SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xing Li,Lei Xing,Chunyu Zhang,Shudan He,Fanghua Liu,Zhen Chen,Huazhen Chang,Junhua Li
Catalytic solvent regeneration is widely considered a promising solution for addressing the intensive heat duty of amine-based carbon dioxide (CO 2 ) capture. This highly challenging application has motivated researchers to develop excellent catalysts with high activity and durability. In this study, we engineered active and durable Fe − N − C catalyst coated with high-graphitization carbon layers (labeled Phen − Fe − N − C) through a secondary thermal pyrolysis treatment. The multiple graphite layers and atomic metal sties were verified by experimental characterization and coordination structure analysis. The improved graphite layers further enhanced the activity of Fe − N − C sites, providing more acid sites for proton-electron transfer and C − N breaking during solvent regeneration (or CO 2 desorption). Thus, the maximal CO 2 desorption rate increased by 50 % when Fe − N − C was used compared with that of the blank case, and the rate further increased by 27 % when Phen − Fe − N − C was used. After 15 days of hydrothermal testing, the single Fe atom over the spent catalysts presented no significant aggregation or dissolution in the solvent, validating the durability of Phen − Fe − N − C. This work demonstrates a feasible and novel strategy to improve M − N − C materials for efficient and robust CO 2 desorption from amine solvents toward energy-saving CO 2 capture.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Zain Ali Saleh Bairq,Hongxia Gao,Fatima Abduh Mohammed Murshed,Paitoon Tontiwachwuthikul,Zhiwu Liang
In the CO2 capture process, decreasing the energy consumption and increasing the desorption rate of loaded MEA-CO2 during the regeneration process of monoethanol amine have been identified as major challenges that need to be addressed. To overcome these challenges, three modified heterogeneous mesoporous catalysts, CMK-3-SiO2, CMK-3-MCM-41, and CMK-3-SBA-15, and a SO42–/ZrO2 solid acid catalyst were initially synthesized and investigated to determine their catalytic effectiveness in the process of CO2 and MEA solvent regeneration with a CO2 loading of 0.5 ± 0.02 mol CO2/mol MEA at 97 °C. According to the experimental results, the CMK-3-modified catalyst significantly decreased the energy requirement for CO2 desorption. The catalytic performance of the synthesized catalysts was in the order of CMK-3-SiO2 > CMK-3-MCM-41 > CMK-3-SBA-15 > SZ. CMK-3-SiO2 exhibited the best catalytic performance by enhancing the desorption rate by 195%, and decreasing the energy requirement by 37.41% compared to monoethanol amine as a blank run. Furthermore, the CMK-3-SiO2 catalyst exhibited the best catalytic performance compared to the literature with excellent stability and no unfavorable effects on the MEA-CO2 absorption activity for the regenerated amine solvent. This performance seems to be a result of the large mesoporous surface area (BET) and the large number of Brϕnsted and Lewis acid sites. In addition, a reasonable reaction mechanism for amine solvent regeneration with the CMK-3 heterogeneous catalyst is proposed.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2019
·
IF 3.021
Chenxu Li,Xiaoqin Shi,Shufeng Shen
Solvent-based absorption using aqueous monoethanolamine (MEA) is the most mature and commercially available carbon dioxide capture technique. However, high capital cost and large energy consumption required for solvent regeneration still remain major disadvantages, which results in delaying the worldwide large-scale deployment of this technology. Several newly developed absorbents have been recently proposed to solve the main issue for the energy-efficient capture process. In this work, several advanced solvents, i.e., aqueous and water-lean amino acid salts (potassium lysinate, potassium prolinate, or potassium sarcosinate) and blends of amines with glycol ethers, were selected as the representatives for aqueous, non-aqueous, and phase-change systems. The CO2 absorption–desorption performance of these absorbents was characterized. The relative heat duty of those CO2-loaded absorbents was also evaluated and compared to conventional aqueous 30 mass % MEA. Preliminary results indicate that non-aqueous and phase-change absorbents investigated in this work have huge potential in reducing energy consumption of regeneration, at about 40–60% reduction.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2018
