Hierarchically Designed Three‐Dimensional Macro/Mesoporous Carbon Frameworks for Advanced Electrochemical Capacitance Storage

Mesoporous carbon (m-C) has potential applica- tions as porous electrodes for electrochemical energy stor- age, 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 solu- tion 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 un- derlying 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 interfa- cial electron and ion diffusion. Consequently, specific capaci- tances 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 ca- pacitance under large degree compression.