Synergistically Active NiCo2 S4 Nanoparticles Coupled with Holey Defect Graphene Hydrogel for High-Performance Solid-State Supercapacitors

In order to make full utilization of the high intrinsic surface area of graphene, recently, porous graphene materials including graphene nanomesh, crumpled graphene and graphene foam, have attracted tremendous attention and research interest, owing to their exceptional porous structure (high surface area, and high pore volume) in combination with the inherent properties of graphene, such as high electronic conductivity, good thermal stability, and excellent mechanical strength. Interestingly, porous graphene materials and their derivatives have been explored in a wide range of applications in the fields of electronic and photonic devices, energy storage, gas separation/storage, oil absorption and sensors. This article reviews recent progress in the synthesis, characterization, properties, and applications of porous graphene materials. We aim to highlight the importance of designing different porous structures of graphene to meet future challenges, and the trend on future design of porous graphene materials is analyzed.

Nanoporous carbons (NPCs) have large specific surface areas, good electrical and thermal conductivity, and both chemical and mechanical stability, which facilitate their use in energy storage device applications. In the present study, highly graphitized NPCs are synthesized by one-step direct carbonization of cobalt-containing zeolitic imidazolate framework-67 (ZIF-67). After chemical etching, the deposited Co content can be completely removed to prepare pure NPCs with high specific surface area, large pore volume, and intrinsic electrical conductivity (high content of sp(2) -bonded carbons). A detailed electrochemical study is performed using cyclic voltammetry and galvanostatic charge-discharge measurements. Our NPC is very promising for efficient electrodes for high-performance supercapacitor applications. A maximum specific capacitance of 238 F g(-1) is observed at a scan rate of 20 mV s(-1) . This value is very high compared to previous works on carbon-based electric double layer capacitors.

Graphene is considered a promising ultracapacitor material toward high power and energy density because of its high conductivity and high surface area without pore tortuosity. However, the two-dimensional (2D) sheets tend to aggregate during the electrode fabrication process and align perpendicular to the flow direction of electrons and ions, which can reduce the available surface area and limit the electron and ion transport. This makes it hard to achieve scalable device performance as the loading level of the active material increases. Here, we report a strategy to solve these problems by transforming the 2D graphene sheet into a crumpled paper ball structure. Compared to flat or wrinkled sheets, the crumpled graphene balls can deliver much higher specific capacitance and better rate performance. More importantly, devices made with crumpled graphene balls are significantly less dependent on the electrode mass loading. Performance of graphene-based ultracapacitors can be further enhanced by using flat graphene sheets as the binder for the crumpled graphene balls, thus eliminating the need for less active binder materials.