4 years ago

High Electroactive Material Loading on a Carbon Nanotube@3D Graphene Aerogel for High-Performance Flexible All-Solid-State Asymmetric Supercapacitors

High Electroactive Material Loading on a Carbon Nanotube@3D Graphene Aerogel for High-Performance Flexible All-Solid-State Asymmetric Supercapacitors
Yuegang Zhang, Wanfei Li, Yongcai Qiu, Jie Yang, Yan Xu, Xinyi Zhang, Zhenghui Pan, Meinan Liu
Freestanding carbon-based hybrids, specifically carbon nanotube@3D graphene (CNTs@3DG) hybrid, are of great interest in electrochemical energy storage. However, the large holes (about 400 µm) in the commonly used 3D graphene foams (3DGF) constitute as high as 90% of the electrode volume, resulting in a very low loading of electroactive materials that is electrically connected to the carbon, which makes it difficult for flexible supercapacitors to achieve high gravimetric and volumetric energy density. Here, a hierarchically porous carbon hybrid is fabricated by growing 1D CNTs on 3D graphene aerogel (CNTs@3DGA) using a facile one-step chemical vapor deposition process. In this architecture, the 3DGA with ample interconnected micrometer-sized pores (about 5 µm) dramatically enhances mass loading of electroactive materials comparing with 3DGF. An optimized all-solid-state asymmetric supercapacitor (AASC) based on MnO2@CNTs@3DGA and Ppy@CNTs@3DGA electrodes exhibits high volumetric energy density of 3.85 mW h cm−3 and superior long-term cycle stability with 84.6% retention after 20 000 cycles, which are among the best reported for AASCs with both electrodes made of pseudocapacitive electroactive materials. A simple, scalable, and environmentally friendly method is described for preparing a novel carbon nanotube (CNT)@3D graphene aerogel (3DGA) that acts as an ideal support for high loading of electroactive materials. Lightweight and flexible all-solid-state asymmetric supercapacitors are assembled from the MnO2@CNTs@3DGA and polypyrrole@CNTs@3DGA electrodes. The devices realize high areal capacitance and superior mechanical strength and hold great promise for future flexible electronics.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/adfm.201701122

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