Asymmetric supercapacitors have attracted tremendous attention in energy storage devices since they have an enhanced energy density in comparison with symmetric supercapacitor devices. Furthermore, the development of diverse and flexible electronic devices requires the asymmetric supercapacitor devices to be flexible and in various configurations. However, it is still a challenge to develop a universal strategy to obtain both capacitive and Faradic electrodes with various architectures. Herein, a spontaneously reducing/assembling strategy in an alkaline condition is developed to fabricate large‐area reduced graphene oxide (RGO) and RGO–metal oxide/hydroxide composite films or microsized structures. As a proof of concept, the large‐area pure RGO and RGO/Mn₃O₄ composite films with porous structure and superior mechanical property are achieved by such strategy. These RGO‐based films can directly serve as the anodes and cathodes of the flexible asymmetric film supercapacitors. Furthermore, the interdigital RGO and RGO/Mn₃O₄ patterns are also obtained via a selectively reducing/assembling process to achieve the asymmetric microsized supercapacitors. These asymmetric supercapacitors with different configurations possess good electrochemical performance and excellent flexibility. Therefore, such reducing and assembling strategy provides a route to achieve large‐area RGO‐based films and microsized structures for the applications in the various fields such as energy storage and photocatalysis.

中文翻译：

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用于柔性不对称三明治和超小型超级电容器的大面积氧化石墨烯复合薄膜

非对称超级电容器与对称超级电容器相比具有更高的能量密度，因此在能量存储设备中引起了极大的关注。此外，多样化和灵活的电子设备的发展要求非对称超级电容器设备要灵活并且具有各种配置。然而，开发一种通用策略以同时获得具有各种架构的电容式和法拉第电极仍然是一个挑战。在此，开发了一种在碱性条件下自发的还原/组装策略，以制造大面积还原的氧化石墨烯（RGO）和RGO-金属氧化物/氢氧化物复合膜或微结构。作为概念验证，使用大面积纯RGO和RGO / Mn ₃ O ₄通过这种策略可以获得具有多孔结构和优异的机械性能的复合膜。这些基于RGO的薄膜可以直接用作柔性不对称薄膜超级电容器的阳极和阴极。此外，还可以通过选择性还原/组装工艺获得叉指型RGO和RGO / Mn ₃ O ₄图案，以实现不对称的微型超级电容器。这些具有不同构型的不对称超级电容器具有良好的电化学性能和出色的柔韧性。因此，这种还原和组装策略为实现大面积基于RGO的薄膜和微细结构提供了一条途径，可用于各种领域，例如能量存储和光催化。