个人信息Personal Information
教授
博士生导师
硕士生导师
性别:女
毕业院校:大连理工大学
学位:博士
所在单位:环境学院
学科:环境工程. 环境科学
办公地点:环境学院 B317
联系方式:0411-84706913
电子邮箱:lixuehua@dlut.edu.cn
论文成果
当前位置: 大连理工大学 李雪花 >> 科学研究 >> 论文成果Theoretical Investigation on the Different Reaction Mechanisms of Aqueous 2-Amino-2-methyl-1-propanol and Monoethanolamine with CO2
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论文类型:期刊论文
发表时间:2014-02-26
发表刊物:INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
收录刊物:SCIE、EI、Scopus
卷号:53
期号:8
页面范围:3363-3372
ISSN号:0888-5885
摘要:A fundamental understanding on the inherent mechanisms leading to the different reactivity of the representative systems for unhindered and hindered families of amines, monoethanolamine (MEA) and 2-amino-2-methyl-1-propanol (AMP) in CO2 capture, is important for the rational design of novel amines. In this work, a comparative study on the reaction mechanisms between AMP + CO2 and MEA + CO2 was investigated at the B3LYP/6-311++G(d,p) level with the appropriate treatment of solvent effects. Two channels that lead to carbamate and bicarbonate were considered. The total reaction rate coefficients, were computed using a microkinetic model. The results indicate that the formation of bicarbonate for AMP + CO2 is more favorable in kinetics than the formation of carbamate. However, the case is reversed for MEA + CO2. This explains well the experimental. observation of different product distributions between the AMP + CO2 and MEA + CO2 reactions. The complementary results from QM/MM molecular dynamics simulations with umbrella sampling confirm the mechanistic difference between AMP + CO2 and MEA + CO2. In addition, it is found that the difference in electrostatic potential distribution between C-a of AMP and MEA is a possible reason leading to their different reaction mechanisms.