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Graphical abstract Hierarchically ordered carbon tube-sheet superstructure (CTSS) is synthesized via combing template-directed self-assembly of polyimide and the following carbonization. Possessing highly ordered superstructures with rich nitrogen dopant and hierarchical porosity, CTSS manifests remarkable performance as both lithium ion battery anode and the carbon support for water splitting catalysts. Highlights • CTSS is obtained by the template-directed self-assembly of PI and carbonization. • CTSS contains vertically oriented carbon sheet arrays with hollow interiors. • CTSS based LIB anode manifests high capacity and good cycling stability. • Water splitting catalysts with CTSS supports have superb activity and stability. • A CTSS-derived self-powered water splitting device is fabricated in this work. Abstract In this work, we report a template-directed self-assembly strategy towards the gram-level synthesis of hierarchically ordered carbon tube-sheet superstructure (CTSS) by using MoO 3 nanorod as the template and polyimide (PI) as the carbon source. Even in large quantities, MoO 3 nanorods can guide the assembly of PI in solution into vertically oriented nanosheet arrays with periodic patterns, which can be converted to nitrogen-doped porous CTSS after the removal of template and thermal carbonization. Possessing hierarchically ordered architecture, rich porosity and high nitrogen content, CTSS is an appealing material for energy storage and conversion devices such as high-performance lithium ion battery anode and water splitting catalyst support. More importantly, the results in this work highlight an avenue for the controllable synthesis of hierarchically ordered carbon superstructures with diversified functions and applications. [ABSTRACT FROM AUTHOR]

In this work, a facial in-situ polymerization strategy is developed for the first time to fabricate the composites of polyimide and carbon black (PI/CBs) by the condensation of 1,2,4,5-benzenetetracarboxylic anhydride and p -phenylenediamine with the presence of carbon black. This composition method can effectively suppress the crystallization of PI and thus allows the sufficient contact of PI and carbon black. As the cathode material in LIBs, the PI/CB composite manifests an extraordinary capacity of 182 mAh g −1 at 0.1 A g −1 , close to the theoretical value of PI. Moreover, the capacity of the PI/CB composite can be retained as 116 m Ah g −1 even at an ultrahigh current density of 10 A g −1 , outperforming the recently reported polymer LIB cathodes. Under the same conditions, the mechanical mixture of highly crystallized PI sheets and carbon black shows a much poorer performance. The approach demonstrated herein is expected to be further applied as an effective processing method to build up high performance electrodes with organic species in secondary batteries. [ABSTRACT FROM AUTHOR]