New covalently tethered CO2 adsorbents are synthesized through the in situ polymerization of N-carboxyanhydride (NCA) of l-alanine from amine-functionalized three-dimensional (3D) interconnected macroporous silica (MPS). The interconnected macropores provide low-resistant pathways for the diffusion of CO2 molecules, while the abundant mesopores ensure the high pore volume. The adsorbents exhibit high molecular weight (of up to 13058 Da), high amine loading (more than 10.98 mmol N g(-1)), fast CO2 capture kinetics (t1/2 < 1 min), high adsorption capacity (of up to 3.86 mmol CO2 g(-1) in simulated flue gas and 2.65 mmol CO2 g(-1) in simulated ambient air under 1 atm of dry CO2), as well as good stability over 120 adsorption-desorption cycles, which allows the overall CO2 capture process to be promising and sustainable.

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Hierarchically porous materials containing interconnected macro-/meso-/micropores are promising candidates for energy storage, catalysis, and gas separation. Here, we present an effective approach for synthesizing three-dimensional (3D) sulfonated graphene coupled microporous organic polymers (SG-MOPs). The resulting SG-MOPs possess uniform macropores with an average size of ca. 350 nm, abundant mesopores, and micropores with an average size of ca. 0.6 nm. The SG-supported adsorbents exhibit a high nitrogen content (more than 38.1 wt %), high adsorption capacity (up to 3.37 mmol CO g), high CO/N selectivity from 42 to 51, moderate heat of adsorption, as well as good stability because of the hierarchical porous structure and excellent thermal conductivity of the SG scaffold. Thus, these nitrogen-enriched adsorbents allow the overall CO capture process to be promising and sustainable.