This paper describes the preparation of a Layered Silicate Sorbent (LSS) for CO2 capture using the layered silicate magadiite and organo-magadiite modified with polyethylenimine (PEI). The sorbents were characterized and revealed the presence of PEI as well as its interaction with CO2 at low temperatures. The thermal stability of sorbents was confirmed by thermogravimetry experiments, and the adsorption capacity was evaluated by CO2-TPD experiments. Two kinds of PEI are present in the sorbent, one exposed PEI layer that is responsible for higher CO2 adsorption because its sites are external and another one, bulky PEI, capable of low CO2 adsorption due to the internal position of sites. The contribution of the exposed PEI layer may be increased by a previous exchange of CTA(+), but the presence of the surfactant decreased the total adsorption capacity. MAG-PEI25 reached a maximum adsorption capacity of 6.11 mmol g(-1) at 75 °C for 3 h of adsorption and showed a kinetic desorption of around 15 min at 150 °C.
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