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Polymers rich in primary amine groups are proposed to be effective adsorbents for the reversible adsorption of CO2 from moderately dilute gas streams (10% CO2) and ultra-dilute gas streams (e.g. ambient air, 400 ppm CO2), with their performance under ultra-dilute conditions being competitive with or exceeding the state-of-the-art adsorbents based on supported poly(ethyleneimine) (PEI). The CO2 adsorption capacity (mmol CO2/g sorbent) and amine efficiency (mmol CO2/mmol amine) of linear poly(allylamine) (PAA), cross-linked poly(allylamine) prepared by post-polymerization crosslinking with epichlorohydrin (PAAEPI), and branched poly(allylamine) prepared by branching of poly(allylamine) with divinylbenzene (PAADVB) are presented here and compared with state-of-the-art adsorbents based on supported PEI, specifically branched and linear, low molecular weight PEI. Silica mesocellular foam, MCF, serves as the support material for impregnation of the amine polymers. In general, branched polymers are found to yield more effective adsorbents materials. Overall, the results of this work show that linear PAA, cross-linked PAAEPI, and branched PAADVB are promising candidates for solid adsorbents with high capacity for CO2.