The development of carbon-based adsorbents capable of reconciling high CO2 capture capacity with low regeneration energy consumption remains a challenge. Herein, we present porous carbon materials (InCPs–H2O–NC) derived from two isomeric In-based coordination polymers (InOF-25/26) through a combined strategy. The hydrolysis process induces hierarchical pore restructuring, while NH3 activation simultaneously achieves nitrogen doping and pore engineering. The obtained InCPs–H2O–NC exhibits a high specific surface area and tunable micro/mesoporosity, achieving an efficient CO2 adsorption capacity of 3.22 mmol g–1 at 298 K and 1.0 bar with moderate isosteric heats of adsorption (13.60–17.09 kJ mol–1), indicative of energy-efficient regeneration. It is noted that N doping introduces pyrrolic/pyridinic configurations to enhance the affinity of CO2 by electron donor–acceptor interactions, while hydrolysis-derived mesopores optimize diffusion kinetics. Theoretical simulations further confirm that N-induced charge redistribution strengthens the CO2 physisorption while reducing desorption energy barriers. This work highlights that the dimensional anisotropy of coordination polymers dictates directional pore evolution in their carbon derivatives, enabling synergistic integration of hierarchical porosity and surface polarity.
Liu et al. (Sun,) studied this question.