膜接触器内TETA-DEEA-TMS-H2O相分离捕获剂吸收CO2传质性能

doi:10.16085/j.issn.1000-6613.2023-1811

化工进展 ›› 2024, Vol. 43 ›› Issue (11): 6039-6048.DOI: 10.16085/j.issn.1000-6613.2023-1811

• 化工过程与装备 • 上一篇

膜接触器内TETA-DEEA-TMS-H₂O相分离捕获剂吸收CO₂传质性能

吴大卫¹(), 尹一涵², 曹智勇², 林海周¹, 范永春¹, 高红霞²(), 梁志武²

^1.中国能源建设集团广东省电力设计研究院有限公司，广东广州 510663
^2.湖南大学二氧化碳捕获与封存国际合作中心，化石能源低碳化高效利用湖南省重点实验室，湖南大学化学化工学院，湖南长沙 410082

收稿日期:2023-10-16 修回日期:2024-01-12 出版日期:2024-11-15 发布日期:2024-12-07
通讯作者: 高红霞
作者简介:吴大卫（1993—），男，博士，研究方向为二氧化碳捕获技术。E-mail：wudawei@gedi.com.cn。
基金资助:
中国能建广东院院级科技项目(EV11211W)

Experimental study on CO₂ mass transfer performance of TETA-DEEA-TMS-H₂O phase separation absorbent in hollow fiber membrane contactor

WU Dawei¹(), YIN Yihan², CAO Zhiyong², LIN Haizhou¹, FAN Yongchun¹, GAO Hongxia²(), LIANG Zhiwu²

^1.China Energy Construction Group Guangdong Electric Power Design and Research Institute Co. , Ltd. , Guangzhou 510663, Guangdong, China
^2.Joint International Center for CO2 Capture and Storage (iCCS)/Hunan Provincial Key Laboratory for Cost-effective Utilization of Fossil Fuel Aimed at Reducing CO2 Emissions/College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, Hunan, China

Received:2023-10-16 Revised:2024-01-12 Online:2024-11-15 Published:2024-12-07
Contact: GAO Hongxia

摘要/Abstract

摘要：

化学吸收法特别是胺法捕获燃烧后尾气中的CO₂目前最具产业化应用前景。然而，传统胺溶液[以30%单乙醇胺（MEA）为基准]存在再生能耗高等难题，在填料塔内吸收CO₂可能会存在液泛、发泡、夹带等操作运行问题。胺基相分离型CO₂吸收剂吸收CO₂后，仅需送富CO₂相溶液去解吸，有望大幅降低CO₂解吸能耗。本文通过高效胺基相分离型捕获剂耦合中空纤维膜接触器强化CO₂吸收传质。首先，利用CO₂吸收-解吸筛选装置探究了几种吸收剂的CO₂吸收-解吸综合性能和分相特性，实验结果表明三乙烯四胺（TETA）-N,N-二乙基乙醇胺（DEEA）-环丁砜（TMS）-水具有较好的分相性能和CO₂捕获性能。然后，在中空纤维膜接触器内研究了CO₂负载量、TETA浓度、液相进料温度、液体流速、进口气速和CO₂分压对TETA-DEEA-TMS-H₂O相分离吸收剂CO₂吸收通量的影响规律。结果表明：CO₂吸收通量随CO₂负载量的增加而降低，随液相进料温度、液体流速、进口气速和CO₂分压的增大而增大，由于分相原因使CO₂吸收通量随TETA浓度的增加呈现先增大后减小的趋势；CO₂脱除率与进口气速和CO₂分压呈负相关关系。最后，建立了较准确的气相总传质系数K_G的预测模型，其绝对平均误差为11.94%。

关键词: 二氧化碳, 相分离型吸收剂, 膜接触器, 吸收-解吸, 传质

Abstract:

