Development of novel AMP-based absorbents for efficient CO2 capture with low energy consumption through modifying the electrostatic potential
Development of novel AMP-based absorbents for efficient CO2 capture with low energy consumption through modifying the electrostatic potential
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DOI：
10.1016/j.cej.2023.145929
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发表时间：
2023-09
影响因子：
15.1
通讯作者：
Guanchu Lu;Zhe Wang;Zongyang Yue;Wenjing Wei;Yi Huang;Xiaolei Zhang;Xianfeng Fan
中科院分区：
文献类型：
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作者：
Guanchu Lu;Zhe Wang;Zongyang Yue;Wenjing Wei;Yi Huang;Xiaolei Zhang;Xianfeng Fan
用于捕获二氧化碳(CO2)的含水胺类吸收剂的高能耗阻碍了它们在全球的部署。这一挑战的一个潜在解决方案是利用非水胺系统，它提供了节能的替代方案。然而，它们在吸收二氧化碳的过程中容易形成沉淀，限制了它们的应用。实验和理论研究相结合，发现控制沉淀的主要因素是氨基甲酸酯的静电势，而不是范德华力，氢键可以有效地降低氨基甲酸酯的静电势，防止沉淀。单溶剂筛选实验也表明，吸收速率与有机溶剂的粘度和官能团对CO2的亲和力密切相关。极性溶剂(二甲基甲酰胺(DMF)、二甲基亚砜(DMSO)和N-甲基甲酰胺(NMF))表现出较高的吸收速率，但存在沉淀问题。富含羟基的溶剂(乙二醇和甘油)具有较低的吸收速率，但不存在沉淀问题。基于这些发现，开发了几种新型的基于2-氨基-2-甲基-1-丙醇(AMP)的非水吸收材料，旨在减少能量损失，改善CO2的吸收和解吸性能。其中AMP-EG-DMF(4-3)的CO_2吸收速率最大，吸收容量为9.91 mg·CO_2/(kg-soln·min)。和122g-CO2/(kg-soln.)，分别比30wt%AMP水溶液高64.1%和28.4%。此外，与30wt%的MEA相比，AMP-EG-DMF(4-3)的能耗降低了46.30%。EG的加入通过增加氢键的数目和强度，有效地改善了AMP-氨基甲酸酯的静电溶解性，从而避免了沉淀的产生。用~(13)C和~1H核磁共振、原位ATR-FTIR和量子化学计算分析了最终产物的种类和反应机理。理论和实验相结合的结果表明，基于AMP的双溶剂吸收剂可以作为低能CO2捕集的一种有前途的替代方案。
The global deployment of aqueous amine absorbents for carbon dioxide (CO2) capture is hindered by their high energy consumption. A potential solution to this challenge lies in the utilization of non-aqueous amine systems, which offer energy-efficient alternatives. However, they are prone to form precipitation during CO2absorption process, which limits their application. Combining experimental and theoretical studies, we found that the electrostatic potential of carbamate, instead of van der Waals force, is a major factor controlling the precipitation, and hydrogen bonds can effectively reduce the electrostatic potential of carbamate and prevent precipitation. Single solvent screening experiments have also demonstrated that the absorption rate is closely related to the viscosity of the organic solvent and the affinity of the functional group for CO2. The polar solvents (Dimethylformamide (DMF), Dimethyl sulfoxide (DMSO), and N-Methylformamide (NMF)) exhibit higher absorption rates, but suffer from issues of precipitation. Hydroxyl group riched solvents (Ethylene glycol (EG) and Glycerol) exhibit lower absorption rate, but they don’t have the issue of precipitation. Based on these findings, several novel 2-Amino-2-methyl-1-propanol (AMP)-based non-aqueous absorbents have been developed aiming at reducing the energy penalty, and improving CO2absorption and desorption performance. Among these absorbents, AMP-EG-DMF (4–3) exhibits maximum CO2absorption rate and absorption capacity of 9.91 g-CO2/(kg-soln.·min.) and 122 g-CO2/(kg-soln.), respectively, which are 64.1% and 28.4% higher than those of 30 wt% AMP aqueous solution, respectively. Additionally, compared to 30 wt% MEA, the energy consumption of AMP-EG-DMF (4–3) shows 46.30% reduction. The addition of EG effectively improves the electrostatic solubility of AMP-carbamate by increasing the number and strength of hydrogen bonds, thus avoiding the generation of precipitation. The final product species and reaction mechanism were analysed by using13C and1H NMR, In-situ ATR-FTIR, and quantum chemical calculation. The combination of theoretical and experimental results indicates that bi-solvent AMP-based absorbents can serve as a promising alternative for low-energy CO2capture.