Laser-irradiated carbonized polyaniline-N-doped graphene heterostructure improves the cyclability of on-chip microsupercapacitor

Abstract

Laser-irradiated graphene-based heterostructures have attracted significant attention for the fabrication of highly conducting and stable metal-free energy storage devices. Heteroatom doping on the graphene backbone has proven to have better charge storage properties. Among other heteroatoms, nitrogen-doped graphene (NG) has been extensively researched due to its several advanced properties while maintaining the original characteristics of graphene for energy storage applications. However, NG is generally prepared via chemical vapor deposition or high temperature pyrolysis method, which gives low yield and has a complex operation route. In this work, first a polyaniline-reduce graphene oxide (PANI-rGO) heterostructure was prepared via in situ electrochemical polymerization, followed by the deposition process. In the next step, laser-irradiation process was employed to carbonize polyaniline as well as doping of nitrogen on the graphene film, simultaneously. For the very first time, laser-irradiated carbonization of PANI on NG (cPANI-NG) heterostructure was utilized for microsupercapacitor (MSC). The as-prepared cPANI-NG-MSC shows extremely high cycling stability with a capacitance enhancement of 135% of its initial capacitance after 70 000 continuous charge–discharge cycles. It is very interesting to know the origin of the capacitance enhancement, which results from the change of pyrrolic N in NG-MSC to the pyridinic and graphitic N. An on-chip NG-MSC exhibits an excellent charge storage capacitance of 43.5 mF cm⁻² at a current density of 0.5 mA cm⁻² and shows impressive power delivery at a very high scan rate of 100 V s⁻¹. The excellent rate capability of the MSC shows capacitance retention up to 70.1% with the variation of current density. This unique approach to fabricate NG-MSC can have a broad range of applications as energy storage devices in the electronics market, as demonstrated by glowing a commercial red LED.