中空纤维膜接触器中N,N-二甲基乙醇胺吸收CO2的特性

doi:10.16085/j.issn.1000-6613.2021-0757

化工进展 ›› 2022, Vol. 41 ›› Issue (4): 2132-2139.DOI: 10.16085/j.issn.1000-6613.2021-0757

中空纤维膜接触器中N,N-二甲基乙醇胺吸收CO₂的特性

吴佳佳¹(), 潘振¹(), 商丽艳², 孙秀丽², 孙超³, 孙祥广⁴

^1.辽宁石油化工大学石油天然气工程学院，辽宁抚顺 113001
^2.辽宁石油化工大学环境与安全工程学院，辽宁抚顺 ;113001
^3.中国石油管道局工程有限公司，河北廊坊 065000
^4.抚顺市特种设备监督检验所，辽宁抚顺 113001

收稿日期:2021-04-12 修回日期:2021-07-02 出版日期:2022-04-23 发布日期:2022-04-25
通讯作者: 潘振
作者简介:吴佳佳（1997—），女，硕士研究生，研究方向为天然气综合利用。E-mail：1580260350@qq.com。
基金资助:
辽宁省博士科研启动基金计划(2019-BS-159);辽宁省教育厅科学研究经费(L2019024);辽宁省教育厅重点科研项目(L2020002)

Characteristics of CO₂ absorption by N,N-dimethylethanolamine (DMEA) in hollow fiber membrane contactor

WU Jiajia¹(), PAN Zhen¹(), SHANG Liyan², SUN Xiuli², SUN Chao³, SUN Xiangguang⁴

^1.College of Petroleum Engineering, Liaoning Petrochemical University, Fushun 113001, Liaoning, China
^2.School of Environmental & Safety Engineering, Liaoning Petrochemical University, Fushun 113001, Liaoning, China
^3.China Petroleum Pipeline Engineering Co. , Ltd. , Langfang 065000, Hebei, China
^4.Fushun Special Equipment Supervision and Inspection Institute, Fushun 113001, Liaoning, China

Received:2021-04-12 Revised:2021-07-02 Online:2022-04-23 Published:2022-04-25
Contact: PAN Zhen

摘要/Abstract

摘要：

N,N-二甲基乙醇胺（DMEA）是一种很有前途的吸收剂，具有较快的反应速率和较高的CO₂捕集能力。在本研究中，DMEA作为一种新型吸收剂被应用于中空纤维膜接触器，用于从CO₂/CH₄气体混合物中分离CO₂。通过建立二维稳态数学模型，模拟了MEA、DEA、MDEA和DMEA四种吸收剂在不同操作条件下对CO₂吸收性能的影响。结果表明，脱碳性能大小为MEA>DMEA>DEA>MDEA；气相参数对脱碳率的影响比液相参数更显著；提高气体流速和CO₂浓度，脱碳率均会下降；提高液速和吸收剂浓度，脱碳率均增大，适当提高吸收剂流速和吸收剂浓度可以提高CO₂去除效率。此外，CO₂吸收通量将随着气体速度的增加而增加，随着液相中CO₂负荷的增加而减少。最后，通过两种影响因素共同作用确定了膜接触器分离酸性气体的最佳操作条件。因此，膜吸收法在天然气脱碳方面有良好的潜力。

关键词: CO₂捕集, 膜接触器, N,N-二甲基乙醇胺, 数值模拟, 传质

Abstract:

N,N-dimethylethanolamine (DMEA) is a promising absorbent because of its fast reaction rate and high CO₂ trapping ability. In this study, DMEA, as a new type of absorbent, was used in hollow fiber membrane contactors to separate CO₂ from CO₂/CH₄ gas mixtures. A two-dimensional steady-state mathematical model was established to simulate the effects of MEA (monoethanolamine), DEA (diethanolamine), MDEA (N-methyldiethanolamine) and DMEA on the absorption properties of CO₂ under different operating conditions. The results showed that the decarbonization performance was MEA>DMEA>DEA>MDEA, the effect of gas phase parameters on decarbonization rate was more significant than liquid phase parameters, the decarbonization rate decreased with the increase of gas flow rate and CO₂ concentration, the decarbonization rate increased with the increase of liquid velocity and absorbent concentration, and the removal efficiency of CO₂can be improved by properly increasing absorbent flow rate and absorbent concentration. In addition, the CO₂ absorption flux will increase with the increase of gas velocity and decrease with the increase of CO₂ load in the liquid phase. Finally, through the joint action of two influencing factors, the best operating conditions of membrane contactor for acid gas separation were determined. Therefore, membrane absorption had good potential in natural gas decarbonization.

