A study on reaction mechanism and kinetics of CO2 and MEA/DEA- tertiary amines in non-aqueous and water-lean solutions

被引：23

作者：

Chen, Mengjie ^{[1
]}

Luo, Qinlan ^{[1
]}

Lin, Haizhou ^{[2
]}

Sun, Qiang ^{[1
]}

Gao, Hongxia ^{[1
]}

Liu, Sen ^{[1
]}

Li, Yuanyuan ^{[1
]}

Liang, Zhiwu ^{[1
]}

机构：

[1] Hunan Univ, Coll Chem & Chem Engn, Joint Int Ctr Capture & Storage iCCS CO2, Prov Hunan Key Lab Cost Effective Utilizat Fossil, Changsha 410082, Peoples R China

[2] Guangdong Elect Power Design Inst Co Ltd, China Energy Engn Grp, Guangzhou 510663, Peoples R China

来源：

CHEMICAL ENGINEERING SCIENCE | 2023年 / 269卷

基金：

中国国家自然科学基金;

关键词：

Kinetic model; Reaction mechanism; Blended amines; Zwitterion mechanism; Non-aqueous; CARBON-DIOXIDE REACTIONS; AQUEOUS N; N-DIETHYLETHANOLAMINE; CARBAMATE FORMATION; LIQUID AMINES; ABSORPTION; CAPTURE; ALKANOLAMINES; SOLUBILITY; MIXTURES; SYSTEMS;

D O I：

10.1016/j.ces.2022.118431

中图分类号：

TQ [化学工业];

学科分类号：

0817 ;

摘要：

The kinetic behavior of the reaction of CO2 with MEA-TREA in ethanol solution was studied using the stopped-flow technique. The results indicate that the zwitterion mechanism successfully correlates the experimentally measured pseudo first-order reaction constant (k0) and that the TREA participated in the deprotonation step of MEA-zwitterion as an alkaline substance after the formation of MEA-zwitterion. Then, the applicability of this proposed mechanism was investigated by using the reaction kinetics of CO2 with MEA-DMEA, MEA-DEEA, MEA-MDEA, DEA-TREA, DEA-DMEA blended amines in non-aqueous ethanol solution, as well as MEA-TREA, MEA-DMEA, DEA-TREA, DEA-DMEA blended amines in water-lean solutions. It was found that the mechanism of the reaction of CO2 with these mixed amines can be expressed by:k0 = KzA_A[A]2 + KzA_B[A][B] + Kz1[A]. The ethanol and water molecules which contribute to Kz1 can be used as proton transfer channels to accelerate proton transfer, but they do not directly par-ticipate in the reaction. In addition, the alkalinity and the steric hindrance effect controlled by the molec-ular structure of tertiary amines affected the reaction rate at the same time. The activation energies in MEA-EtOH and MEA-TREA-EtOH system were estimated by fitting the second-order rate constants to the Arrhenius expression, indicating that TREA can reduce the reaction activation energy and make the reaction more kinetically favorable.(c) 2023 Elsevier Ltd. All rights reserved.

引用

页数：13

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