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2-Amino-2-methyl-1-propanol regulated triethylenetetramine-based nonaqueous absorbents for solid-liquid phase-change CO2 capture: Formation of crystalline powder products and mechanism analysis
Separation and Purification Technology ( IF 8.1 ) Pub Date : 2022-11-24 , DOI: 10.1016/j.seppur.2022.122722
Zhifang Tu , Fei Han , Chao Liu , Yingxue Wang , Jianwen Wei , Xiaobin Zhou

Solid-liquid phase-change absorbents (SLPCAs) have a great potential to reduce the energy consumption of CO2 capture. The main issue in the practical application of SLPCAs is the difficulty in the phase separation of gelatinous solid products. In this study, 2-amino-2-methyl-1-propanol (AMP) was used as a regulator to tune the physical form of the solid products of triethylenetetramine (TETA)-based SLPCAs. Experimental results showed that the AMP-regulated TETA-based SLPCAs successfully avoided the formation of gelatinous products (viscosity up to more than 1000 mPa·s) and yielded easily separated crystalline powders. Among the investigated SLPCAs, TETA/AMP/N-methyl-2-pyrrolidone (NMP) (TETA:AMP = 2:8, 1 M) exhibited the best CO2 capture performance with a high CO2 loading of 0.94 mol·mol−1 and a high regeneration efficiency of 84.14 %. XRD, FT-IR and 13C NMR analyses indicated that TETA/AMP/NMP absorbed CO2 to form highly polar carbamate species and protonated amines, which could break the original assimilation state of the SLPCA system; thus, the polar products precipitated out from less polar NMP, leading to a phase change. The theoretical calculations revealed that in the absence of AMP, the TETA-derived products had a tendency to form gelatinous aggregation with large amounts of hydrogen bonds; with the introduction of AMP, the AMP-derived products tended to combine with the TETA-derived products via strong electrostatic attraction and Van der Waals force and effectively inhibited the aggregation formation. Since there was only one hydrogen bond forming between the AMP- and TETA-derived product molecules, the amount of hydrogen bonds was significantly reduced. Eventually, the TETA/AMP/NMP SLPCA avoided the formation of gelatinous products and yielded crystalline powder products.



中文翻译:

2-氨基-2-甲基-1-丙醇调节三乙烯四胺基非水吸收剂用于固-液相变CO2捕获:结晶粉末产物的形成及机理分析

固液相变吸收剂 (SLPCA) 具有降低 CO 2捕获能耗的巨大潜力。SLPCAs实际应用中的主要问题是凝胶状固体产物的相分离困难。在这项研究中,2-amino-2-methyl-1-propanol (AMP) 被用作调节剂来调整基于三乙烯四胺 (TETA) 的 SLPCA 固体产物的物理形态。实验结果表明,AMP 调控的基于 TETA 的 SLPCAs 成功地避免了凝胶状产物(粘度高达 1000 mPa·s 以上)的形成,并产生易于分离的结晶粉末。在研究的 SLPCA 中,TETA/AMP/ N -methyl -2-pyrrolidone (NMP) (TETA:AMP = 2:8, 1 M) 表现出最好的 CO 2具有0.94 mol·mol -1的高 CO 2负载和 84.14 % 的高再生效率。XRD、FT-IR 和13 C NMR 分析表明 TETA/AMP/NMP 吸收了 CO 2形成高极性的氨基甲酸酯物种和质子化胺,可以打破SLPCA系统的原始同化状态;因此,极性产物从极性较小的 NMP 中沉淀出来,导致相变。理论计算表明,在不存在 AMP 的情况下,TETA 衍生产品倾向于形成具有大量氢键的凝胶状聚集体;随着AMP的引入,AMP衍生产物倾向于通过强静电引力和范德华力与TETA衍生产物结合,有效抑制聚集形成。由于 AMP 和 TETA 衍生产物分子之间仅形成一个氢键,因此氢键的数量显着减少。最终,

更新日期:2022-11-24
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