Abstract

Lasers offer a versatile means towards the single-step, binder-free synthesis of three-dimensional graphene-like porous networks, providing an enticing alternative over energy intensive, multi-step traditional synthesis protocols creating unwanted waste streams. Here, we report on a novel laser-assisted method for the one-step preparation of the electrode component, not solely the active material, based on the simultaneous synthesis of turbostratic graphene-like structures on a carbon precursor and its transfer/deposition on the selected current collector. The performance of the graphene-based electrodes was electrochemically evaluated for both electric double layer capacitor (EDLC) and zinc-ion hybrid capacitor (ZIC) configurations. The performance of the EDLC devices was found to be superior to that of the current state-of-the-art devices prepared by laser-grown graphene. The ZIC exhibited higher areal energy density than the symmetric devices by one order of magnitude. The devices showed very low equivalent series resistance, good rate performance and high long-term cycling stability. Notably, the EDLC with the KOH electrolyte demonstrated an unexpected ∼20% increase in capacitance during the stability test of 10,000 cycles. This result was attributed to the substantial increase of oxygen content of the graphene electrodes, which act as sites for redox activity.

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