Abstract

Solid-liquid biphasic solvents (SLBSs) hold promise as energy-efficient candidates for CO2 capture. Nevertheless, the premature phase transition of current SLBSs leads to inopportune solid precipitation, posing operational challenges for the CO2 capture system. This study proposed a promising strategy that using aminoethylethanolamine (AEEA) as a regulator to fine-tune the phase transition time node of the 2-amino-2-methyl-1-propanol (AMP)/N-methylpyrrolidone (NMP) SLBS, enabling the phase transition to occur precisely as desired. Experimental results showed that the AEEA/AMP/NMP (A/A/N) SLBS exhibited tunable phase transition time nodes, modulated by the concentration of AEEA. Specifically, with the addition of 0.2 mol·L−1 AEEA, the CO2 loading associated with the phase transition increased significantly, from 0.19 to 0.54 mol·mol−1, approaching the saturation loading of 0.57 mol·mol−1. The delayed phase transition would facilitate the CO2 absorption operation. The regulatory mechanism of AEEA on the phase transition were thoroughly studied via 13C NMR and quantum calculations. AMP reacted with CO2 to produce AMPCOO− and AMPH+, which had a significantly stronger affinity for each other than for the solvent NMP, mediated by strong hydrogen bond interactions. Consequently, the continuous and fast aggregation of AMPCOO− and AMPH+ caused their swift precipitation from NMP. With the introduction of AEEA, the derived product AEEAH+(S)COO–(P) acted as a bridge-builder, connecting AMPCOO− or AMPH+ and NMP via hydrogen bonds, increasing the solubility of the AMP-derived products in NMP, thus effectively delaying the phase transition. Thermodynamic analysis revealed that the A/A/N SLBS exhibited a total regeneration energy consumption of 1.94 GJ·ton−1 CO2, representing a significant reduction of 48.9 % compared to that of 30 wt% MEA. This study provided a novel idea for designing SLBSs with controllable phase transition behavior, and offered a promising A/A/N SLBS for energy-efficient CO2 capture.

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