·
IF 3.927
Hao Ling,Sen Liu,Hongxia Gao,Zhiwu Liang
In order to study the effect of heat-stable salts (HSSs) on the CO 2 absorption performance of amine solution, the CO 2 absorption/desorption rates and cyclic CO 2 capacity of 30 wt% (monoethanolamine) MEA solutions in the presence of various acidic degradation products were comprehensively investigated systematically by an improved rate-based screening method. In addition, the initial pH values and CO 2 equilibrium solubility were also evaluated. These acidic degradation products considered were formic acid , acetic acid, propionic acid , butyric acid , glycolic acid, oxalic acid , lactic acid, malonic acid and bicine. The experimental results indicated that the carboxylic acids with different chemical structures can reduce the initial pH values, equilibrium solubility of CO 2 , absorption rate and cyclic CO 2 solubility, but promote the CO 2 desorption rate of aqueous MEA solution. Furthermore, a countermeasure was proposed to maintain absorption performance and reduce the energy requirement of solvent regeneration for an MEA amine-treating unit. The obtained results can provide a guidance for developing corresponding countermeasure for heat-stable salts control and removal in the CO 2 absorption-stripping process using amine solutions.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chaowu Wang,Qibo Zhang
Efficiently recovering critical metals from secondary resources is crucial to decreasing the environmental impact of mineral-resource mining and reducing production costs and process energy consumption. Herein, we propose a simple and comprehensive approach to recycle Co 3 O 4 from waste choline chloride/ethylene glycol (named Ethaline) electrolyte containing Co(II) ions along with solvent regeneration. Through the rational coordination adjustment using water, [CoCl 4 ] 2− complex in the Ethaline-based electrolyte is transformed to [CoCl 2 (H 2 O) 4 ] 0 and [CoCl 2 (H 2 O) 5 ] + to facilitate precipitation separation. Adding oxalic acid (OA) as a precipitator can reach 97.1% cobalt recovery efficiency with a high value-added Co 3 O 4 rod-like structure obtained by calcining the oxalate precipitate. In addition, the water-containing solvent can be regenerated via reduced pressure distillation with a high recovery efficiency of up to 98.0%. FT-IR and 1 H NMR characterizations verify that the regenerated Ethaline exhibits good structural stability. Impressively, the proposed recovery path shows high recovery efficiencies for both cobalt and Ethaline in various practical Co(II) ion-containing electrolytes. This study establishes a novel technical pathway for the resource utilization of metal-bearing waste Ethaline electrolytes, which shows an excellent prospect in solvent recycling after metal processing.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ENERGY
·
2019
·
IF 8.426
Zain Ali Saleh Bairq,Hongxia Gao,Yufei Huang,Haiyan Zhang,Zhiwu Liang
A significant impediment to the widespread adoption of amine-based post-combustion technique for CO 2 capture from flue gas is the huge energy demand for amine solvent regeneration. In this study, five novel bifunctional heterogeneous catalysts e.g., SO 4 2− /ZrO 2 /SiO 2 with different molar ratios of zirconia and SO 4 2− /ZrO 2 as a parent catalyst were synthesized and applied to evaluate their effectiveness in enhancing the CO 2 desorption and solvent regeneration of 5M monoethanolamine solution with CO 2 loading of 0.5 ± 0.01 mol CO 2 /mol monoethanolamine at 97 °C. The catalysts were characterized by Fourier transform-infrared spectrometry, pyridine-infrared spectroscopy, X-ray diffraction, N 2 -adsorption-desorption, and ammonia-temperature programmed desorption. The results demonstrated that these catalysts can significantly reduce the heat duty for CO 2 desorption by 36.48% compared to without catalyst and enhance desorption rate by 35.1%. The results also showed that SO 4 2− /ZrO 2 /SiO 2 15% presented the highest efficiency compared to the other SO 4 2− /ZrO 2 /SiO 2 ratios and the super solid acid catalyst SO 4 2− /ZrO 2 . Additionally, to investigate if the catalysts induce any unfavorable effects on the amine, the absorption of CO 2 by regenerated amine solvent was studied. Finally, a reaction mechanism for the amine solvent regeneration with the synthesized catalyst e.g., SO 4 2− /ZrO 2 /SiO 2 was suggested.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
