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

被引:339
作者
Lv, Bihong [1 ]
Guo, Bingsong [1 ]
Zhou, Zuoming [1 ]
Jing, Guohua [1 ]
机构
[1] Huaqiao Univ, Dept Environm Sci & Engn, Coll Chem Engn, Xiamen 361021, Fujian, Peoples R China
基金
中国国家自然科学基金;
关键词
CARBON-DIOXIDE ABSORPTION; CARBAMATE FORMATION; AQUEOUS-SOLUTION; IONIC LIQUID; AB-INITIO; KINETICS; REGENERATION; STORAGE; ALKANOLAMINES; DESORPTION;
D O I
10.1021/acs.est.5b02356
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
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 CO, loading during absorption/desorption processes. To get a clear picture of the process mechanism, C-13 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-/CO32-, 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 CO, and MEA. At high CO2 loading, it is formed by the reaction of CO3-/CO32- with MBA, 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 carbarnic acid (MEAH(+)) to form carbamate, and the carbamate was then decomposed to MEA and CO2.
引用
收藏
页码:10728 / 10735
页数:8
相关论文
共 36 条
[1]   CO2 absorption in aqueous solutions of alkanolamines:: Mechanistic insight from quantum chemical calculations [J].
Arstad, Bjornar ;
Blom, Richard ;
Swang, Ole .
JOURNAL OF PHYSICAL CHEMISTRY A, 2007, 111 (07) :1222-1228
[2]  
BLAUWHOFF PMM, 1984, CHEM ENG SCI, V39, P207, DOI 10.1016/0009-2509(84)80021-4
[3]   Online NMR spectroscopic study of species distribution in MEA-H2O-CO2 and DEA-H2O-CO2 [J].
Boettinger, Wolfram ;
Maiwald, Michael ;
Hasse, Hans .
FLUID PHASE EQUILIBRIA, 2008, 263 (02) :131-143
[4]   Carbon capture and storage update [J].
Boot-Handford, M. E. ;
Abanades, J. C. ;
Anthony, E. J. ;
Blunt, M. J. ;
Brandani, S. ;
Mac Dowell, N. ;
Fernandez, J. R. ;
Ferrari, M. -C. ;
Gross, R. ;
Hallett, J. P. ;
Haszeldine, R. S. ;
Heptonstall, P. ;
Lyngfelt, A. ;
Makuch, Z. ;
Mangano, E. ;
Porter, R. T. J. ;
Pourkashanian, M. ;
Rochelle, G. T. ;
Shah, N. ;
Yao, J. G. ;
Fennell, P. S. .
ENERGY & ENVIRONMENTAL SCIENCE, 2014, 7 (01) :130-189
[5]   GAS-LIQUID MASS-TRANSFER WITH PARALLEL REVERSIBLE-REACTIONS .1. ABSORPTION OF CO2 INTO SOLUTIONS OF STERICALLY HINDERED AMINES [J].
BOSCH, H ;
VERSTEEG, GF ;
VANSWAAIJ, WPM .
CHEMICAL ENGINEERING SCIENCE, 1989, 44 (11) :2723-2734
[6]   Eddy Covariance Method for CO2 Emission Measurements in CCUS Applications: Principles, Instrumentation and Software [J].
Burba, George ;
Madsen, Rodney ;
Feese, Kristin .
EUROPEAN GEOSCIENCES UNION GENERAL ASSEMBLY 2013, EGUDIVISION ENERGY, RESOURCES & THE ENVIRONMENT, ERE, 2013, 40 :329-336
[7]   KINETICS OF CARBAMATE FORMATION AND BREAKDOWN [J].
CAPLOW, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1968, 90 (24) :6795-&
[8]   Comprehensive Kinetic and Thermodynamic Study of the Reactions of CO2(aq) and HCO3- with Monoethanolamine (MEA) in Aqueous Solution [J].
Conway, William ;
Wang, Xiaoguang ;
Fernandes, Debra ;
Burns, Robert ;
Lawrance, Geoffrey ;
Puxty, Graeme ;
Maeder, Marcel .
JOURNAL OF PHYSICAL CHEMISTRY A, 2011, 115 (50) :14340-14349
[9]   Ab initio study of the reaction of carbamate formation from CO2 and alkanolamines [J].
da Silva, EF ;
Svendsen, HF .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2004, 43 (13) :3413-3418
[10]   REACTION OF CO2 WITH ETHANOLAMINES [J].
DANCKWERTS, PV .
CHEMICAL ENGINEERING SCIENCE, 1979, 34 (04) :443-446