基于二乙烯三胺甲酸盐-乙醇胺-二甲亚砜无水CO2吸收剂的制备及性能

doi:10.16085/j.issn.1000-6613.2024-1446

摘要/Abstract

摘要：

针对传统醇胺水溶剂在吸收和解吸CO₂过程中出现的能耗高和腐蚀性强的问题，本文以乙醇胺（MEA）为主体吸收剂，二乙烯三胺甲酸盐（[DETAH][HCOO]）为活化剂，二甲亚砜（DMSO）为溶剂制备二乙烯三胺甲酸盐复配无水吸收剂（[DETAH][HCOO]-MEA-DMSO），并系统研究吸附剂的吸附性能、解吸性能及耐腐蚀性能。研究表明，在温度20℃、[DETAH][HCOO]与MEA的质量比为1∶1、[DETAH][HCOO]与MEA的总质量分数为20%、气液比为2∶1的条件下，无水吸收剂中部分氨基（—NH₂）与CO₂反应生成氨基甲酸，吸收CO₂后并未产生HCO₃^-/CO₃^2-，腐蚀性极低。无水吸收剂与水体系混合吸收剂相比，CO₂吸收容量提高了14.67%，CO₂最大吸收速率提高了1.24%，解吸负荷提高了35.61%，同时解吸能耗降低了54.41%。该研究为新型CO₂吸收剂的开发提供了新的思路，助力我国“双碳”战略的稳步实施。

关键词: CO₂捕集, 离子液体, 吸收, 解吸, 耐腐蚀性

Abstract:

In order to address the problems of high energy consumption and corrosive nature that occur in the absorption and desorption of CO₂ with traditional alcoholamine aqueous solvents, [DETAH][HCOO]-MEA-DMSO (diethylene-triamine formate) was fabricated by using ethanolamine (MEA) as the main adsorbent, [DETAH][HCOO] (diethylenetriamine) as the activator and DMSO (dimethyl sulfoxide) as the solvent. Desorption properties, resolving properties and corrosion resistance of the adsorbent were systematically investigated. It was confirmed that at the temperature of 20℃, the ratio of [DETAH][HCOO] and MEA was 1∶1, the total mass fraction of [DETAH][HCOO] and MEA was 20% and the gas-liquid ratio was 2∶1, part of the amino group (—NH₂) in the anhydrous absorbent reacted with CO₂ to form carbamic acid without HCO₃^-/CO₃^2- formation after absorbing CO₂ to produce very low corrosivity. Compared with the mixed absorbent of water system, it was found that the CO₂ absorption capacity of the nonaqueous absorbent was increased by 14.67%, the maximum CO₂ absorption rate was increased by 1.24%, the desorption load was increased by 35.61% and the energy consumption of desorption was reduced by 54.41%. This work provided a novel strategy for the development of CO₂ absorbent, which would strongly promote the steady implementation of the dual carbon strategy in China.

Key words: CO₂ capture, ion liquids, absorption, desorption, corrosion resistance

中图分类号:

TQ01-9

张样, 黄志甲, 谢福松, 鲁月红. 基于二乙烯三胺甲酸盐-乙醇胺-二甲亚砜无水CO₂吸收剂的制备及性能[J]. 化工进展, 2025, 44(10): 6073-6082.

ZHANG Yang, HUANG Zhijia, XIE Fusong, LU Yuehong. Preparation and properties investigation of CO₂ anhydrous absorbent based on diethylenetriamine-ethanolamine-dimethyl sulfoxide[J]. Chemical Industry and Engineering Progress, 2025, 44(10): 6073-6082.

图/表 15

表1 混合吸收剂吸收CO2前后的相态对比

有机溶剂	反应前	反应后
[DETAH][HCOO]-MEA-苯甲醇	均相	均相
[DETAH][HCOO]-MEA-N-甲基吡咯烷酮	均相	液-固分层
[DETAH][HCOO]-MEA-乙二醇甲醚	均相	液-固分层
[DETAH][HCOO]-MEA-乙二醇丁醚	均相	液-固分层
[DETAH][HCOO]-MEA-乙二醇二丁醚	均相	液-固分层
[DETAH][HCOO]-MEA-二甲亚砜	均相	均相
[DETAH][HCOO]-MEA-N,N-二甲基甲酰胺	均相	液-固分层
[DETAH][HCOO]-MEA-三甘醇单乙醚	均相	液-固分层
[DETAH][HCOO]-MEA-乙二醇乙醚	均相	液-固分层
[DETAH][HCOO]-MEA-聚乙二醇200	均相	均相
[DETAH][HCOO]-MEA-二乙二醇丁醚	均相	液-固分层

图1 部分混合吸收剂吸收CO2后出现分层现象

图2 CO2吸收实验装置示意图1—CO2检测仪；2—干燥器；3—冷凝器；4—温度计；5—水浴锅；6—磁力搅拌器；7—温度控制器；8—阀门；9—气体混合器；10—流量控制器；11—CO2气瓶；12—N₂气瓶

图3 CO2解吸实验装置示意图1—智能电表；2—油浴锅；3—低温恒温冷水浴池；4—冷凝管；5—温度计；6—流量计

图4 不同溶剂吸收容量对比

图5 吸收容量随温度变化

图6 不同溶剂解吸负荷对比

图7 不同溶剂解吸能耗对比

图8 无水吸收剂解吸率随温度变化

图9 无水吸收剂循环次数对吸收容量影响

图10 不同溶剂对CO2吸收速率的影响

表2 无水吸收剂的指标对比

参数	本文	参考文献[31]	参考文献[32]	参考文献[33]
吸收剂	无水吸收剂（[DETAH][HCOO]-MEA-DMSO）	MEA-DMSO	EHA-DMSO	L-苏氨酸钾溶液（PL-T）
吸收容量/mol·mol^-1	0.977	0.710	0.310	0.660
吸收速率/mol·(mol·min)^-1	0.00808	—	0.00246	0.00033
解吸负荷/mol·mol^-1	0.674	0.380	0.306	0.270
解吸能耗/MJ·kg^-1	3.10	—	22.95	0.515

图11 MEA-H2O、[DETAH][HCOO]-MEA-H2O和[DETAH][HCOO]-MEA-DMSO吸收剂腐蚀前后照片对比

图12 功能离子液体[DETAH][HCOO]的红外光谱图

图13 [DETAH][HCOO]-MEA-DMSO饱和溶液核磁共振碳谱

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基于二乙烯三胺甲酸盐-乙醇胺-二甲亚砜无水CO₂吸收剂的制备及性能

Preparation and properties investigation of CO₂ anhydrous absorbent based on diethylenetriamine-ethanolamine-dimethyl sulfoxide

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