N-doped carbon nanospheres synthesized from a newly designed eco-friendly sustainable polymer for highly selective CO2 capture

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. Graphical abstract: (Figure presented.) © The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2024.