基于表面活性剂改性单乙醇胺的新型多流态CO2吸收塔传质强化

doi:10.16085/j.issn.1000-6613.2025-1109

摘要/Abstract

摘要：

提出了一种结合雾化、发泡与填料的多流态CO₂吸收塔，通过使用表面活性剂AEO-9改性单乙醇胺（MEA）溶液，显著提升了CO₂的脱除效率。实验结果表明，AEO-9的引入使MEA的表面张力降低了约49.5%，有效促进了发泡现象，进而使CO₂脱除效率最高提升了31.8%。AEO-9对贫液黏度影响较小，但富液黏度增加了约37.5%，抑制了反应后期的发泡稳定性。并且¹³C NMR与FTIR表征证实，CO₂吸收产物对溶液物理化学性质没有显著影响。此外，正交试验与极差分析结果表明，液体流量和MEA浓度是影响CO₂脱除效率的关键因素，最佳操作条件为气体流量60L/min、液体流量500mL/min、CO₂体积分数8%、MEA质量分数30%。在此条件下，CO₂脱除效率提高48.42%以上，总吸收速率达1.198kmol/(m³·h)。该研究为多流态CO₂吸收塔的设计优化和工业应用提供了重要指导。

关键词: 表面活性剂改性, 多流态CO₂吸收, CO₂脱除效率, 传质强化, 吸收机理

Abstract:

This study proposes a multi-flow CO₂ absorption tower integrating atomization, foaming, and packing. By modifying the monoethanolamine（MEA） solution with the surfactant AEO-9, the CO₂ removal efficiency was significantly improved. Experimental results showed that the introduction of AEO-9 reduced the surface tension of MEA by approximately 49.5%, effectively promoting foaming and subsequently increasing CO₂ removal efficiency by 11.3%—31.8%. AEO-9 had minimal impact on solution viscosity; however, the viscosity of the rich solvent increased by about 37.5%, which suppressed foam stability in the later stages of the reaction. Characterization by ¹³C NMR and FTIR confirmed that CO₂ absorption products significantly influenced the physicochemical properties of the solution. Orthogonal experiments and range analysis identified liquid flow rate and MEA concentration as the key factors affecting CO₂ removal efficiency. The optimal operating conditions were determined to be a gas flow rate of 60L/min, liquid flow rate of 500mL/min, CO₂ concentration of 8%, and MEA concentration of 30%. Under these conditions, the CO₂ absorption efficiency increased by more than 48.42%, with a total absorption rate reaching 1.198kmol/(m³·h). This study provides important guidance for the design optimization and industrial application of multi-flow CO₂ absorption towers.

Key words: surfactant-modified, multi-phase-flow CO₂ absorption, decarbonization effectiveness, mass transfer mechanisms, absorption enhancement

中图分类号:

TQ028.1

王泽宇, 葛煜聪, 杨丽, 张真真, 衡迅瑄, 刘方, 杨霄. 基于表面活性剂改性单乙醇胺的新型多流态CO₂吸收塔传质强化[J]. 化工进展, 2025, 44(12): 6798-6812.

WANG Zeyu, GE Yucong, YANG Li, ZHANG Zhenzhen, HENG Xunxuan, LIU Fang, YANG Xiao. Foaming decarbonization performance of surfactant-modified monoethanolamine and application in co-current reactor[J]. Chemical Industry and Engineering Progress, 2025, 44(12): 6798-6812.

图/表 27

图1 泡沫性能测试装置

图2 鼓泡反应装置系统

图3 CO2平衡溶解度滴定装置

图4 多流态CO2吸收塔实验平台

表1 因素等级表

等级	气体流量（A）/L·min^-1	液体流量（B）/mL·min^-1	CO₂体积分数（C）/%	MEA质量分数（D）/%
1	40	200	8	10
2	50	300	10	20
3	60	400	12	30
4	70	500	14	35

表2 多流态吸收塔的正交实验设计因素与水平

实验编号	因素				等级
实验编号	A	B	C	D	A/L·min^-1	B/mL·min^-1	C/%	D/%
1	1	1	1	1	40	200	8	10
2	1	2	2	4	40	300	10	35
3	1	3	3	2	40	400	12	20
4	1	4	4	3	40	500	14	30
5	2	1	2	3	50	200	10	30
6	2	2	1	2	50	300	8	20
7	2	3	4	4	50	400	14	35
8	2	4	3	1	50	500	12	10
9	3	1	3	4	60	200	12	35
10	3	2	4	1	60	300	14	10
11	3	3	1	3	60	400	8	30
12	3	4	2	2	60	500	10	20
13	4	1	4	2	70	200	14	20
14	4	2	3	3	70	300	12	30
15	4	3	2	1	70	400	10	10
16	4	4	1	4	70	500	8	35

图5 起泡时间和泡沫半衰期

图6 CO2脱除效率

图7 不同复配比吸收剂CO2脱除速率

图8 不同MEA浓度下贫液与富液的起泡性能对比

图9 表面张力和黏度

图10 CO2平衡溶解度（α）

图11 CO2平衡溶解度逐时间图（α'）

图12 13C NMR光谱

表3 通过13C NMR化学位移识别的官能团[46-47]

