CHEMICAL ENGINEERING SCIENCE
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2024
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IF 4.1
Longyun Zheng,Zhangyu Guo,Hui Liu,Kai Guo,Chunjiang Liu
CO 2 absorption into amine solutions is an important method for reducing carbon emissions. The influence mechanism of chemical reactions on the bubble behavior and mass transfer needs to be comprehensively investigated. In this study, firstly, we measure the bubble behavior and mass transfer of single CO 2 bubbles freely rising in monoethanolamine (MEA)/ N , N -diethylethanolamine (DEEA) blended solutions and DEEA solutions by high-speed photography. Moreover, we investigate the effect of amine concentration on the bubble shape, aspect ratio, rising trajectory, rising velocity, and mass transfer coefficient. The results show that CO 2 bubbles in MEA/DEEA blended solutions experience significant shape deformation, oscillation damping, surface contamination, and mass transfer deterioration. In contrast, CO 2 bubbles in DEEA solutions behave similarly to those in ultrapure water, i.e. negligible surface contamination and mass transfer enhancement. Furthermore, we consider the differences in the bubble behavior and mass transfer from the viewpoint of the chemical reaction kinetics and bubble surface contamination degree. The location where a chemical reaction occurs is close to the bubble surface with a fast reaction, and as a result, the bubble surface is likely to be contaminated. Finally, this study provides insights into the intensification of amine-based CO 2 chemical absorption processes.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
Greenhouse Gases-Science and Technology
·
2019
·Vol. 9
·期 3
·553-566
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IF 1.693
Menglong Liu,Siyang Tang,Kui Ma,Changjun Liu,Hairong Yue,Bin Liang
Monoethanolamine (MEA) solution has been used widely in the post-combustion CO 2 capture process; however, the high heat duty and reaction temperature (e.g. 125°C) for MEA regeneration leads to a high energy requirement (nearly 70–80% of the total running cost). We report the use of solid particles (H-Zeolite Socony Mobile-5 (HZSM-5), quartz, and activated carbon) to facilitate the mass transfer of CO 2 bubble nucleation and enhance the CO 2 desorption rate. The results show that the mass transfer of CO 2 from liquid phase to gas phase is the rate-determining step, rather than the chemical reaction. The addition of HZSM-5 particles in the solution significantly enhanced CO 2 bubble nucleation by providing nucleation sites and gas cavities, leading to an average CO 2 desorption rate enhancement of 43.2%, and an energy consumption reduction of 23.3%. This process also operated at ∼95°C, which is a much lower temperature than that used in the commercial process and is feasible for industrial applications. © 2019 Society of Chemical Industry and John Wiley & Sons, Ltd.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2018
·
IF 3.927
Yaran Yin,Taotao Fu,Chunying Zhu,Rongwei Guo,Youguang Ma,Huaizhi Li
The evolution of the size and velocity of CO 2 bubble absorbed into MEA/[Bmim][BF 4 ] aqueous solutions was in-line investigated by a high-speed camera. The coupling effect between the variation of volume and the velocity of bubbles was highlighted. According to the evolution of average mass transfer coefficient, the mass transfer performance in the whole flow process was studied. The results indicated that both the length and velocity of bubble decreased gradually in the flow process due to mass transfer. A linear correlation between the relative velocity (the ratio of average bubble velocity to two-phase superficial velocity) and the relative lost length (the ratio of the lost length to the initial length) was proposed. The increase in overall liquid-phase volumetric mass transfer coefficient ( k L a ) at higher gas flow rate could be ascribed to the shorter residence time and larger specific surface area. While the increase of k L a at higher liquid flow rate and MEA or [Bmim][BF 4 ] concentration was resulted from intensified mass transfer. An empirical correlation of overall liquid-phase volumetric mass transfer coefficient was proposed taking the gas-phase Reynolds number, liquid-phase Reynolds number and Damköhler number into account.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2019
·
IF 5.107
Hao Ling,Sen Liu,Hongxia Gao,Haiyan Zhang,Zhiwu Liang
