ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2019
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IF 7.149
Lidong Wang,Shanshan Liu,Rujie Wang,Qiangwei Li,Shihan Zhang
Biphasic solvents containing mixed amines have a phase separation behavior and energy-efficient regeneration for CO2 capture. However, the trade-off between the CO2 absorption capacity and the volume ratio of the CO2-rich phase presents a critical challenge to the reducing potential in regeneration energy consumption. In this study, sulfolane was proposed to regulate the phase separation behavior of a N,N-diethylethanolamine (DEEA)–triethylenetetramine (TETA) biphasic absorbent by simultaneously decreasing the volume ratio and increasing the CO2 loading of the rich phase, without sacrificing the high CO2 capacity. In the DEEA–TETA–sulfolane biphasic absorbent, sulfolane acted as a phase splitter and physical activator. The replacement of a part of H2O by hydrophobic sulfolane contributed to a substantial decrease in the volume ratio of the rich phase from 83 to 39% and an increase in CO2 loading of the rich phase from 3.10 to 4.92 mol/L. The regeneration heat decreased to 1.81 GJ/t CO2, 26.4% less than DEEA–TETA, and 54.6% less than the 5 M monoethanolamine system. Moreover, by promoting the mass transfer coefficient of CO2 in DEEA–TETA–sulfolane to 1.8 times the original DEEA–TETA system, sulfolane was validated as a physical activator. Our study provides a promising strategy for regulating the phase separation behavior of biphasic solvents and enhancing the regeneration energy efficiency for CO2 capture.
研究领域:
化学工程
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碳捕集与封存
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分离科学
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能源效率
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Yiming Zhao,Yongchun Zhang,Qi Liu,Xinwen Guo,Yang Cao,Nan Xu,Tianqinji Qi,Yongbo Chen,Shaoyun Chen
Water vapor contained in industrial waste gas will be accumulated in non-aqueous amine solvents when used for CO 2 capture and subsequently affect capture efficiency. While Piperazine (PZ) could be considered as an activator of the solution. Hence the effect of different contents of water and PZ added into the non-aqueous amine solvents on the CO 2 capture performance has been investigated. 13 C NMR has been used to identify the compounds present in aqueous CO 2 -rich amine solvents to characterize the mechanism of reactions. The energy consumption using 2-(ethylamino)ethanol (EMEA) water-lean amine solvent and aqueous monoethanolamine (MEA) solution was tested and compared on lab-scale, and further a comprehensive evaluation in a bench-scale pilot plant has been performed; It was found that the regeneration efficiency of the solution was reduced by approximately 10% when the water content was 10 wt%. The addition of PZ can recover the regeneration efficiency of the solvent to 94.2%. And its energy consumption was reduced by about 45% compared to the aqueous MEA solution in a 72-hour continuous absorption-desorption experiment. The results demonstrated that the aqueous PZ solution could improve the regeneration efficiency by involving in the proton transfer process. This work has proven that the blend of water-lean amine solvent and PZ is a novel, energy-efficient absorbent for CO 2 capture.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Yanan Yu,Yao Shen,Ke Wang,Jingkai Zhao,Jiexu Ye,Lidong Wang,Shihan Zhang
Amine-based technology is promising for CO 2 capture from the flue gas . However, it encounters high energy penalty and thus hampers its industrial application. Currently, the catalytic solvent regeneration is developing to lower down regeneration temperature, accelerate regeneration rate, and cut down energy consumption for monoethanolamine (MEA)-based process. However, the information on catalytic regeneration of biphasic solvent is seldom available. This work develops a facile synthesized robust catalyst, α-Fe 2 O 3, to promote the biphasic solvent regeneration such as triethylenetetramine (TETA) and 2-(diethylamino) ethanol (DEEA) blend. Experimental results revealed that, with the aid of α-Fe 2 O 3 , the efficient regeneration of TETA-DEEA occurred at 94 °C, which is far below the conventional MEA-based process (110–120 °C). The corresponding CO 2 stripping rate increased by 2.4 times compared with uncatalytic scenario. Furthermore, the relative energy consumption was furtherly decreased by 41.6%. Different from MEA regeneration, the biphasic solvent regeneration with α-Fe 2 O 3 depended on the enhancement of water molecules proton donation rather than the abundant Brønsted acid and Lewis acid of the catalyst. Based on DFT calculation and 13 C NMR spectra analysis, the water molecules on α-Fe 2 O 3 surface and the protonated DEEA were parallel served as proton donors for carbamate decomposition. Consequently, a novel proton transfer mechanism was proposed for the biphasic solvent TETA-DEEA regeneration. The water molecules adsorbed on α-Fe 2 O 3 surface generated oxyhydrogen groups and thus donate protons for the carbamate decomposition. This work proposes a novel proton transfer mechanism for solvent regeneration and advances its industrial application with a low energy penalty.
