Two major aspects, which are CO2-specific binding sites (nitrogen) in conjunction with increased surface polarity by ionic groups (oxygen) , have been described in literature that facilitate the adsorption of CO2 in porous carbon materials. DFT calculations confirm a strong energetic interaction between CO2 and N-containing functional groups, in particular to multi-Ncontaining species like imidazole units. The laser-treatment of LPO2-Ade38090/Glu30010 under high O2 concentration enhances its surface polarity by introducing oxygen-containing groups such as C-O and C=O (Figure , Figure ) and strongly enhances the response (Figure ).