Abstract

Monolithic binder-free CO 2 adsorbents with high adsorption capacity, selectivity, adsorption-desorption kinetics, and regenerability are highly desired to both reduce the environmental impact of anthropogenic CO 2 emissions and purify valuable gases from CO 2 . Herein, we report a strategy to prepare monolithic carbonaceous CO 2 adsorbents from low-cost and underutilized bioresources, which enabled the formation of a delicate anisotropic, hierarchical porous structure. With optimized material composition and processing conditions, the biobased carbon adsorbent demonstrated a CO 2 adsorption capacity of 4.49 mmol g -1 at 298 K and 100 kPa, relatively weak adsorbent-adsorbate affinity, good CO 2 /N 2 selectivity, and advantageous hydrophobicity against water vapor. Moreover, the unique anisotropic porous structure provided high stiffness and good flexibility to the adsorbent in the axial and radial directions, respectively. We confirmed that this type of carbon adsorbent could be packed in a column for dynamic CO 2 capture independent of any binders, indicating its promising future for further development toward widespread utilization. • Biocarbon aerogels with anisotropic, hierarchical porous structure were prepared. • Carbon aerogels reached CO 2 adsorption capacity of 4.49 mmol g −1 (298 K, 100 kPa). • Carbon aerogels showed good CO 2 /N 2 selectivity and low water vapor adsorption. • Carbon aerogels exhibited strong and unique anisotropic mechanical properties. • Carbon aerogels were packed in a column without binders for large-scale CO 2 capture.

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