研究领域:
环境科学
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化学工程
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催化
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能源技术
✓ 已验证
DOI
高影响因子
APPLIED ENERGY
·
2018
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IF 7.9
Fei Liu,Mengxiang Fang,Wenfeng Dong,Tao Wang,Zhixiang Xia,Qinhui Wang,Zhongyang Luo
Using biphasic solvents for carbon dioxide (CO 2 ) capture is regarded as a promising technology to drastically reduce the regeneration energy. However, this technology hasn’t been put into commercial application due to lack of the biphasic solvents with high stabilities and low costs. To overcome this challenge, we developed a novel type of biphasic solvent based on alkanolamine-alkanolamine blends, i.e., aqueous blends of 2-(diethylamino)-ethanol (DEEA, 50 wt%) and monoethanolamine (MEA, 25 wt%) or 2-((2-aminoethyl) amino) ethanol (AEEA, 25 wt%). The aqueous DEEA-AEEA solvent demonstrated a cyclic capacity as high as 0.64 mol CO 2 /mol which is significantly higher than those of 30 wt% MEA and other reported biphasic solvents. In addition, a phase split time as short as a few minutes is obtained. The phase split dynamics were analyzed to investigate the effects of CO 2 loading, temperature, gas flow rate and height-to-diameter ratio. Quantitative 13 C NMR analysis was then performed to reveal the reaction and phase split mechanism of CO 2 absorption in the DEEA-AEEA solvent. It indicated that the reaction of AEEA with CO 2 dominated at the beginning of CO 2 absorption and the products are formed as carbamates. Then, DEEA began reacting with CO 2 to yield bicarbonate and carbonate. The phase split mechanism indicated that the reaction products of carbamates and HCO 3 − /CO 3 2− migrated to the lower phase while DEEA and unreacted AEEA migrated to the upper phase. Finally, the cyclic tests were repeated and the energy consumption was evaluated. The regeneration energy of the biphasic solvent, without process optimizations, is 2.58 GJ/tCO 2 , which is 32% lower than that of the traditional 30 wt% MEA solvent.
研究领域:
化学工程
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环境科学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
Scientific Reports
·
2024
·Vol. 14
·期 1
·1-16
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IF 3.8
Wang Qian,Gong Dehong,Zhang Zhongxiao,Zhu Jiangdong,Luo Qingling
The high energy consumption of Carbon Capture Utilization and Storage(CCUS) promotes the research of integrated absorption and mineralization technology. A novel DEEA/AEP biphasic absorbent is used to absorb \(\hbox {CO}_{2}\) . After phase separation, only one phase enriched with the absorption product is sent into the mineralization system, then reacts with \(\hbox {Ca(OH)}_{2}\) to produce \(\hbox {CaCO}_{3}\) at normal temperature and pressure. The effects of temperature, Ca/C and dispersion of the system were investigated, and cyclic utilization experiment was also conducted. The process was characterized and analyzed by Thermal gravimetric analysis (TGA), X-ray diffraction (XRD), and nuclear magnetic resonance ( 13 C NMR). The results showed that at 50 \(^{\circ }\) C, Ca/C = 1, the extent of mineralization of \(\hbox {CO}_{2}\) -enriched phase mineralization was 95.73% after ultrasonic treatment for 30 min. During 6 cycles, the volume percentage of \(\hbox {CO}_{2}\) -enriched phase could be maintained at 52–55%, and the \(\hbox {CO}_{2}\) load was 11.92mol/L. The results above indicate that the \(\hbox {CO}_{2}\) -enriched phase mineralization technology after absorption by biphasic absorbent can effectively capture \(\hbox {CO}_{2}\) , realize recycling, and reduce CCUS energy consumption.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Zehui Shang,Chunying Zhu,Taotao Fu,Youguang Ma
A liquid-liquid AEP/DEEA/n-butanol/H 2 O absorbent is developed. • Multi-variable optimization of absorption and desorption is performed. • NMR reveals carbamate and bicarbonate/carbonate absorption pathways. • Desorption energy AEP/DEEA/n-butanol/H 2 O is 66% of that of 30 wt% MEA/H 2 O. High regeneration energy remains a major obstacle to the practical application of alkanolamine-based absorbents for CO 2 capture. To reduce the regeneration energy demand, a liquid-liquid phase-change absorbent composed of polyamine 1-(2-aminoethyl)piperazine (AEP), 2-(diethylamino)ethanol (DEEA), n-butanol and H 2 O was developed. The effects of composition and operating conditions on the absorption–desorption performance were systematically investigated, identifying 1.8:1.2 AEP/DEEA, 4:3 n-butanol/H 2 O, 30 wt% total amine, and 303.15 K as suitable microchannel absorption conditions. 13 C and 1 H NMR analyses showed that AEP mainly absorbed CO 2 via the carbamate pathway, whereas the tertiary amine site of AEP and DEEA mainly promoted CO 2 hydration to form HCO 3 − /CO 3 2− . Under the optimal composition of 18 wt% AEP, 12 wt% DEEA, 40 wt% n-butanol, and 30 wt% H 2 O, the volume fraction and CO 2 loading of the rich phase reached 48.68% and 3.42 mol CO 2 ·kg −1 solution, respectively. Under desorption at 363.15 K with 2 mL lean-phase addition for 60 min, the desorption efficiency and cyclic capacity reached 58.91% and 1.95 mol CO 2 ·kg −1 solution, respectively, while the apparent desorption energy consumption was only 66% of that of 30 wt% MEA. Overall, this phase-change absorbent achieved effective synergy among rapid absorption, reversible regeneration, and phase-separation intensification, demonstrating its potential for low-energy CO 2 capture.
