Mass transfer study of CO2 absorption by TETA/DEEA biphasic absorbent in the microchannel

doi:10.11949/0438-1157.20241447

Abstract

Abstract:

The CO₂ absorption and mass transfer characteristics of the TETA/DEEA (triethylenetetramine/diethylaminoethanol) biphasic absorbent solution in the microchannel were investigated by high-speed video, and the effects of two-phase flow rates, absorbent concentration, and TETA proportion in the total amine on the initial bubble length L_B0, bubble volume reduction ΔV_B, CO₂ absorption percent φ and liquid-side volumetric mass transfer coefficient k_La were systematically examined. The results show that L_B0is closely related to ΔV_B, and both decrease with the increase of liquid flow rate, total amine concentration and the proportion of TETA in total amines, as well as the decrease of gas flow rate. For CO₂ absorption percent, it decreased with the increase of gas flow rate, and showed a tendency of increasing and then decreasing with the increase of TETA proportion. The experimentally measured k_La values ranged from 0.88 s^-1 to 13.65 s^-1, which were 1—2 orders of magnitude higher than those of the conventional reactor, indicating that the microchannel reactor can significantly enhance the CO₂ capture process by the TETA/DEEA biphasic absorbent. In addition, based on the experimental data, an empirical correlation was proposed to predict the k_La with good prediction performance.

Key words: microchannels, biphasic absorbent, absorption, gas-liquid flow, mass transfer

摘要：

利用高速摄像研究了微通道内两相吸收剂三乙烯四胺/二乙氨基乙醇（TETA/DEEA）的CO₂吸收传质特性，系统考察了气液两相流量、吸收剂总胺浓度及总胺中TETA占比对初始气泡长度L_B0、气泡体积减小量ΔV_B、CO₂吸收率φ和液侧体积传质系数k_La的影响。结果表明，L_B0与ΔV_B密切相关，均随液体流量、总胺浓度和总胺中TETA占比的增加，以及气体流量的降低而降低。CO₂吸收率随气体流量的增加而降低，随总胺中TETA占比的增加呈现先增加后降低的趋势。实验测得的k_La值在0.88~13.65 s^-1之间，比传统反应器高1~2个数量级，表明微通道反应器可显著强化TETA/DEEA两相吸收剂捕集CO₂过程。此外，基于实验数据提出了k_La预测关联式，预测效果较好。

关键词: 微通道, 两相吸收剂, 吸收, 气液两相流, 传质

CLC Number:

TQ 021.4

Xiaotian MI, Hongchen LIU, Kejun WANG, Wenna TANG, Yongwei XU, Mei YANG. Mass transfer study of CO₂ absorption by TETA/DEEA biphasic absorbent in the microchannel[J]. CIESC Journal, 2025, 76(6): 2667-2677.

米晓天, 刘宏臣, 王克军, 唐文娜, 徐永伟, 杨梅. 微通道内两相吸收剂TETA/DEEA吸收CO₂过程的传质研究[J]. 化工学报, 2025, 76(6): 2667-2677.

Figures/Tables 14

Table 1 Physical properties of the TETA/DEEA biphasic solvents

C_TETA/(mol/L)	C_DEEA/(mol/L)	总胺浓度 C_T/(mol/L)	总胺中TETA 占比M	密度 ρ/(kg·m^-3)	黏度 μ/(mPa·s)
0.5	2.0	2.5	0.2	965	7.6
0.6	2.4	3.0	0.2	970	12.2
0.7	2.8	3.5	0.2	968	22.3
0.8	3.2	4.0	0.2	948	30.7
1.6	2.4	4.0	0.4	979	78.9
2.4	1.6	4.0	0.6	989	118.8
3.2	0.8	4.0	0.8	992	122.6

Fig.1 (a) Schematic diagram of the microchannel structure;(b) Sketch of the experimental setup

Fig.2 Typical flow patterns for gas-liquid flow in the microchannel

Fig.3 Effect of gas-liquid two-phase flow rates on initial bubble length (CT=4 mol/L, M=0.2)

