Wan Zhijian, Hunt Russell, White Cameron, Gillbanks Jeremy, Czapla Jason, Xiao Gongkui, Surin Sophia, Wood Colin
Energy Business Unit, Commonwealth Scientific Industrial Research Organisation (CSIRO), Kensington, Western Australia, 6151, Australia.
Department of Chemical Engineering, The University of Western Australia, 35 Stirling Highway, Crawley, Western Australia, 6009, Australia.
ChemSusChem. 2024 Sep 23;17(18):e202400212. doi: 10.1002/cssc.202400212. Epub 2024 May 23.
Conventional usage of tetraethylenepentamine (TEPA) via being supported on porous solid materials for carbon capture is susceptible to oxidative degradation during regeneration cycles. This study reports a novel method to synthesize a TEPA based solid polymer for efficient CO removal via direct air capture (DAC). The polymer was obtained through epoxy-amine crosslinking reaction, leading to the transformation of liquid TEPA to a self-supported solid polymer. The synthesis was conducted under ambient conditions via a one-pot process with no waste products, which is aligned with green synthesis. The performance of the solid amine was evaluated in DAC under realistic conditions and compared with TEPA supported on SiO and zeolite 13X prepared through the conventional method. The solid TEPA amine exhibited a high CO uptake of 6.2 wt.% comparable to the conventional counterparts. More importantly, the solid TEPA amine demonstrated high resistance to oxidation during the accelerated ageing process at 80 °C in air for 24 h, whereas the two supported TEPA samples experienced severe degradation, with zeolite 13X supported TEPA incurring a reduction of 86.5 % in CO capturing capacity after the ageing. This work sheds light on the novel usage of TEPA as an efficient solid amine for practical DAC operation.
通过负载在多孔固体材料上用于碳捕获的传统四乙烯五胺（TEPA）在再生循环过程中易受氧化降解影响。本研究报道了一种通过直接空气捕获（DAC）合成基于TEPA的高效CO去除固体聚合物的新方法。该聚合物通过环氧 - 胺交联反应获得，导致液态TEPA转变为自支撑固体聚合物。合成在环境条件下通过一锅法进行，无废弃物产生，符合绿色合成理念。在实际条件下对该固体胺在DAC中的性能进行了评估，并与通过传统方法制备的负载在SiO和13X沸石上的TEPA进行了比较。固体TEPA胺表现出6.2 wt.%的高CO吸收量，与传统对应物相当。更重要的是，固体TEPA胺在80 °C空气中加速老化24小时的过程中表现出高抗氧化性，而两个负载TEPA样品经历了严重降解，老化后负载在13X沸石上的TEPA的CO捕获能力降低了86.5 %。这项工作揭示了TEPA作为用于实际DAC操作的高效固体胺的新用途。