Key words: CO₂ capture, membrane contactor, DMEA, numerical simulation, mass transfer

中图分类号:

TE64

吴佳佳, 潘振, 商丽艳, 孙秀丽, 孙超, 孙祥广. 中空纤维膜接触器中N,N-二甲基乙醇胺吸收CO₂的特性[J]. 化工进展, 2022, 41(4): 2132-2139.

WU Jiajia, PAN Zhen, SHANG Liyan, SUN Xiuli, SUN Chao, SUN Xiangguang. Characteristics of CO₂ absorption by N,N-dimethylethanolamine (DMEA) in hollow fiber membrane contactor[J]. Chemical Industry and Engineering Progress, 2022, 41(4): 2132-2139.

图/表 12

图1 中空纤维膜接触器

表1 中空纤维膜接触器参数

参数	数值
纤维内径r₁/μm	172
纤维外径r₂/μm	221
膜接触器半径r₃/μm	478
纤维长度L/m	0.8
膜孔径d_p/μm	0.02
纤维数量N	7000
膜孔隙率ε/%	45
薄膜弯曲度τ	2
有效膜面积S/m²	6.05

表2 管程、膜截面和壳程三区域控制微分方程的初始条件和边界条件

位置	管程	膜	壳程
z=0	$C C O 2 - t u b e = 0$ $C l i q - t u b e = C l i q - t u b e, i n i t i a l$		$? C C O 2 - s h e l l ? r = 0$
z=L			$C C O 2 - s h e l l = C C O 2, i n i t i a l$
r=0	$? C i - t u b e ? r = 0$
r=r₁	$? C l i q - t u b e ? r = 0$	$C C O 2 - m e m = C C O 2 - t u b e m$
r=r₂		$C C O 2 - m e m = C C O 2 - s h e l l$	$C C O 2 - s h e l l = m × C C O 2 - m e m$

表2 管程、膜截面和壳程三区域控制微分方程的初始条件和边界条件

位置	管程	膜	壳程
z=0	$C C O 2 - t u b e = 0$ $C l i q - t u b e = C l i q - t u b e, i n i t i a l$		$? C C O 2 - s h e l l ? r = 0$
z=L			$C C O 2 - s h e l l = C C O 2, i n i t i a l$
r=0	$? C i - t u b e ? r = 0$
r=r₁	$? C l i q - t u b e ? r = 0$	$C C O 2 - m e m = C C O 2 - t u b e m$
r=r₂		$C C O 2 - m e m = C C O 2 - s h e l l$	$C C O 2 - s h e l l = m × C C O 2 - m e m$

图2 所研究胺吸收剂的化学结构

表3 理化性质和动力学参数

参数	CO₂-MEA	CO₂-DEA	CO₂-MDEA	CO₂-DMEA	参考文献
壳程传质速率/m²·s^-1	1.8×10^-5				［26］
膜内传质速率/m²·s^-1	1.8×10^-5（ε/τ）				［10］
气体常数/m³·atm^-1·mol^-1·K^-1	8.314				［27］
亨利常数/mol·mol^-1	0.86	0.8	0.798	0.763	［10，27-28］
管程传质速率/m²·s^-1	1.29×10^-9	1.05×10^-9	1.11×10^-9	9.2×10^-10	［23，27-29］
管程液相传质速率/m²·s^-1	7.71×10^-10	4.97×10^-10	4.58×10^-10	5.8×10^-10	［23，27-29］
CO₂与吸收剂反应速率/m³·mol^-1·s^-1	6.244	5.814	5.259	22.911	［28-29］

图3 膜接触器中气液浓度分布

图4 建模预测与实验结果的CO2脱除效率比较

图5 气体流量对脱碳效率和CO2出口浓度的影响

图6 液体流量对脱碳效率的影响

图7 CO2入口浓度对脱碳效率的影响

图8 吸收剂浓度对脱碳效率的影响

图9 气体和液体条件对CO2吸收影响的3D趋势图

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中空纤维膜接触器中N,N-二甲基乙醇胺吸收CO₂的特性

Characteristics of CO₂ absorption by N,N-dimethylethanolamine (DMEA) in hollow fiber membrane contactor

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