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Analysis for the speciation in CO2 loaded aqueous MEDA and MAPA solution using 13C NMR technology
International Journal of Greenhouse Gas Control ( IF 3.9 ) Pub Date : 2018-02-17 , DOI: 10.1016/j.ijggc.2018.02.001
Rui Zhang , Xiao Luo , Qi Yang , Hai Yu , Graeme Puxty , Zhiwu Liang

The competitive and cooperative reactions between the intramolecular primary and secondary amino groups in CO2 absorption have been investigated in this work. N-Methylethylenediamine (MEDA) and N-methylpropane-1,3-diamine (MAPA) were studied with various CO2 loadings at 25 °C. The 13C NMR technology was employed to obtain accurate 13C peak areas and chemical shifts for determining the concentration of each species in both of the diamine-CO2H2O systems. The results showed that the relative amounts of the species is primary-carbamate >> secondary-carbamate > di-carbamate in the CO2 absorption process. Moreover, the relative hydrolysis order of the carbamates is di-carbamate > secondary-carbamate > primary-carbamate. The competitive and cooperative reaction mechanism was then proposed based on these results. Finally, it was found that in both the MEDA and the MAPA ternary systems, the whole CO2 absorption process can be divided into three stages: competitive stage, buffer stage and hydrolysis stage, each of which showed a different trend in the amount of each species as well as in the pH value.



中文翻译:

使用13 C NMR技术分析CO 2负载的MEDA和MAPA水溶液中的形态

在这项工作中,已经研究了分子内伯氨基和仲氨基之间在CO 2吸收中的竞争性和协同反应。Ñ -Methylethylenediamine(MEDA)和Ñ -methylpropane -1,3-二胺(MAPA)与各种CO进行了研究2负载量在25℃下。采用13 C NMR技术获得准确的13 C峰面积和化学位移,以确定两种二胺-CO 2 H 2 O系统中每种物质的浓度。结果表明,CO 2中该种类的相对量为伯氨基甲酸酯>>仲氨基甲酸酯>二氨基甲酸酯吸收过程。此外,氨基甲酸酯的相对水解顺序为二氨基甲酸酯>仲氨基甲酸酯>伯氨基甲酸酯。基于这些结果,提出了竞争与合作反应机制。最后,发现在MEDA和MAPA三元系统中,整个CO 2吸收过程都可以分为三个阶段:竞争阶段,缓冲阶段和水解阶段,每个阶段的数量都有不同的趋势。种类以及pH值。

更新日期:2018-02-17
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