Ultrahigh‐Areal Capacitance Flexible Supercapacitors Based on Laser Assisted Construction of Hierarchical Aligned Carbon Nanotubes

Abstract Electrochemical energy storage is a key technology for a clean and sustainable energy supply. In this respect, supercapacitors (SC) have recently received considerable attention due to their excellent performance, including high‐power density and long‐cycle life. However, the poor binding strength between the active materials and substrate, the low active material loading, and small specific capacitance hinder the overall performance improvement of the device. In this study, an ultrahigh‐areal capacitance flexible SC based on the Al micro grid‐based hierarchical vertically aligned carbon nanotubes (VACNTs) is studied. Interestingly, the Al micro grid‐based VACNTs exhibit ultrahigh loading (13 mg cm −2 ), and the as‐fabricated VACNTs electrode display outstanding electrochemical performance, including an impressive areal capacitance of 1,300 mF cm −2 at the current density of 13 mA cm −2 and excellent stability with a retention ratio of 90% after 20,000 cycles at the current density of 130 mA cm −2 . Furthermore, the hierarchical VACNT electrodes show excellent mechanical flexibility when assembled into quasi‐solid‐state SC using Na 2 SO 4 ‐PVA gel as the electrolyte. The capacitance of this device is hardly changed bending different angles, even 180°. This study demonstrates the tremendous potential of Al micro grid‐based hierarchical VACNTs as electrodes for high‐performance flexible and wearable energy storage devices.