Fig.4 Effect of absorbent concentrations on initial bubble length (M=0.2, QG=20 mL/min)

Fig.5 Effect of TETA proportion on initial bubble length (CT=4 mol/L, QG=20 mL/min)

Fig.6 Effect of gas flow rates on the evolution of bubble volume reduction (a) and CO2 absorption percent (b) along the microchannel (QL=3 ml/min, CT=4 mol/L, M=0.2)

Fig.7 Effect of liquid flow rates on the evolution of bubble volume reduction (a) and CO2 absorption percent (b) along the microchannel (QG=4 ml/min, CT=4 mol/L, M=0.2)

Fig.8 Effect of absorbent concentrations on the evolution of bubble volume reduction (a) and CO2 absorption percent (b) along the microchannel (M=0.2, QL=5 ml/min, QG=20 mL/min)

Fig.9 Effect of TETA proportion on the evolution of bubble volume reduction (a) and CO2 absorption percent (b) along the microchannel (CT=4 mol/L, QL=5 ml/min, QG=20 mL/min)

Fig.10 Effect of gas-liquid flow rates on liquid side volumetric mass transfer coefficient (CT=4 mol/L, M=0.2)

Fig.11 Effect of absorbent concentrations on liquid side volumetric mass transfer coefficient (M=0.2, QG=20 ml/min)

Fig.12 Effect of TETA proportion on liquid side volumetric mass transfer coefficient (CT=4 mol/L, QG=20 ml/min)

