In the current work, computational modeling was used to explore the potential of 1,2,4-triazolylidene-derived N-heterocyclic olefins (trNHOs) systems as CO 2 capturer. After new structural modifications are performed, the energy required to activate CO 2 by m-trNHOs systems is lower than that observed in known analogous systems. Further substitutions were carried out in the triazolium ring showing that faster CO 2 sequestration or more suitable carboxylate for CO 2 storage can be favored depending on the selected substituent group. In addition, the nucleophilicity index, the molecular electrostatic potential (MESP) and the Density Overlap Regions Indicator (DORI) analysis were used to shed more light on their reactivity, stability and electronic structure.