Hierarchically designed three-dimensional macro/mesoporous carbon frameworks for advanced electrochemical capacitance storage.

Mesoporous carbon (m-C) has potential applications as porous electrodes for electrochemical energy storage, but its applications have been severely limited by the inherent fragility and low electrical conductivity. A rational strategy is presented to construct m-C into hierarchical porous structures with high flexibility by using a carbon nanotube (CNT) sponge as a three-dimensional template, and grafting Pt nanoparticles at the m-C surface. This method involves several controllable steps including solution deposition of a mesoporous silica (m-SiO2 ) layer onto CNTs, chemical vapor deposition of acetylene, and etching of m-SiO2 , resulting in a CNT@m-C core-shell or a CNT@m-C@Pt core-shell hybrid structure after Pt adsorption. The underlying CNT network provides a robust yet flexible support and a high electrical conductivity, whereas the m-C provides large surface area, and the Pt nanoparticles improves interfacial electron and ion diffusion. Consequently, specific capacitances of 203 and 311 F g(-1) have been achieved in these CNT@m-C and CNT@m-C@Pt sponges as supercapacitor electrodes, respectively, which can retain 96 % of original capacitance under large degree compression.

Core-double-shell, carbon nanotube@polypyrrole@MnO2 sponge as freestanding, compressible supercapacitor electrode.

Design and fabrication of structurally optimized electrode materials are important for many energy applications such as supercapacitors and batteries. Here, we report a three-component, hierarchical, bulk electrode with tailored microstructure and electrochemical properties. Our supercapacitor electrode consists of a three-dimensional carbon nanotube (CNT) network (also called sponge) as a flexible and conductive skeleton, an intermediate polymer layer (polypyrrole, PPy) with good interface, and a metal oxide layer outside providing more surface area. These three components form a well-defined core-double-shell configuration that is distinct from simple core-shell or hybrid structures, and the synergistic effect leads to enhanced supercapacitor performance including high specific capacitance (even under severe compression) and excellent cycling stability. The mechanism study reveals that the shell sequence is a key factor; in our system, the CNT-PPy-MnO2 structure shows higher capacitance than the CNT-MnO2-PPy sequence. Our porous core-double-shell sponges can serve as freestanding, compressible electrodes for various energy devices.