Fig.13 Comparison of experimental and predicted values of kLa

References 39

[1]	Hepburn C, Adlen E, Beddington J, et al. The technological and economic prospects for CO₂ utilization and removal[J]. Nature, 2019, 575(7781): 87-97.
[2]	Bui M, Adjiman C S, Bardow A, et al. Carbon capture and storage (CCS): the way forward[J]. Energy & Environmental Science, 2018, 11(5): 1062-1176.
[3]	Liang Z W, Fu K Y, Idem R, et al. Review on current advances, future challenges and consideration issues for post-combustion CO₂ capture using amine-based absorbents[J]. Chinese Journal of Chemical Engineering, 2016, 24(2): 278-288.
[4]	Veawab A, Tontiwachwuthikul P, Chakma A. Corrosion behavior of carbon steel in the CO₂ absorption process using aqueous amine solutions[J]. Industrial & Engineering Chemistry Research, 1999, 38(10): 3917-3924.
[5]	Borhani T N, Wang M H. Role of solvents in CO₂ capture processes: the review of selection and design methods[J]. Renewable and Sustainable Energy Reviews, 2019, 114: 109299.
[6]	Jing G H, Qian Y H, Zhou X B, et al. Designing and screening of multi-amino-functionalized ionic liquid solution for CO₂ capture by quantum chemical simulation[J]. ACS Sustainable Chemistry & Engineering, 2018, 6(1): 1182-1191.
[7]	Sun C, Wen S J, Zhao J K, et al. Mechanism and kinetics study of CO₂ absorption into blends of N-methyldiethanolamine and 1-hydroxyethyl-3-methylimidazolium glycine aqueous solution[J]. Energy & Fuels, 2017, 31(11): 12425-12433.
[8]	Heldebrant D J, Koech P K, Glezakou V A, et al. Water-lean solvents for post-combustion CO₂ capture: fundamentals, uncertainties, opportunities, and outlook[J]. Chemical Reviews, 2017, 117(14): 9594-9624.
[9]	Raksajati A, Ho M T, Wiley D E. Comparison of solvent development options for capture of CO₂ from flue gases[J]. Industrial & Engineering Chemistry Research, 2018, 57(19): 6746-6758.
[10]	Wang X F, Akhmedov N G, Hopkinson D, et al. Phase change amino acid salt separates into CO₂-rich and CO₂-lean phases upon interacting with CO₂ [J]. Applied Energy, 2016, 161: 41-47.
[11]	Zhang X W, Zhang R, Liu H L, et al. Evaluating CO₂ desorption performance in CO₂-loaded aqueous tri-solvent blend amines with and without solid acid catalysts[J]. Applied Energy, 2018, 218: 417-429.
[12]	Zhang W D, Jin X H, Tu W W, et al. Development of MEA-based CO₂ phase change absorbent[J]. Applied Energy, 2017, 195: 316-323.
[13]	Zhuang Q, Clements B, Dai J Y, et al. Ten years of research on phase separation absorbents for carbon capture: achievements and next steps[J]. International Journal of Greenhouse Gas Control, 2016, 52: 449-460.
[14]	Raynal L, Bouillon P A, Gomez A, et al. From MEA to demixing solvents and future steps, a roadmap for lowering the cost of post-combustion carbon capture[J]. Chemical Engineering Journal, 2011, 171(3): 742-752.
[15]	Yang F S, Jin X H, Fang J W, et al. Development of CO₂ phase change absorbents by means of the cosolvent effect[J]. Green Chemistry, 2018, 20(10): 2328-2336.
[16]	Wang L D, Liu S S, Wang R J, et al. Regulating phase separation behavior of a DEEA-TETA biphasic solvent using sulfolane for energy-saving CO₂ capture[J]. Environmental Science & Technology, 2019, 53(21): 12873-12881.
[17]	Zhang S H, Shen Y, Shao P J, et al. Kinetics, thermodynamics, and mechanism of a novel biphasic solvent for CO₂ capture from flue gas[J]. Environmental Science & Technology, 2018, 52(6): 3660-3668.
[18]	Wang L D, Yu S H, Li Q W, et al. Performance of sulfolane/DETA hybrids for CO₂ absorption: phase splitting behavior, kinetics and thermodynamics[J]. Applied Energy, 2018, 228: 568-576.
[19]	Ye Q, Wang X L, Lu Y Q. Screening and evaluation of novel biphasic solvents for energy-efficient post-combustion CO₂ capture[J]. International Journal of Greenhouse Gas Control, 2015, 39: 205-214.
[20]	Zhang S H, Shen Y, Wang L D, et al. Phase change solvents for post-combustion CO₂ capture: principle, advances, and challenges[J]. Applied Energy, 2019, 239: 876-897.
