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The synthesis of five-membered cyclic carbonates via catalytic cycloaddition reaction of CO2 with epoxides is considered to be an effective technology for alleviation of the energy crisis and global warming. Various commercial organic bases and ionic salts were used as catalysts, while the relationship of catalytic activity and compound structure has been seldom explored. Herein, a facilely obtained binary catalytic system based on triethylamine/NBu4Br was developed for CO2 activation and chemical fixation. The highly efficient catalytic system showed outstanding conversion and above 99% selectivity under metal-free mild reaction conditions (100 degrees C, 1 atm) in one hour. The detailed process of CO2 activation and chemical fixation was investigated at the molecular level by a series of experiments and theoretical calculation, which provided a mode for the design and synthesis of a highly efficient catalytic system for conversion of CO2 under mild conditions.