Non-aqueous absorbents(NAAs)have attracted increasing attention for CO_(2)capture because of their great energy-saving potential.Primary diamines which can provide high CO_(2)absorption loading are promising candidates for formulating NAAs but suffer disadvantages in regenerability.In this study,a promising strategy that using tertiary amines(TAs)as proton-transfer mediators was proposed to enhance the regenerability of an aminoethylethanolamine(AEEA,diamine)/dimethyl sulfoxide(DMSO)(A/D)NAA.Surprisingly,some employed TAs such as N,N-diethylaminoethanol(DEEA),N,N,N’,N’’,N’’-pentamethyldiethylenetriamine(PMDETA),3-dimethylamino-1-propanol(3DMA1P),and N,N-dimethylethanolamine(DMEA)enhanced not only the regenerability of the A/D NAA but also the CO_(2)absorption performance.Specifically,the CO_(2)absorption loading and cyclic loading were increased by about 12.7%and 15.5%-22.7%,respectively.The TA-enhanced CO_(2)capture mechanism was comprehensively explored via nuclear magnetic resonance technique and quantum chemical calculations.During CO_(2)absorption,the TA acted as an ultimate proton acceptor for AEEA-zwitterion and enabled more AEEA to form carbamate species(AEEACOO-)to store CO_(2),thus enhancing CO_(2)absorption.For CO_(2)desorption,the TA first provided protons directly to AEEACOO-as a proton donor;moreover,it functioned as a proton carrier and facilitated the low-energy step-wise proton transfer from protonated AEEA to AEEACOO-.Consequently,the presence of TA made it easier for AEEACOO-to obtain protons to decompose,resulting in enhanced CO_(2)desorption.In a word,introducing the TA as a proton-transfer mediator into the A/D NAA enhanced both the CO_(2)absorption performance and the regenerability,which was an efficient way to“kill two birds with one stone”.
Xiaobin ZhouDanWangChao LiuGuohua JingBihong LvDunqiu Wang
