Nitriding an Oxygen-Doped Nanocarbonaceous Sorbent Synthesized via Solution Plasma Process for Improving CO2 Adsorption Capacity

Abstract

The synthesis of carbon nanoparticles (Cn) and oxygen-doped nanocarbon (OCn) was successfully done through a one-step synthesis by the solution plasma process (SPP). The Cn and OCn were nitrogen-doped by nitridation under an ammonia atmosphere at 800 °C for 2 h to yield NCn and NOCn, respectively, for carbon dioxide (CO2) adsorption. The NOCn exhibited the highest specific surface area (~570 m2 g−1) and highest CO2 adsorption capacity (1.63 mmol g−1 at 25 °C) among the synthesized samples. The primary nitrogen species on the surface of NOCn were pyridinic-N and pyrrolic-N. The synergistic effect of microporosity and nitrogen functionality on the NOCn surface played an essential role in CO2 adsorption enhancement. From the thermodynamic viewpoint, the CO2 adsorption on NOCn was physisorption, exothermic, and spontaneous. The NOCn showed a more negative enthalpy of adsorption, indicating its stronger interaction for CO2 on the surface, and hence, the higher adsorption capacity. The CO2 adsorption on NOCn over the whole pressure range at 25–55 °C best fitted the Toth model, suggesting monolayer adsorption on the heterogeneous surface. In addition, NOCn expressed a higher selective CO2 adsorption than Cn and so was a good candidate for multicycle adsorption.