In order to establish an integrative mass transfer coefficient (K G a V ) model for CO 2 absorption into blended monoethanolamine (MEA)/1-dimethylamino-2-propanol (1DMA2P) solution in packed column, the models of CO 2 Henry’s law constants (He CO₂-MEA/1DMA2P ) and the equilibrium CO 2 solubility (α eq ) were constructed. The experimental produced data can be reasonably analyzed. In this work, the Arrhenius equation was employed to fit the values of He CO₂-MEA/1DMA2P at different temperature with AARD of 4.06%; the Kent-Eisenberg prediction model and empirical polynomial prediction model were used to predict the data of α eq under different CO 2 partial pressures and temperatures with AARDs of 2.64% and 0.83%, respectively; the empirical K G a V model proposed by Li, the empirical K G a V model proposed by Aroonwilas and new K G a V model were used to correlate the average values of K G a V with AARDs of 14.36%, 12.44% and 9.03%, respectively; the model for outlet CO 2 concentration (y CO₂,out ) in packed column was developed with AARD of 15.97%. Moreover, the heat of CO 2 absorption in 6 kmol/m 3 MEA/1DMA2P solution was estimated by Gibbs-Helmholtz equation which gave a value of −39.8 kJ/mol. The results show that the blended MEA/1DMA2P solution has advantages that make it a potential absorbent for CO 2 capture.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Lijian Jin,Xueyan Hou,Lingxiao Zhan,Shangzhi Xie,Lina Gu,Hangqi Yang,Xin Wang,Xinfeng Qian,Jianchong Shen,Linjun Yang
In order to ameliorate the issues of corrosion and high regeneration energy associated with traditional biphasic solvents, a nonaqueous biphasic solvent has been proposed as a potential alternative. This study introduces Tetramethylethylenediamine (TMEDA) as a phase splitter within the Ethanolamine (MEA)/Dimethyl sulfoxide (DMSO) system, resulting in a novel nonaqueous biphasic solvent, TMEDA/MEA/DMSO. Compared with other screened phase splitters, the appropriate polar size and intermolecular interaction force of TMEDA are the key factors that make it comply with the screening of nonaqueous biphasic solvent. When the mass ratio of TMEDA/MEA/DMSO is maintained at 3:3:4, the CO 2 loading attains 0.54 mol (CO 2 )/mol (MEA), with the rich phase comprising 75 % of the total. 13 C NMR and FT-IR characteristics showed that the absorbent product is mainly in the form of MEACOO − /MEAH + . Absorption and phase separation mechanisms of absorbent elucidated by DFT calculations and molecular dynamics simulations. The limited opportunity for TMEDA to interact with MEA molecules emerges as the primary reason for its reduced involvement in the reaction, with the inclusion of TMEDA intensifying the aggregation of MEACOO − /MEAH + and triggering phase transition. In comparison to a 30 wt% MEA water-based absorbent, TMEDA/MEA/DMSO exhibits a 40 % reduction in regeneration energy (estimate) and possesses energy-saving attributes, rendering it a promising candidate for CO 2 capture.
研究领域:
化学工程
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环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF CHEMICAL THERMODYNAMICS
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2025
·
IF 2.2
Lijiao Ma,Yudong Ding,Yi Zhang,Xun Zhu,Hong Wang,Min Cheng,Qiang Liao
To reduce CO 2 emissions and address issues with conventional amine-based aqueous absorbents, a mixed nonaqueous solution of monoethanolamine (MEA) and N , N -dimethylformamide (DMF) was proposed. The density, dynamic viscosity and refractive index of fresh MEA-DMF solutions (10-50 wt% MEA) and CO 2 -loaded solutions (0.10–0.51 mol CO 2 ·(mol MEA) −1 ) were measured across the temperature range of 298.15–333.15 K. The values for fresh solutions were correlated with concentration and temperature using the Jouyban-Acree model (JAM) and an exponential equation. Then the results after CO 2 absorption were derived from the CO 2 loading amount. Additionally, CO 2 absorption performance of MEA-DMF with various concentrations at 303.15–333.15 K and 9.64–134.52 kPa was assessed to determine gas-liquid equilibrium and develop semi-empirical correlations. Nuclear magnetic resonance (NMR) analysis confirmed that carbamate was the primary product formed after CO 2 absorption in the nonaqueous absorbent. These studies provide essential data for equipment design and absorbent optimization. MEA-DMF solutions demonstrate favorable viscosity and CO 2 absorption performance, supporting the potential use of nonaqueous absorbents in industrial CO 2 capture technologies.
