N-doped carbon nanospheres synthesized from a newly designed eco-friendly sustainable polymer for highly selective...

N-doped carbon nanospheres and porous carbon were produced by a hydrothermal template and the activation of hexamethylenetetramine (HMTA as a nitrogen source and activator) and ZnCl₂ (only as an activator) from a poly(Ri-S-ε-CL-PDMS) multiblock/graft copolymer produced using a renewable resource and eco-friendly autoxidation. N-doped carbon nanospheres (PPiSiHMTA) exhibited excellent CO₂ adsorption (2.73 mmol/g at 0 °C and 0.15 atm, 1.72 mmol/g at 25 °C and 0.15 atm) and CO₂/N₂ selectivity (344-512). Despite the higher BET surface area and pore volume, porous carbon (PPiSi) showed low CO₂ adsorption (1.21 and 0.71 mmol/g, 0.15 atm) and CO₂/N₂ selectivity (57 and 112). PPiSiHMTA and PPiSi have low isosteric heats of adsorption (Qst, 18-33 kJ/mol) and stability in humid environments. In addition, PPiSiHMTA exhibited an excellent CO₂ recycling performance. The experimental data on CO₂ adsorption was evaluated using various isotherm models, including Freundlich, Langmuir, Sips, and Temkin. The results demonstrated a nearly perfect fit between the Freundlich isotherm and the experimental data, indicating the heterogeneous nature of the adsorbent surfaces. Our study is promising for industrial applications, offering excellent CO₂ adsorption, CO₂/N₂ selectivity, moisture stability, and porous material fabrication strategies.