CO2-Derived Nanocarbons with Controlled Morphology and High Specific Capacitance

ACS Omega. 2023 Jul 31;8(32):29500-29511. doi: 10.1021/acsomega.3c03207. eCollection 2023 Aug 15.

Abstract

The conversion of CO2 to nanocarbons addresses a dual goal of harmful CO2 elimination from the atmosphere along with the production of valuable nanocarbon materials. In the present study, a simple one-step metallothermic CO2 reduction to nanocarbons was performed at 675 °C with the usage of a Mg reductant. The latter was employed alone and in its mixture with ferrocene, which was found to control the morphology of the produced nanocarbons. Scanning electron microscopy (SEM) analysis reveals a gradual increase in the amount of nanoparticles with different shapes and a decrease in tubular nanostructures with the increase of ferrocene content in the mixture. A possible mechanism for such morphological alterations is discussed. Transmission electron microscopy (TEM) analysis elucidates that the nanotubes and nanoparticles gain mainly amorphous structures, while sheet- and cloud-like morphologies also present in the materials possess significantly improved crystallinity. As a result, the overall crystallinity was preserved constant for all of the samples, which was confirmed by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) techniques. Finally, electrochemical tests demonstrated that the prepared nanocarbons retained high specific capacitance values in the range of 200-310 F/g (at 0.1 V/s), which can be explained by the measured high specific surface area (650-810 m2/g), total pore volume (1.20-1.55 cm3/g), and the degree of crystallinity. The obtained results demonstrate the suitability of ferrocene for managing the nanocarbons' morphology and open perspectives for the preparation of efficient "green" nanocarbon materials for energy storage applications and beyond.