化学位移	官能团/化学结构	所处碳环境
41.31/41.37	仲碳	R-NH-COO^-（氨基甲酸盐）
42.27/42.28	伯碳	CH₂-OH（MEA）
43.15	仲碳	R-NH-COO^-（氨基甲酸盐）
58.26/58.48	伯碳	CH₂-OH（MEA）
61.32/61.33	仲碳	CH₂-NH₂（MEA）
63.07	仲碳	CH₂-NH₂（MEA）
161.04/161.11	季碳	HCO₃^-或CO₃^2-（碳酸氢盐或碳酸盐）
164.72/164.73	季碳	HCO₃^-或CO₃^2-（碳酸氢盐或碳酸盐）

图13 FTIR光谱

表4 MEA富液的红外峰对应关系

波数/cm^-1	官能团（归属组分）
1565	$C O O -$ （氨基甲酸盐）
1488	$N H 3 +$ （质子化的MEA）
1386	$C — O$ (氨基甲酸盐)
1360	$C — N$ 或 $C — O$ （MEA, 氨基甲酸盐）
1326	$N — C O O -$ （氨基甲酸盐）
1066	$C — N$ 或 $C — O$ （质子化的MEA, 氨基甲酸盐）
958	$C — N H 2$ （MEA）

表4 MEA富液的红外峰对应关系

波数/cm^-1	官能团（归属组分）
1565	$C O O -$ （氨基甲酸盐）
1488	$N H 3 +$ （质子化的MEA）
1386	$C — O$ (氨基甲酸盐)
1360	$C — N$ 或 $C — O$ （MEA, 氨基甲酸盐）
1326	$N — C O O -$ （氨基甲酸盐）
1066	$C — N$ 或 $C — O$ （质子化的MEA, 氨基甲酸盐）
958	$C — N H 2$ （MEA）

表5 正交实验结果

实验编号	因素				CO₂脱除效率（Ψ）/%	总吸收速率（φ）/ kmol·m^-3·h^-1
实验编号	A	B	C	D	CO₂脱除效率（Ψ）/%	总吸收速率（φ）/ kmol·m^-3·h^-1
1	1	1	1	1	55.05	0.417
2	1	2	2	4	60.96	0.578
3	1	3	3	2	65.30	0.743
4	1	4	4	3	86.72	1.151
5	2	1	2	3	56.53	0.670
6	2	2	1	2	74.04	0.702
7	2	3	4	4	62.29	1.03
8	2	4	3	1	54.63	0.777
9	3	1	3	4	56.53	0.965
10	3	2	4	1	50.06	0.997
11	3	3	1	3	87.56	0.996
12	3	4	2	2	78.58	1.117
13	4	1	4	2	41.47	0.963
14	4	2	3	3	69.79	1.389
15	4	3	2	1	62.51	1.037
16	4	4	1	4	90.29	1.198

表6 CO2脱除效率的极差分析

实验编号	因素
实验编号	A	B	C	D
K₁	2.68	2.10	3.07	2.22
K₂	2.48	2.55	2.59	2.59
K₃	2.73	2.78	2.46	3.01
K₄	2.64	3.10	2.41	2.95
k₁	0.67	0.52	0.77	0.56
k₂	0.62	0.64	0.65	0.65
k₃	0.68	0.69	0.62	0.75
k₄	0.66	0.78	0.60	0.74
R_j	0.06	0.25	0.17	0.20
各因素最优水平	60L/min	500mL/min	8%	30%
各因素显著性排序	液体流量-MEA浓度-CO₂浓度-气体流量

图14 各因素对CO2脱除效率的影响程度

图15 各因素对总吸收速率的影响程度

表7 CO2总吸收速率的极差分析

实验编号	因素
实验编号	A	B	C	D
K₁	2.89	3.01	3.31	3.23
K₂	3.18	3.67	3.40	3.52
K₃	4.07	3.81	3.87	4.21
K₄	4.59	4.24	4.14	3.96
k₁	0.72	0.75	0.83	0.81
k₂	0.80	0.92	0.85	0.88
k₃	1.02	0.95	0.97	1.05
k₄	1.15	1.06	1.04	0.99
R_j	0.42	0.31	0.21	0.24
各因素最优水平	70L/min	500mL/min	14%	30%
各因素显著性排序	气体流量-液体流量-MEA浓度-CO₂浓度

图16 极差分析

图17 总气流量对CO2脱除效率和总吸收速率的影响

图18 液体流量对CO2脱除效率和总吸收速率的影响

图19 CO2浓度对CO2脱除效率和总吸收速率的影响

图20 MEA浓度对CO2脱除效率和总吸收速率的影响

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基于表面活性剂改性单乙醇胺的新型多流态CO₂吸收塔传质强化

Foaming decarbonization performance of surfactant-modified monoethanolamine and application in co-current reactor

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