胺溶液吸收燃煤电厂烟气中CO2是目前减少CO2排放的有效技术途径.采用真实溶剂似导体屏蔽模型COSMO-RS结合密度泛函理论DFT预测了多种伯胺和仲胺溶液的pKa值,计算中采用了不同的密度泛函和基组方法,表明在BLYP/TZP方法下得到的pKa值与已有实验值符合最好.在BLYP/TZP方法下计算了各组分的吉布斯自由能,评估了胺溶液吸收CO2后溶液中氨基甲酸离子与碳酸氢根离子的比率.此外,通过液相状态下的DFT计算研究了氨甲基丙醇(AMP)溶液吸收CO2过程中碳酸氢根离子生成的反应机理,结果表明碳酸氢根离子更有可能是由胺、H2O和CO2直接反应生成,而不是由氨基甲酸离子水解生成.
参考文献
| [1] | Eirik F. da Silva;Hallvard F. Svendsen .Prediction of the pK_a Values of Amines Using ab Initio Methods and Free-Energy Perturbations[J].Industrial & Engineering Chemistry Research,2003(19):4414-4421. |
| [2] | Hidetaka Yamada;Shinkichi Shimizu;Hiromichi Okabe .Prediction of the Basicity of Aqueous Amine Solutions and the Species Distribution in the Amine-H2O-CO2 System Using the COSMO-RS Method[J].Industrial & Engineering Chemistry Research,2010(5):2449-2455. |
| [3] | Jae-Goo Shim;Jun-Han Kim;Young H Jhon .DFT Calculations on the Role of Base in the Reaction between CO2 and Monoethanolamine[J].Industrial & Engineering Chemistry Research,2009(4):2172-2178. |
| [4] | Xie, H.-B.;Zhou, Y.;Zhang, Y.;Johnson, J.K. .Reaction mechanism of monoethanolamine with CO_2 in aqueous solution from molecular modeling[J].The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory,2010(43):11844-11852. |
| [5] | Arstad B;Blom R;Swang O .CO2 absorption in aqueous solutions of alkanolamines: Mechanistic insight from quantum chemical calculations[J].The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory,2007(7):1222-1228. |
| [6] | Xu S.;Otto FD.;Mather AE.;Wang YW. .KINETICS OF THE REACTION OF CARBON DIOXIDE WITH 2-AMINO-2-METHYL-1-PROPANOL SOLUTIONS[J].Chemical Engineering Science,1996(6):841-850. |
| [7] | 牟天成,Jürgen Gmenhling.真实溶剂似导体屏蔽模型（COSMO-RS）[J].化学进展,2008(10):1487-1494. |
| [8] | 李庆领,范连翠,李太星,陈海龙.操作参数对MEA法捕集CO2吸收过程的影响研究[J].太原理工大学学报,2010(05):585-588. |
| [9] | 卢敏,武斌,朱家文,杨安.醇胺有机溶液吸收和解吸CO2的研究[J].石油与天然气化工,2006(02):117-118,124. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%