a high surface area of 450 m2 g−1. The formation of the M–N–C bond, confirmed through XPS analysis, established a direct interaction between metal and carbon material. Thus, an indisputable synergistic effect was observed leading to a high capacitance of 182 F g−1 at a current density of 1 A g−1 despite its low metal loading of ∼1%. It also exhibited a highly robust cycling stability of ∼100% capacitance retention even after 5000 cycles (10 A g−1). In this study, a new mechanism was proposed wherein the metal (iron) center features an electron access point via its highly reversible redox reactivity, providing a shuttle effect for charge transfer to the conductive graphitic carbon matrix.

中文翻译:

电子传输梭机构通过从超级电容器的共轭微孔聚合物衍生的Fe-N-C键

在800°C的温度下热解后,制备了一种新的创新电极材料(Fe-P800),该材料由利用铁-卟啉共轭微孔聚合物(Fe-CMP)固定在碳的金属络合物组成。带有铁-卟啉重复单元的聚合物的使用可最大程度地在样品主体中形成Fe–N x配位,同时热处理使碳骨架在高表面的金属,氮和碳之间形成独特的排列面积450 m 2 g -1。XPS分析证实了M–N–C键的形成,建立了金属与碳材料之间的直接相互作用。因此,观察到了无可争议的协同效应,尽管金属负载量约为1%,但在1 A g -1的电流密度下却产生了182 F g -1的高电容。即使在5000次循环(10 A g -1)之后,它也表现出〜100%的电容保持率的高度鲁棒的循环稳定性。在这项研究中,提出了一种新的机制,其中金属(铁)中心通过其高度可逆的氧化还原反应性而具有电子接入点,从而为电荷转移到导电石墨碳基质提供了穿梭效应。
更新日期:2017-12-04
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