[21]	Aghel B, Sahraie S, Heidaryan E, et al. Experimental study of carbon dioxide absorption by mixed aqueous solutions of methyl diethanolamine (MDEA) and piperazine (PZ) in a microreactor[J]. Process Safety and Environmental Protection, 2019, 131: 152-159.
[22]	宋仕容, 刘宏臣, 米晓天, 等. 同轴微通道内管结构对液滴生成的影响规律研究[J]. 化工学报, 2024, 75(2): 566-574.
	Song S R, Liu H C, Mi X T, et al. Experimental investigation of droplet formation in coaxial microchannels with different geometries of inner channel[J]. CIESC Journal, 2024, 75(2): 566-574.
[23]	Yao C Q, Zhao Y C, Ma H Y, et al. Two-phase flow and mass transfer in microchannels: a review from local mechanism to global models[J]. Chemical Engineering Science, 2021, 229: 116017.
[24]	Chen G W, Yue J, Yuan Q. Gas-liquid microreaction technology: recent developments and future challenges[J]. Chinese Journal of Chemical Engineering, 2008, 16(5): 663-669.
[25]	Kashid M N, Renken A, Kiwi-Minsker L. Gas-liquid and liquid-liquid mass transfer in microstructured reactors[J]. Chemical Engineering Science, 2011, 66(17): 3876-3897.
[26]	Chu C Y, Zhang F B, Zhu C Y, et al. Mass transfer characteristics of CO₂ absorption into 1-butyl-3-methylimidazolium tetrafluoroborate aqueous solution in microchannel[J]. International Journal of Heat and Mass Transfer, 2019, 128: 1064-1071.
[27]	Xu Z B, Wang T T, Wu J M, et al. Mass transfer characteristics of CO₂ and blended aqueous solutions of [C₂OHmim] [Lys]/MDEA in a microchannel[J]. Industrial & Engineering Chemistry Research, 2023, 62(22): 8926-8938.
[28]	Guo R W, Zhu C Y, Yin Y R, et al. Mass transfer characteristics of CO₂ absorption into 2-amino-2-methyl-1-propanol non-aqueous solution in a microchannel[J]. Journal of Industrial and Engineering Chemistry, 2019, 75: 194-201.
[29]	Shaterabadi F, Rashidi H. Experimental and modeling study of CO₂ capture by phase change blend of triethylenetetramine-ethanol solvent[J]. Energy, 2024, 307: 132809.
[30]	Ye J X, Jiang C K, Chen H, et al. Novel biphasic solvent with tunable phase separation for CO₂ capture: role of water content in mechanism, kinetics, and energy penalty[J]. Environmental Science & Technology, 2019, 53(8): 4470-4479.
[31]	Yao C Q, Dong Z Y, Zhao Y C, et al. An online method to measure mass transfer of slug flow in a microchannel[J]. Chemical Engineering Science, 2014, 112: 15-24.
[32]	Yao C Q, Zhao Y C, Ye C B, et al. Characteristics of slug flow with inertial effects in a rectangular microchannel[J]. Chemical Engineering Science, 2013, 95: 246-256.
[33]	尧超群, 陈光文, 袁权. 微通道内气-液两相传质过程行为及其应用[J]. 化工学报, 2019, 70(10): 3635-3644.
	Yao C Q, Chen G W, Yuan Q. Mass transfer characteristics of gas-liquid two-phase flow in microchannels and applications[J]. CIESC Journal, 2019, 70(10): 3635-3644.
[34]	Yao C Q, Zhao Y C, Zheng J, et al. The effect of liquid viscosity and modeling of mass transfer in gas-liquid slug flow in a rectangular microchannel[J]. AIChE Journal, 2020, 66(5): e16934.
[35]	Powell R E, Roseveare W E, Eyring H. Diffusion, thermal conductivity, and viscous flow of liquids[J]. Industrial & Engineering Chemistry, 1941, 33(4): 430-435.
[36]	Yin Y R, Fu T T, Zhu C Y, et al. Dynamics and mass transfer characteristics of CO₂ absorption into MEA/[Bmim] [BF₄] aqueous solutions in a microchannel[J]. Separation and Purification Technology, 2019, 210: 541-552.
[37]	Kies F K, Benadda B, Otterbein M. Experimental study on mass transfer of a co-current gas-liquid contactor performing under high gas velocities[J]. Chemical Engineering and Processing: Process Intensification, 2004, 43(11): 1389-1395.
[38]	Yue J, Chen G W, Yuan Q, et al. Hydrodynamics and mass transfer characteristics in gas-liquid flow through a rectangular microchannel[J]. Chemical Engineering Science, 2007, 62(7): 2096-2108.
[39]	Li C F, Zhu C Y, Ma Y G, et al. Experimental study on volumetric mass transfer coefficient of CO₂ absorption into MEA aqueous solution in a rectangular microchannel reactor[J]. International Journal of Heat and Mass Transfer, 2014, 78: 1055-1059.