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DOI
高影响因子
Nano Research
·
2021
·Vol. 15
·期 1
·510-518
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IF 8.897
Wu Jia-Si,Li Jia-Xian,Shu Na,Duan Qi-Jia,Tong Qi-Song,Zhang Jing-Yang,Huang Yong-Cong,Yang Si-Yu,Zhao Zhi-Bin,Du Jin-Zhi
Tumor associated macrophages (TAMs) tend to exhibit tumor-promoting M2 phenotype and contribute to the development of immunosuppressive microenvironment of solid tumors. Reprograming TAMs from M2 into tumoricidal M1 phenotype is robust for stimulating tumor immunosuppressive microenvironment (TIME). In this study, we developed a poly(amidoamine) (PAMAM) derivative dendrimer (denoted as fourth generation- N,N -diethylaminoethyl (G4-DEEA)) for efficient loading of Toll-like receptor 7 and 8 (TLR7/8) agonist (R848) to remodel the TIME for potent cancer immunotherapy. G4-DEEA exhibited a high loading capacity of R848 up to 35.9 wt% by taking advantage of its dendritic structure. The resulting formulation (designated as G4-DEEA@R848) effectively polarized M2 macrophages into M1 phenotype in vitro , and improved the maturation and activation of antigen-presenting cells. In the 4T1 orthotopic breast cancer model, G4-DEEA@R848 showed a stronger tumor inhibitory effect than free drug. The mechanistic studies suggested that G4-DEEA@R848 could significantly stimulate the TIME by repolarizing TAMs into M1 phenotype, reducing the presence of immunosuppressive myeloid cells and increasing the infiltration of tumor cytotoxic T cells. This study provides a simple but effective dendrimer-based strategy to improve the formulation of R848 for improved cancer immunotherapy.
研究领域:
癌症免疫治疗
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药学
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免疫学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Tianzi Liu,Jialuo Xiang,Ding Wei,Yangqiang Huang,Hao Chen,Xiao Luo
This study comprehensively reports the physical and chemical equilibrium solubility data, along with a detailed chemical equilibrium analysis, of carbon dioxide (CO2) absorption into a blended amine solution consisting of 2-methylaminoethanol (MAE) and N,N-diethylethanolamine (DEEA). Four models were employed to analyze the CO2 physical solubility using N2O analogy, with the Artificial Neural Network (ANN) model exhibiting an average absolute relative deviation (AARD) of 2.78%. The CO2 chemical solubilities were then analyzed experimentally at various temperatures (298–313 K), CO2 partial pressures (8–100 kPa), and concentrations (1–5 mol/L). In addition, the heat of CO2 absorption was estimated to be 46.96 kJ/mol using the Gibbs–Helmholtz equation, which is approximately half that of the benchmark amine, monoethanolamine (MEA). A rigorous 13C NMR investigation was conducted to identify and quantify the species formed during the absorption process across varying temperatures, CO2 loadings, and MAE/DEEA molar ratios, to clarify the capture mechanisms and intricate role of MAE and DEEA in the capture process. As a result, at an MAE/DEEA ratio of 1:4, the carbamate concentration peaks at a CO2 load of about 0.45 mol of CO2 /mol of amine at about 0.6 mol/L, which is only one-third of the concentration at the higher ratio, which contributes to the reduction of energy consumption for CO2 desorption.
研究领域:
化学工程
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碳捕集与封存（CCS）
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热力学
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气体溶解度
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反应机理
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）