Facile preparation of nitrogen-doped microporous carbon from potassium citrate/urea for effective CH4 separation and uptake

Abstract

N-doped microporous carbons have attracted much attention for micromolecule gas separation and accumulation owning to their superior adsorption potential and surface polarizability. However, to prepare N-doped microporous carbon usually acquire excess corrosive KOH as activator, which limits its application in industry. Here, we propose a non-corrosion method for the manufacture of narrow N-doped microporous carbons using potassium citrate acts as activating agent, and urea acts as both a nitrogen doping agent and coactivator without any solvent. The BET surface area, micropore volume, pore size distribution and N content can be easily adjusted by changing the potassium citrate/urea ratio and activating temperature. The influence of porous structure and N content on CH4 uptake and separation was investigated, and ultra-micropore volume (<1nm) plays a dominate role in CH4 selectivity adsorption. ACK2N1 had the largest CH4 adsorption capacity of 3.00 mmol/g and CH4/N2 selectivity of 7.11 at 273.15 K and 100 KPa due to its largest ultra-micropore volume and N content. The adsorption breakthrough, regeneration experiments and adsorption thermodynamics showed that the prepared well-developed N-doped microporous carbons have very good potential for CH4 separation and enrichment from low coal bed methane. Furthermore, the pore formation mechanism of the well microporous carbon materials is proposed.