致密无孔石墨烯/聚苯胺复合电极材料的电荷存储和输运机制研究

The dense graphene/PANI composite is almost free of porosity and exhibits a record high volumetric capacitance and excellent rate and cycling performance, which shows great advantages in supercapacitors towards high volumetric performance. Given the seeming contradiction between nonporous structure and excellent electrochemical performance, the project focuses on the energy storage behavior of the graphene/PANI composite, aims to reveal the energy storage mechanism in the nonporous dense composite materials and then supplement the design principle of high volumetric composite electrode materials to improve the volumetric performance of the composite materials. The energy storage behavior of the dense composites in supercapacitors will be studied to clarify the proton bulk transport mechanism of PANI in the nonporous composite. Pseudocapacitive reaction and structure conversion of the composite in different conditions, especially in alkaline, will also be discussed to analyze the electron and ion transport processes, and reveal the synergistic energy storage mechanism of polyaniline and carbon framework in the composites. Based on the above design principles of high volumetric composite electrode materials, the performance of composite materials will be further optimized. This project is of great importance not only from the points of fundamental study but also is helpful to develop supercapacitors with high volumetric performance.

致密无孔石墨烯/聚苯胺复合电极材料表现出超高的体积比容量和良好的倍率及循环特性，在高体积容量超级电容器方面展现出巨大优势。针对复合材料致密无孔特征与优良的电荷存储和输运特性这一看似矛盾的现象，本项目聚焦石墨烯/聚苯胺复合材料的电化学储能行为，致力于阐明致密无孔复合材料的储能机制，完善高体积容量复合电极材料的构建原则，提升复合材料性能。研究高密复合材料的储能行为，阐明在致密无孔复合材料中聚苯胺的质子体相传输机制；研究复合体系在不同环境下的赝电容反应及其结构转化规律，尤其是在碱性环境中的特殊行为，给出解析电子和离子传输过程的设计方案，揭示聚苯胺复合体系的协同储能机制；提出高体积容量致密复合电极材料的设计原则，获得高性能致密复合材料。项目的实施为探索和完善导电聚合物储能机制、拓展电极材料开发方向提供新的思路，具有重要的理论研究价值，同时对高体积容量超级电容器的研发和实用化具有指导意义。

随着便携式电子器件的持续小型化以及电动车的快速发展，在尽可能小的空间中实现尽可能高的容量成为下一代高性能储能材料和器件研发的必然要求。因具有超高的体积比容量和良好的电化学性能，致密石墨烯/聚苯胺复合电极材料在致密储能领域展现出广阔的应用前景。本项目立足于石墨烯基材料的复合与致密化，聚焦于石墨烯/聚苯胺复合材料的电化学储能行为展开研究，进而完善高密复合电极材料的设计原则，开发高体积容量储能器件。本项目在石墨烯基复合电极材料的设计及其协同储能机制研究、电极材料的致密化及高体积容量致密复合电极材料的设计与可控制备、高体积容量储能器件的构建等方面取得了一系列重要进展。同时，将致密储能的思想从超级电容器的设计与构建拓展到锂硫电池、锂离子电容器等更多储能器件中，并且将碳基聚苯胺复合材料应用在柔性储能领域。本项目的实施不仅为从材料和器件层面实现致密储能提供了重要的数据支撑和理论依据，同时对推进高体积容量电化学储能器件的实用化进程具有重要意义。