Chemical absorption methods, especially the amine method, are currently the most promising for industrialization of CO₂ capture in post-combustion exhaust gases. However, traditional amine solutions [based on 30% monoethanolamine (MEA)] have high energy consumption for regeneration, and CO₂ absorption in packed towers may have operational problems such as liquid flooding, foaming, and entrainment. The amine-based phase separation CO₂ absorbent is expected to significantly reduce CO₂ desorption energy consumption, because only the CO₂-rich phase solution needs to be sent for desorption. In this paper, the CO₂ absorption mass transfer was enhanced by a highly efficient amine-based phase separation absorbent coupled with a hollow fiber membrane contactor. Firstly, the comprehensive CO₂ absorption-desorption performance and phase-separation characteristics of several absorbents were investigated by using CO₂ absorption-desorption device. The experimental results showed that triethylenetetramine (TETA)-diethylaminoethanol (DEEA)-cyclobutanesulfone (TMS)-water had better phase-separation and CO₂ capture performance. Then, the effects of CO₂ loading, TETA concentration, liquid phase temperature, liquid flow rate, inlet gas velocity, and CO₂ partial pressure on the CO₂ absorption flux of TETA-DEEA-TMS-H₂O phase separation absorbent were investigated in a hollow fiber membrane contactor. The results showed that the CO₂ absorption flux decreased with the increase of the CO₂ loading and increases with the increase of the liquid phase temperature, liquid flow rate, inlet gas velocity, and CO₂ partial pressure. At the same time, the CO₂ absorption flux tended to increase and then decrease with increase of the TETA concentration due to phase separation. The CO₂ removal rate had a negative correlation with the inlet gas velocity and CO₂ partial pressure. Finally, a more accurate prediction model of the gas-phase total mass transfer coefficient K_G was established with an absolute average deviation of 11.94%.

Key words: CO₂ capture, membrane contactors, phase separation absorbent, absorption and desorption, mass transfer

中图分类号:

X511

吴大卫, 尹一涵, 曹智勇, 林海周, 范永春, 高红霞, 梁志武. 膜接触器内TETA-DEEA-TMS-H₂O相分离捕获剂吸收CO₂传质性能[J]. 化工进展, 2024, 43(11): 6039-6048.

WU Dawei, YIN Yihan, CAO Zhiyong, LIN Haizhou, FAN Yongchun, GAO Hongxia, LIANG Zhiwu. Experimental study on CO₂ mass transfer performance of TETA-DEEA-TMS-H₂O phase separation absorbent in hollow fiber membrane contactor[J]. Chemical Industry and Engineering Progress, 2024, 43(11): 6039-6048.

图/表 13

表1 中空纤维膜和接触器详细参数

名称	参数	单位	数值
PTFE中空纤维膜	膜内径	mm	1.0
	膜外径	mm	1.7
	平均孔径	μm	0.3
	孔隙度	%	50
接触器	有效长度	cm	20×3
	组件内径	mm	18
	装填膜数量	根	20
	填充度	%	17.8

图1 CO2吸收实验装置图1—气体流量控制器；2—气体混合器；3—水饱和器；4—恒温水浴锅；5—冷却装置；6—干燥管；7—CO2红外分析仪；8—外接工作台

图2 CO2解吸实验装置图1—气体流量控制器；2—气体混合器；3—防倒吸吸收瓶；4—恒温油浴锅；5—温度计；6—冷却装置；7—干燥管；8—CO2红外分析仪；9—外接工作台

图3 中空纤维膜接触器内CO2吸收实验装置图1—气体流量控制器；2—气体混合器；3—中空纤维膜接触器；4—恒温水浴锅；5—恒流蠕动泵；6—贫液槽；7—干燥管；8—CO2红外分析仪；9—外接工作台；10—富液槽

图4 吸收速率变化曲线

图5 CO2负载随解吸时间的变化曲线

图6 CO2负载量对JCO2的影响规律

图7 TETA浓度对JCO2的影响规律

图8 液相进料温度对JCO2的作用规律

图9 液体流速与JCO2的作用规律

图10 进口气速对JCO2和ηCO2的作用规律

图11 CO2分压对JCO2和ηCO2的作用规律

图12 KG实验值和预测值比较

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膜接触器内TETA-DEEA-TMS-H₂O相分离捕获剂吸收CO₂传质性能

Experimental study on CO₂ mass transfer performance of TETA-DEEA-TMS-H₂O phase separation absorbent in hollow fiber membrane contactor

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