Experimental and Theoretical Investigation of the Reaction Between Co<sub>2</Sub> and Carbon Dioxide Binding Organic Liquids

Abstract

The reaction kinetics of CO2 absorption into new carbon dioxide binding organic liquids (CO(2)BOLs) was comprehensively studied to evaluate their potential for CO2 removal. A stopped-flow apparatus with conductivity detection was used to determine the CO2 absorption kinetics of novel CO(2)BOLs composed of DBN (1,5-diazabicyclo[4.3.0]non-5-ene)/1-propanol and TBD (1,5,7-triazabicyclo[4.4.0]dec-5-ene)/1-butanol. A modified termolecular reaction mechanism for the reaction of CO2 with CO(2)BOLs was used to calculate the observed pseudo-first order rate constant k(0) (s(-1)) and second-order reaction rate constant k(2) (m(3)/kmol.s). Experiments were performed by varying organic base (DBN or TBD) weight percentage in alcohol medium for a temperature range of 288-308 K. It was found that k(0) increased with increasing amine concentration and temperature. By comparing using two different CO2BOL systems, it was observed that the TBD/1-butanol system has faster reaction kinetics than the DBN/1-propanol system. Finally, experimental and theoretical activation energies of these CO2BOL systems were obtained and compared. Quantum chemical calculations using spin restricted B3LYP and MP2 methods were utilized to reveal the structural and energetic details of the single-step termolecular reaction mechanism.