研究领域:
化学工程
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环境科学
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物理化学
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材料科学
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产品关联
DOI
高影响因子
ENERGY & FUELS
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2017
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IF 3.091
Hongxia Gao,Zeyang Wu,Helei Liu,Xiao Luo,Zhiwu Liang
The absorption/desorption performance of carbon dioxide (CO2) in aqueous 5 M monoethanolamine (MEA) solutions in the presence of various solution regeneration promoters was comprehensively investigated using a multiple rapid screening method. The promoters considered were N-methyldiethanolamine (MDEA), N,N-dimethylethanolamine (DMEA), N,N-diethylethanolamine (DEEA), 1-dimethylamino-2-propanol (1DMA2P), 1-diethylamino-2-propanol (1DEA2P), 3-dimethylamino-1-propanol (3DMA1P), 2-(dimethylamino)-2-methyl-1-propanol (2DMA2M1P), triethanolamine (TEA), 3-(dimethylamino)-1,2-propanediol (3DMA-1,2-PD), and 3-(diethylamino)-1,2-propanediol (3DEA-1,2-PD). The molar concentration of these promoters added into 5 M MEA was set to 1 mol/L. At the atmospheric pressure, the absorption and stripping experiments were carried out at 313.15 and 353.15 K, respectively. Especially, the CO2 partial pressure was controlled at constant 15 kPa for absorption experiments. In addition, the equilibrium solubility of CO2 was also determined in order to evaluate the driving force of each amine system. The results showed that the highest CO2 equilibrium solubility of 0.5548 mol CO2/mol amine was obtained by MEA/1DEA2P, whereas both the fastest absorption and regeneration rates were achieved for aqueous blended MEA/1DMA2P solution which made MEA/1DMA2P to exhibit the highest CO2 cyclic capacity of 1.6710 mol CO2/L.
研究领域:
化学工程
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环境科学
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能源技术
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物理化学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2016
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IF 2.567
Rui Zhang,Xiao Luo,Qi Yang,Fan Cao,Shupanxiang Chen,Zhiwu Liang
This work has investigated CO2 absorption using 3-(diethylamino)propylamine (DEAPA), a diamine that contains one primary and one tertiary amine in the same molecule. The results are compared with those for the blended amine system of monoethanolamine and methyldiethanolamine (MEA–MDEA), a mixed amine solvent with an equal number of moles of primary and tertiary amine. The 2 M DEAPA, 2 M MEA, and 4 M MEA–MDEA (1:1 mole ratio) were tested for their CO2 absorption performance. The experimental results show that the intramolecular tertiary amino group of DEAPA can promote the CO2 absorption rate of the intramolecular primary amino group and enhance its CO2 absorption capacity. The results using 13C nuclear magnetic resonance also showed that the intermolecular tertiary amine in the MEA–MDEA system was more favored for the promotion of the primary amine in the blend to form bicarbonate at an earlier CO2 equivalent loading stage and produced less carbamate than the intramolecular tertiary amino group of DEAPA did with respect to its primary amine. Furthermore, the CO2 equilibrium solubility of DEAPA was measured at different temperatures with various CO2 partial pressures, and then an empirical model based on these experimental data was developed. The results predicted by this model were fitted well with the experimental results. The Gibbs–Helmholtz equation was used to estimate the CO2 absorption heat of the DEAPA system, and the results showed that DEAPA has a CO2 absorption heat (−36.4 kJ/mol) lower than those of MEA, MDEA, and DEA. The results demonstrate that DEAPA has the potential to be an alternative solvent with a high absorption rate, a high CO2 capacity, and a low heat of absorption in CO2 capture processes.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
Bin Zhao,Yujing Liu,Bo Zhou,Peidong Zuo,Liping Chang,Jiawei Zhong,Zhenyi Du,Mengmeng Wu,Zhifeng Qin
Understanding the structure-property-performance relationship of mixed amine solvents is essential for developing high-efficiency Carbonyl sulfur (COS) removal technologies. In this work, the thermophysical properties, intermolecular interactions, and COS capture performance of monoethanolamine (MEA) and N-methyldiethanolamine (MDEA) binary aqueous systems were systematically investigated. The density ( ρ ) and viscosity ( ν ) of MEA - MDEA mixtures were measured over a temperature range of 293.15–318.15 K with varying MDEA mole fractions. Key thermodynamic parameters, including viscosity deviation (Δ η ), excess molar volume ( V m E ), and excess Gibbs free energy of activation (Δ G *E ), were subsequently calculated. The results reveal that within an MDEA mole fraction range of 0.35–0.60, Δ η reaches a maximum while V m E remains negative, indicating stronger intermolecular attraction and denser molecular packing. Spectroscopic characterizations combined with quantum chemical calculations further confirm the formation of directional O—N–H hydrogen bonds between the hydroxyl groups of MDEA and the amino nitrogen of MEA, which stabilize the solvent microstructure. Based on these findings, COS absorption-desorption experiments were conducted. Notably, the mixed amine systems with MDEA mole fractions of 0.3852 and 0.5446 exhibited a significant synergistic effect, maintaining over 95 % COS removal efficiency throughout the 120 min absorption process, along with excellent regeneration performance characterized by higher and more stable desorption rates during the 60 min regeneration phase. This work establishes a clear structure-property-reaction correlation, providing valuable molecular-level insights for the rational design of efficient amine-based absorbents for industrial COS capture.
