In this work, nitrogen-doped porous carbons obtained from chitosan, gelatine, and green algae were investigated in their role as supercapacitor electrodes. The effects of three factors on electrochemical performance have been studied—of the specific surface area, functional groups, and a porous structure. Varying nitrogen contents (from 5.46 to 10.08 wt.%) and specific surface areas (from 532 to 1095 m² g⁻¹) were obtained by modifying the carbon precursor and the carbonization temperature. Doping nitrogen into carbon at a level of 5.74–7.09 wt.% appears to be the optimum for obtaining high electrochemical capacitance. The obtained carbons exhibited high capacitance (231 F g⁻¹ at 0.1 A g⁻¹) and cycle durability in a 0.2 mol L⁻¹ K₂SO₄ electrolyte. Capacitance retention was equal to 91% at 5 A g⁻¹ after 10,000 chronopotentiometry cycles. An analysis of electrochemical behaviour reveals the influence that nitrogen functional groups have on pseudocapacitance. While quaternary-N and pyrrolic-N nitrogen groups have an enhancing effect, due to the presence of a positive charge and thus improved electron transfer at high current loads, the most important functional group affecting energy storage performance is graphite-N/quaternary-N. The study points out that the search for the most favourable organic precursors is as important as the process of converting precursors to carbon-based electrode materials.

The manuscript presents results on the influence of external pressure on graphene exfoliation and subsequent 3D structuring by means of liquid-phase exfoliation. In contrast to known and applied exfoliation methods, the current study exploits the enhancement of splitting forces caused by the application of high pressure. The manufacturing pathway allowed to increase the surface area from 750 m²/g (nanoplatelets) to ca. 1100 m²/g (after 3D structuring). Electrochemical studies revealed that the 3D graphene materials were active in the oxygen reduction reaction (ORR). The outstanding ORR activity of 3D structured graphene materials should not be ascribed to heteroatom catalytic centers since such heteroatoms were successively removed upon increasing the carbonization temperature. XPS data showed that the presence of transition metals and nitrogen (usually regarded as catalytic centers) in G-materials was marginal. The results highlight the importance of structural factors of electrodes in the case of graphene-based materials for Zn–air batteries and ORR.

This paper addresses the problem of improving electrochemical energy storage with electrode materials obtained from common raw ingredients in a facile synthesis. In this study, we present a simple, one-pot route of synthesizing microporous carbon via a very fast reaction of sucrose and graphene (carbon source), chitosan (carbon and nitrogen source), and H₃PO₄. Porous carbons were successfully produced during high temperature carbonization, using nitrogen as a shielding gas. Samples were characterized using X-ray powder diffractometry, elemental analysis, N₂ adsorption-desorption measurements, scanning electron microscopy, and Raman spectroscopy. The developed carbon material possessed a high surface area, up to 1313 m² g⁻¹, with no chemical or physical activators used in the process. The structural parameters of the microporous carbons varied depending on the ratio of reagents and mass composition. Samples were prepared both with and without chitosan. The present synthesis route has the advantages of being a single-step approach and only involving low-cost and environmentally friendly sources of carbon. More importantly, microporous carbon was prepared without any activators and potentially offers great application in supercapacitors. Cyclic voltammetry and constant current charge–discharge tests show that sucrose-based porous carbons show excellent electrochemical performance with a specific capacitance of up to 143 F g⁻¹ at a current density of 1 A g⁻¹ in a 6 M KOH electrolyte.

In this paper, we show the carbonization of binary composites consisting of graphene nanoplatelets and melamine (GNP/MM), multi-walled carbon nanotubes and melamine (CNT/MM) and trinary composites containing GNP, CNT, and MM. Additionally, the manuscript presents results on the influence of structural factors for the electrochemical performance of carbon composites on their catalytic activity. This study contributes to the wide search and design of novel hybrid carbon composites for electrochemical applications. We demonstrate that intensive nitrogen atom insertion is not the governing factor since hybrid system modifications and porous structure sometimes play a more crucial role in the tailoring of electrochemical properties of the carbon hybrids seen as a noble metal-free alternative to traditional electrode materials. Additionally, HRTEM and Raman spectra study allowed for the evaluation of the quality of the obtained hybrid materials.

The design and fabrication of a new effective manufacturing method of heteroatom-doped carbon materials is still ongoing. In this paper, we present alternative and facile methods to obtain N-rich graphene with the use of low energy gamma radiation. This method was used as a pure and facile method for altering the physical and chemical properties of graphene. The obtained materials have an exceptionally high N content—up to 4 wt %. (dry method) and up to 2 wt %. (wet method). High-resolution transmission electron microscopy (HRTEM), scanning electron microscopy (SEM), X-ray diffraction (XRD), Raman spectra and X-ray photoelectron spectroscopy (XPS) studies allowed us to evaluate the quality of the obtained materials. The presented results will provide new insights in designing and optimizing N-doped carbon materials potentially for the development of anode or cathode materials for electrochemical device applications, especially supercapacitors, metal–air batteries and fuel cells. Nitrogen atoms are exclusively bonded as quaternary groups. The method is expandable to the chemical insertion of other heteroatoms to graphene, especially such as sulfur, boron or phosphorus.

The development of effective catalysts for the oxygen reduction reaction (ORR) is a significant challenge in energy conversion systems, e.g., Zn–air batteries. Herein, green-algae- and gelatine-derived porous, nitrogen-rich carbons were extensively investigated as electrode materials for electrochemical catalytic reactions. These carbon-based catalysts were designed and optimized to create a metal-free catalyst via templating, carbonization, and subsequent removal of the template. The additional incorporation of graphene improved electronic conductivity and enhanced the electrochemical catalytic reaction. Porous carbons with heteroatoms were used as effective platinum-free ORR electrocatalysts for energy conversion; the presence of nitrogen in the carbon provided more active sites for ORR. Our catalyst also displayed notable durability in a rechargeable Zn–air battery energy system. More importantly, the nitrogen-containing porous carbons were found to have comparable ORR performance in alkaline media to commercially available electrocatalysts. The manuscript demonstrates that nitrogen atom insertion is an appropriate approach when aiming to eliminate noble metals from the synthesis route. N-doped carbons are competitive materials compared to reference platinum-based catalysts.