Mass transfer study of CO₂ absorption by TETA/DEEA biphasic absorbent in the microchannel

微通道内两相吸收剂TETA/DEEA吸收CO₂过程的传质研究

RichHTML

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 14

References 39

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	Wei SU, Dahai ZHAO, Xu JIN, Zhongyan LIU, Jing LI, Xiaosong ZHANG. Delaying condensation frosting using biphilic surfaces coupled with spatial control of liquid desiccant [J]. CIESC Journal, 2025, 76(S1): 140-151.
[2]	Qingtai CAO, Songyuan GUO, Jianqiang LI, Zan JIANG, Bin WANG, Rui ZHUAN, Jingyi WU, Guang YANG. Numerical study on influence of perforated plate on retention performance of liquid oxygen tank under negative gravity [J]. CIESC Journal, 2025, 76(S1): 217-229.
[3]	Ting HE, Shuyang HUANG, Kun HUANG, Liqiong CHEN. Research on the coupled process of natural gas chemical absorption decarbonization and high temperature heat pump based on waste heat utilization [J]. CIESC Journal, 2025, 76(S1): 297-308.
[4]	Aihua MA, Shuai ZHAO, Lin WANG, Minghui CHANG. Research on dynamic simulation methods for solar-powered absorption refrigeration cycles [J]. CIESC Journal, 2025, 76(S1): 318-325.
[5]	Congqi HUANG, Shuangquan SHAO. Research on characteristics of compression-absorption refrigeration system driven by waste heat in liquid-cooled data center [J]. CIESC Journal, 2025, 76(S1): 326-335.
[6]	Haolei DUAN, Haoyuan CHEN, Kunfeng LIANG, Lin WANG, Bin CHEN, Yong CAO, Chenguang ZHANG, Shuopeng LI, Dengyu ZHU, Yaru HE, Dapeng YANG. Performance analysis and comprehensive evaluation of thermal management system schemes with low GWP refrigerants [J]. CIESC Journal, 2025, 76(S1): 54-61.
[7]	Xianchao REN, Yaxiu GU, Shaobin DUAN, Wenzhu JIA, Hanlin LI. Experimental study on heat and mass transfer performance of elliptical tube-fin evaporative condenser [J]. CIESC Journal, 2025, 76(S1): 75-83.
[8]	Changqiu HE, Jiameng TIAN, Yiqi CHEN, Yuchen ZHU, Xin LIU, Hai WANG, Zhentao WANG, Junfeng WANG, Zhifu ZHOU, Bin CHEN. Synergistic heat transfer enhancement characteristics due to electric field and macro-structured surface during thin film boiling [J]. CIESC Journal, 2025, 76(6): 2589-2602.
[9]	Ruijie MA, Zixuan HUANG, Xueqian GUAN, Guangjin CHEN, Bei LIU. Efficient ethane and methane separation using ZIF-8/DMPU slurry [J]. CIESC Journal, 2025, 76(5): 2262-2269.
[10]	Guanglei WANG, Xiaoling LIU, Zhen XU, Lin LI. Performances of gas-water direct contact heat exchange for compressed air energy storage [J]. CIESC Journal, 2025, 76(4): 1595-1603.
[11]	Feng ZHU, Yue ZHAO, Fengxiang MA, Wei LIU. Adsorption properties of modified UIO-66 for SF₆/N₂ gas mixture and its decomposition products [J]. CIESC Journal, 2025, 76(4): 1604-1616.
[12]	Luochang WU, Zeyu YANG, Jianguo YAN, Xutao ZHU, Yang CHEN, Zichen WANG. Experimental study on convection heat transfer characteristics of supercritical carbon dioxide flowing in mini square channels [J]. CIESC Journal, 2025, 76(4): 1583-1594.
[13]	Shaoyang MA, Hanzhuo XU, Liangliang ZHANG, Baochang SUN, Haikui ZOU, Yong LUO, Guangwen CHU. Research progress of liquid-liquid heterogeneous reactions and intensification methods towards their transfer processes [J]. CIESC Journal, 2025, 76(4): 1391-1403.
[14]	Yihao JIN, Junxin LUO, Zhangmao HU, Wei WANG, Qian YIN. Experimental investigation on hydrophilic functionalized MgSO₄/expanded vermiculite composites for water adsorption and heat storage [J]. CIESC Journal, 2025, 76(4): 1852-1862.
[15]	Ke QI, Di WANG, Zhe XIE, Dongsheng CHEN, Yunlong ZHOU, Lingfang SUN. Research on transient characteristics of solid oxide fuel cells considering coupling features of multiphysics fields [J]. CIESC Journal, 2025, 76(3): 1264-1274.