Biphasic solvents hold immense promise for CO2 capture, but often struggle to maintain stable performance over long-term cyclic use. Alcohols possess low dielectric constants, which can provide protons for amine-CO2 reaction products, enhancing the regeneration performance of absorbents while maintaining stability. In this study, diethylenetriamine (DETA) + 2-(diethylamino)ethanol (DEEA) + H2O was used as the biphasic solvent, with n-propanol (PrOH) serving as the regulator to develop the DETA + DEEA + PrOH water-lean biphasic solvent. Replacing half of the water with PrOH improved the cyclic stability of the absorbent, reduced the rich phase ratio (46 %) and energy consumption (2.05 GJ·ton−1 CO2), while effectively enhanced corrosion resistance and thermal stability, confirming the feasibility of PrOH as the regulator. The detailed reaction mechanism of the absorbent for CO2 absorption was elucidated through 13C NMR and DFT calculations. Quantum chemical calculations have provided the first compelling evidence for PrOH’s involvement in the absorption reaction: PrOH stores the reaction products in the form of PrOCOOH/PrOCOO−. By regenerating DETA, it restores its CO2 absorption capacity. Through polarity and hydrogen bonding, the reaction products aggregate in one phase, enhancing CO2 loading. In summary, the PrOH regulated water-lean biphasic solvent presents a highly promising absorbent for industrial use.
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