One-Pot Solvent-Free Strategy for the Facile and Fast\nSynthesis of Highly Enriched Nitrogen-Doped Carbons

Abstract

Hierarchical\nporous nitrogen-doped carbons (HNCs) were successfully\nprepared by a facile and highly efficient one-pot solvent-free method\nthrough the <i>in situ</i> copolymerization of resorcinol,\np-phthalaldehyde, melamine, and Pluronic F127. This method involves\nonly a simple thermal treatment process, thus making it a potential\nchoice for fast and large scaled production of HNCs. The obtained\nHNCs were comprehensively characterized by X-ray diffraction, Raman\nspectroscopy, N₂ sorption, scanning electron microscopy,\ntransmission electron microscopy, CHN analysis, X-ray photoelectron\nspectroscopy, elemental mapping, and CO₂ adsorption. The\nresults show that HNCs possess well-developed hierarchical porous\nstructures and highly dispersed nitrogen contents. Even though the\nincorporated nitrogen content is as high as 11.80 wt %, the HNCs still\nexhibit high porosity and surface area. Due to the incorporation of\na large number of nitrogen species in carbon frameworks, the HNC exhibits\nexcellent CO₂ adsorption performance with CO₂ capacity of 1.66 mmol/g at 348 K and 1.0 bar, and CO₂/N₂ selectivity of 241 under flue gas conditions. In addition,\non the basis of the experimental and simulation results, it is believed\nthat among different nitrogen species the pyridinic nitrogen is likely\nto be the most favorable for CO₂ adsorption.