Functional and structural tailoring of three-dimensional (3D) conducting polymer nanoarchitectures is a promising route but remains challenging to develop high-performance electrodes for electrochemical energy storage. Herein, we design poly(3, 4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) 3D mesoporous aerogel electrodes through a simple and original one-pot mechanochemical processing route. The hierarchical structure of neat PEDOT:PSS aerogels displays a highly interpenetrated porous conductive network with a record high active surface area of 470 m² g^-1 amongst the class of conducting polymer architectures. Robust structural and electrochemical performances are achieved with high gravimetric, areal and volumetric capacitance metrics of 120 F g^-1, 2.5 F cm^-2, and 124 F cm^-3, respectively, as the result of a mixed hybrid faradaic - capacitive charge storage mechanism. Moreover, these performances are attained in organic based electrolytes, reported so far to be incompatible or hinder the electrochemical activity of PEDOT:PSS. We undermine the fundamentals of the electrochemical operation in these electrodes and show that the electrolyte chemistry and the aerogel morphology particularly impact the charge storage performances demonstrating the superiority of the mesoporous architecture for charge transfer and ion exchange. Asymmetric cells are built having a specific capacitance of 40 F g^-1 based on the total mass of electrodes and a good cyclic stability with 90% capacitance retention after 1,000 charge and discharge cycles. This study offers a new route to enhance the electrochemical properties of conducting polymers and provides suggestive insights for developing high-performance polymer electrode materials for electrochemical energy storage.

中文翻译：

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用于高性能混合电化学储能的3D介孔导电聚合物气凝胶的机械化学组装

三维（3D）导电聚合物纳米结构的功能和结构定制是一种有前途的途径，但在开发用于电化学能量存储的高性能电极方面仍然具有挑战性。在这里，我们通过简单且原始的一锅式机械化学加工路线设计了聚（3，4-乙撑二氧噻吩）：聚苯乙烯磺酸盐（PEDOT：PSS）3D介孔气凝胶电极。整齐的PEDOT：PSS气凝胶的分层结构显示出高度互穿的多孔导电网络，在导电聚合物体系结构类别中，其记录的活性表面积高达470 m ²  g ^-1。借助120 F g ^-1的高重量，面积和体积电容指标，可实现稳定的结构和电化学性能，混合法拉第电容电容存储机制的结果分别是2.5 F cm ^-2和124 F cm ^-3。而且，这些性能是在有机基电解质中获得的，到目前为止，据报道它们是不相容的或阻碍了PEDOT：PSS的电化学活性。我们破坏了这些电极中电化学操作的基础，并表明电解质的化学性质和气凝胶的形态特别影响电荷存储性能，这证明了介孔结构在电荷转移和离子交换方面的优越性。构建具有40 F g ^-1的比电容的不对称电池基于电极的总质量和良好的循环稳定性，经过1000次充放电循环后具有90％的电容保持率。这项研究为增强导电聚合物的电化学性能提供了一条新途径，并为开发用于电化学储能的高性能聚合物电极材料提供了有益的见解。