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产品关联
DOI
高影响因子
RSC Advances
·
2024
·Vol. 14
·期 5
·3146-3157
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IF 3.9
Yanlong Hu,Qiang Wang,Dingkai Hu,Yingshuang Zhang,Muhammad Furqan,Shijian Lu
Monoethanolamines (MEAs) are widely used for CO2 capture, but their regeneration energy consumption is very high. CO2 Phase change absorbents (CPCAs) can be converted into CO2-rich and CO2-lean phases after absorbing CO2, and the regeneration energy consumption can be reduced because only the CO2-rich phase is thermally desorbed. In this paper, a novel CPCA with the composition “MEA/n-butanol/H2O (MNBH)” is proposed. Compared with the reported MEA phase change absorbent, the MNBH absorbent has higher CO2 absorption capacity, smaller absorbent viscosity and CO2-rich phase volume. The MNBH absorbent has the highest CO2 absorption capacity of 2.5227 mol CO2 per mol amine at a mass ratio of 3 : 4 : 3. The CO2 desorption efficiency reaches 89.96% at 120 °C, and the CO2 regeneration energy consumption is 2.6 GJ tCO2−1, which is about 35% lower than that of the 30 wt% MEA absorbent. When the mass ratio of MNBH absorbent was 3 : 6 : 1, the CO2 recycling capacity was 4.1918 mol CO2 L−1, which is 76% higher than that of the conventional 30 wt% MEA absorbent. The phase change absorbent developed in this paper can reduce the desorbent volume by about 50% and has good absorption performance for CO2 in flue gas.
研究领域:
化学工程
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环境科学
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产品关联
DOI
PubMed
高影响因子
International Journal of Greenhouse Gas Control
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2019
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IF 3.231
Mimi Xu,Shujuan Wang,Lizhen Xu
21 pairs of physical-chemical biphasic solvents were screened out using a fast screening facility and the distribution of components was detected both in upper and lower phases after absorption. The physical solvents and amines were enriched in opposite phases due to the limited solubility of absorption products in the physical solvents, and the enrichment of components gets higher as the loading time goes by. Comparisons of the cyclic capacity showed that MEA and DETA were much better main solvents than BDA in biphasic solvents, and 2.5 DETA-4 sulfolane has the highest CO 2 cyclic capacity of 4.486 mol L −1 , which was much higher than that of 30 wt% MEA. The concentrations of physical solvents influence the cyclic capacity a lot rather than the types of physical solvents. Then the phase separation character and absorption performance were analyzed for solutions in different amine to physical solvent concentration ratios, and the results showed that increasing the concentration of the physical solvent within certain range benefits to raising cyclic absorption capacity and reducing the energy penalty. At last, the sensible heat and vaporization heat of two biphasic solvents were estimated with a flash module of Aspen Plus, which showed less energy penalty than that of 30 wt% MEA.
研究领域:
化学工程
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环境科学
✓ 已验证
DOI
高影响因子
AICHE JOURNAL
·
2018
·Vol. 64
·期 11
·3988-4001
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IF 3.326
Xiaowen Zhang,Jieling Hong,Helei Liu,Xiao Luo,Wilfred Olson,Paitoon Tontiwachwuthikul,Zhiwu Liang
In this work, the composite catalysts, SO 4 2 /ZrO 2 /γ-Al 2 O 3 (SZA), with different ZrO 2 and γ-Al 2 O 3 mass ratios were prepared and used for the first time for the carbon dioxide (CO 2 )-loaded monoethanolamine (MEA) solvent regeneration process to reduce the heat duty. The regeneration characteristics with five catalysts (three SZA catalysts and two parent catalysts) of a 5 M MEA solution with an initial CO 2 loading of 0.5 mol CO 2 /mol amine at 98°C were investigated in terms of CO 2 desorption performance and compared with those of a blank test. All the catalysts were characterized using X-ray diffraction, Fourier transform infrared spectroscopy, N 2 adsorption–desorption experiment, ammonia temperature programmed desorption, and pyridine-adsorption infrared spectroscopy. The results indicate that the SZA catalysts exhibited superior catalytic activity to the parent catalysts. A possible catalytic mechanism for the CO 2 desorption process over SZA catalyst was proposed. The results reveal that SZA1/1, which possesses the highest joint value of Brφnsted acid sites (BASs) and mesopore surface area (MSA), presented the highest catalytic performance, decreasing the heat duty by 36.9% as compared to the catalyst-free run. The SZA1/1 catalyst shows the best catalytic performance as compared with the reported catalyst for this purpose. Moreover, the SZA catalyst has advantages of low cost, good cyclic stability, easy regeneration and has no effect on the CO 2 absorption performance of MEA. © 2018 American Institute of Chemical Engineers AIChE J , 64: 3988–4001, 2018
研究领域:
化学工程
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催化材料
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环境科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）