Mechanisms of CO2 Capture into Monoethanolamine Solution with Different CO2 Loading during the Absorption/Desorption Processes

解吸 氨基甲酸酯 氨基甲酸 化学 吸收(声学) 两性离子 水解 反应机理 无机化学 有机化学 吸附 催化作用 分子 材料科学 复合材料
作者
Bihong Lv,Bingsong Guo,Zuoming Zhou,Guohua Jing
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:49 (17): 10728-10735 被引量:403
标识
DOI:10.1021/acs.est.5b02356
摘要

Though the mechanism of MEA-CO2 system has been widely studied, there is few literature on the detailed mechanism of CO2 capture into MEA solution with different CO2 loading during absorption/desorption processes. To get a clear picture of the process mechanism, (13)C nuclear magnetic resonance (NMR) was used to analyze the reaction intermediates under different CO2 loadings and detailed mechanism on CO2 absorption and desorption in MEA was evaluated in this work. The results demonstrated that the CO2 absorption in MEA started with the formation of carbamate according to the zwitterion mechanism, followed by the hydration of CO2 to form HCO3(-)/CO3(2-), and accompanied by the hydrolysis of carbamate. It is interesting to find that the existence of carbamate will be influenced by CO2 loading and that it is rather unstable at high CO2 loading. At low CO2 loading, carbamate is formed fast by the reaction between CO2 and MEA. At high CO2 loading, it is formed by the reaction of CO3(-)/CO3(2-) with MEA, and the formed carbamate can be easily hydrolyzed by H(+). Moreover, CO2 desorption from the CO2-saturated MEA solution was proved to be a reverse process of absorption. Initially, some HCO3(-) were heated to release CO2 and other HCO3(-) were reacted with carbamic acid (MEAH(+)) to form carbamate, and the carbamate was then decomposed to MEA and CO2.
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