Primary and secondary amine-based sorbents were synthesized to investigate the operation capacity for the carbon dioxide separation TSA process. (3-Aminopropyl) triethoxysilane was used as a primary amine precursor as a crosslinking agent to synthesize a secondary amine precursor in which amine groups were crosslinked with a crosslinking agent. Carbon dioxide absorbed by primary amines is completely separated above 170 °C. The working capacity of the primary amine absorbent was less than 2% when regenerated at 130°C. The secondary amine absorbent has a higher carbon dioxide separation capacity at a lower regeneration temperature than the primary amine absorbent. The secondary amine absorbent could predict process operation performance of about 6.5% with 2% carbon dioxide absorption and 100% carbon dioxide regeneration conditions. Therefore, it was found that the working capacity of the secondary amine absorbent was higher than that of the primary amine.