MEA吸收CO2富液解吸过程中固体颗粒表面的强化作用分析

doi:10.11949/0438-1157.20221565

摘要/Abstract

摘要：

单乙醇胺(MEA)溶液吸收二氧化碳在碳捕集封存或利用技术中应用广泛，但MEA吸收富液再生能耗高。有报道称具有催化性质的固体填料可以强化CO₂解吸，但固体作用原理并未被清楚证实。为了分析颗粒填料的作用，通过比较不同固体颗粒(硅铝比为25、50、80的HZSM-5和活性炭)在再生过程中的作用，证实了非稳态过程HZSM-5颗粒存在表面酸中心吸附有机胺促进解吸的现象，最大有15.75%的促进效果，呈现HZSM-5-25>HZSM-5-50>HZSM-5-80>AC>Blank的规律。但是，颗粒酸中心有限的吸附量不能持续促进解吸，恒温段的促进效果降低至1.61%~2.67%，此时传质即气泡成核是提升解吸速率的主要原因，颗粒表面提供非均相成核位点，疏水性强的表面更可能促进气液分离。通过传热影响分析，表明改变热通量对CO₂解吸速率的影响显著，相比传质速率与反应速率，传热速率在影响解吸速率的因素中占据主要地位。

关键词: 二氧化碳捕集, 解吸, 成核, 传质, 传热

Abstract:

The absorption of carbon dioxide by monoethanolamine (MEA) solution is widely used in carbon capture, utilization and storage technology, but the regeneration of MEA absorbing rich liquid requires high energy consumption. It has been reported that solid packing with catalytic properties can strengthen CO₂desorption, however, the principle of solid action has not been clearly demonstrated. In this work, in order to investigate the effects of the particle packing, the effect of different solid particles (HZSM-5 with Si/Al ratio of 25, 50, 80 and activated carbon) on the regeneration process was compared, and it was showed that the surface acid sites on HZSM-5 zeolite promoted desorption in transit period by the adsorption of amine, and the maximum effect was 15.75%. The promotion was in the order of HZSM-5-25>HZSM-5-50>HZSM-5-80>AC>Blank. However, the solid particles could not be served as a catalyst due to limited adsorption capacity of the acid sites, it did not show significant promotion influence on the desorption in the stable continuously operation. During the constant desorption period, the promotion effect was only 1.61%—2.67%. Compared the acidic particles with the non-acidic AC particle, heterogeneous bubble nucleation was suggested to be a reason to promote the desorption. A hydrophobic surface may be the efficient packing material in industrial device to enhance gas-liquid separation. Furthermore, the effect of heating rate was investigated, and the results showed that heat flux is a much more important factor compared with the influences of catalysis and nucleation.

Key words: CO₂ capture, desorption, bubble nucleation, mass transfer, heat transfer

中图分类号:

TQ 028.8

王皓, 唐思扬, 钟山, 梁斌. MEA吸收CO₂富液解吸过程中固体颗粒表面的强化作用分析[J]. 化工学报, 2023, 74(4): 1539-1548.

Hao WANG, Siyang TANG, Shan ZHONG, Bin LIANG. An investigation of the enhancing effect of solid particle surface on the CO₂ desorption behavior in chemical sorption process with MEA solution[J]. CIESC Journal, 2023, 74(4): 1539-1548.

图/表 14

参考文献 31

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时间/s	标准差
时间/s	HZSM-5-25	HZSM-5-50	HZSM-5-80	AC	Blank
0	3.59×10^-3	3.59×10^-3	3.59×10^-3	3.59×10^-3	3.59×10^-3
300	0	3.35×10^-3	1.38×10^-3	1.84×10^-3	2.88×10^-3
600	1.61×10^-3	3.25×10^-3	2.31×10^-3	2.39×10^-3	0.80×10^-3
900	3.35×10^-3	3.50×10^-3	2.80×10^-3	1.84×10^-3	0
1200	0.93×10^-3	3.04×10^-3	2.01×10^-3	1.66×10^-3	2.3×10^-3
1800	4.26×10^-3	0.80×10^-3	1.22×10^-3	2.39×10^-3	2.01×10^-3
2400	0.57×10^-3	3.34×10^-3	1.13×10^-3	3.60×10^-3	0

时间/s	标准差
时间/s	HZSM-5-25	HZSM-5-50	HZSM-5-80	AC	Blank
0	3.59×10^-3	3.59×10^-3	3.59×10^-3	3.59×10^-3	3.59×10^-3
300	0	3.35×10^-3	1.38×10^-3	1.84×10^-3	2.88×10^-3
600	1.61×10^-3	3.25×10^-3	2.31×10^-3	2.39×10^-3	0.80×10^-3
900	3.35×10^-3	3.50×10^-3	2.80×10^-3	1.84×10^-3	0
1200	0.93×10^-3	3.04×10^-3	2.01×10^-3	1.66×10^-3	2.3×10^-3
1800	4.26×10^-3	0.80×10^-3	1.22×10^-3	2.39×10^-3	2.01×10^-3
2400	0.57×10^-3	3.34×10^-3	1.13×10^-3	3.60×10^-3	0

时间/s	相对偏差/%
时间/s	HZSM-5-25	HZSM-5-50	HZSM-5-80	AC	Blank
0~300	4.2	0.1	7.1	3.0	9.0
300~600	6.4	5.6	3.0	5.2	4.0
600~900	8.5	10.3	7.9	7.6	3.1
900~1200	1.9	1.5	7.8	3.3	0.9
1200~1800	4.7	5.7	12.0	11.0	15.6
1800~2400	0.5	0.1	2.1	9.8	11.0
平均值	4.4	3.9	6.7	6.7	7.2

时间/s	相对偏差/%
时间/s	HZSM-5-25	HZSM-5-50	HZSM-5-80	AC	Blank
0~300	4.2	0.1	7.1	3.0	9.0
300~600	6.4	5.6	3.0	5.2	4.0
600~900	8.5	10.3	7.9	7.6	3.1
900~1200	1.9	1.5	7.8	3.3	0.9
1200~1800	4.7	5.7	12.0	11.0	15.6
1800~2400	0.5	0.1	2.1	9.8	11.0
平均值	4.4	3.9	6.7	6.7	7.2

颗粒	平均解吸速率/(mmol/min)	促进效果/%
HZSM-5-25	9.522	15.75
HZSM-5-50	9.299	13.04
HZSM-5-80	9.000	9.41
AC	8.358	1.60
Blank	8.226	—

MEA吸收CO₂富液解吸过程中固体颗粒表面的强化作用分析

An investigation of the enhancing effect of solid particle surface on the CO₂ desorption behavior in chemical sorption process with MEA solution

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图/表 14

参考文献 31

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颗粒	平均解吸速率/(mmol/min)	CO₂平衡浓度/ (mol/L)	CO₂实际浓度/ (mol/L)	过饱和度	促进效果/%
HZSM-5-25	8.7371	0.0016	0.0188	10.72	2.20
HZSM-5-50	8.7770	0.0016	0.0188	10.72	2.67
HZSM-5-80	8.6973	0.00159	0.0209	12.15	1.74
AC	8.6861	0.00159	0.0212	12.35	1.61
Blank	8.5487	0.00157	0.0272	16.37	—

名称	富液CO₂负载量/(mol/mol)	解吸温度/℃	平均解吸速率/ (mmol/min)
Blank1	0.4998	91~92	6.790^①	6.107^②
Blank2	0.4886	91~92	6.714^①	6.107^②
HZSM-5-25	0.4886	91~92	6.763^①	6.136^②

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