Theoretical studies of carbon-centered organocatalysts for CO2 activation and mechanism studies for its conversion to methanol are the purposes of this research. Three possible pathways are proposed in this study for methanol production from CO2 and 9-BBN. Two distinct mechanisms can be considered for CO2 activation, which include an insertion reaction and a two-step reaction. The activation strain model (ASM) and electron localization function (ELF) concepts were applied for justification of the nucleophilic attack behavior of the studied organocatalysts in CO2 activation. Proton transfer in step 2 of the CO2 activation is studied as the rate-determining step of the reaction by nuclear-independent chemical shift (NICS-XY) scan. The results show that a lower absolute value of NICSnZZ in the case of organocatalysts with an electron-withdrawing group represents a higher stabilization in developing π-electron on the five-member ring of the organocatalysts and a lower ∆G≠ value than the other ones. Finally, the organocatalysts with the electron withdrawing substituents are kinetically and thermodynamically the best candidates for CO2 activation based on various different analyses.

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