APPLIED ENERGY
·
2017
·
IF 7.182
Tao Wang,Wei Yu,Yann Le Moullec,Fei Liu,Yili Xiong,Hui He,Jiahui Lu,Emily Hsu,Mengxiang Fang,Zhongyang Luo
Using an inert, immiscible organic component as the purging gas is an innovative technology in the CO 2 stripping process. It allows stripping at a lower temperature and overcomes the inherent problem of high energy consumption in steam-based CO 2 stripping processes. This work focused on developing a novel, direct non-aqueous gas stripping process and exploiting its potential for energy saving through experiments. An elaborate pre-screening of carrier gases was conducted through hydrocarbon, alcohols, aldehydes, ketones, and their isomers, etc. Pentane, hexane, and cyclohexane were selected as the carrier candidates for their good immiscibility with water/amine, low vaporization energy, mild condensation conditions, and low toxicity. The effects of carrier gas category, carrier gas flow rate , and rich solvent feeding temperature on the stripping performance were investigated. Pentane was found to be the superior carrier gas due to its low heat of vaporization, high regeneration rate, and low energy requirement. A unique phenomenon of water evaporation from the solvent was discovered in the organic gas stripping process, providing a promising approach to break the gas-liquid interface for enhanced diffusion kinetics . The feasibility of low temperature CO 2 stripping was analyzed by varying the rich solvent feeding temperature (70–100 °C). With pentane as the stripping gas, it was interesting to find an optimum rich-feed temperature lower than 90 °C, indicating great potential for a reduction in the overall energy requirement. Under the optimal conditions, the energy consumption during CO 2 regeneration, using pentane as the carrier gas, was 2.38 GJ/t CO 2 , 38.8% lower than that of the conventional stripping process. Furthermore, parasitic issues, such as water loss and solvent loss, were discussed. An improved direct non-aqueous gas stripping process with two-stage compression was used to tackle the carrier gas recovery problem. The simulation results show that more than 98% of the carrier gas can be recovered through preliminary separation approaches.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ENERGY
·
2019
·
IF 8.426
Xiaowen Zhang,Yufei Huang,Hongxia Gao,Xiao Luo,Zhiwu Liang,Paitoon Tontiwachwuthikul
The extensive energy penalty of CO 2 -loaded solution regeneration is one of the most crucial challenges facing industrial application of amine-based CO 2 capture technology. Here, to decrease the energy requirement, the regeneration behaviors of the rich 5 M monoethanolamine (MEA) and 3 M MEA-2.5 M N-methyl-diethanolamine (MDEA)−0.5 M piperazine (PZ) tri-solvent blended amines (tri-blend) with four different solid acid catalysts (H-mordenite, Hβ, HZSM-5 and Al 2 O 3 ) were studied at 98 °C. For the catalyst-free tests, the results revealed that the tri-blend hugely enhanced the CO 2 desorption kinetics and reduced the relative energy consumption compared to 5 M MEA. Based on the results of 13 C NMR, the multiple proton transfer paths and abundant bicarbonate ions in the tri-blend contribute to the improved regeneration performance. Additionally, the use of catalyst further improved the CO 2 desorption activity of the tri-blend. The combination of Hβ and tri-blend presented the best regeneration performance, increasing the desorption performance by 1360.8%, and reducing the relative energy requirement by 66.1% compared with the blank run of MEA. In addition, a plausible catalytic mechanism of solvent regeneration over the solid acid catalyst in the tri-blend was suggested. The superior catalytic performance of Hβ resulted from the large mesoporous surface area, larger number of Brϕnsted acid sites and prominent total acid sites. Furthermore, Hβ displayed excellent stability and had no adverse influence on the CO 2 absorption activity. Results herein manifest that the combination of tri-blend amines with high-efficiency catalyst is exceptional strategy for tremendously decreasing the energy consumption of amine-based CO 2 capture processes, ultimately making this technology more technically and economically feasible.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2019
·
IF 3.021
Xiayi Hu,Qian Yu,Yuanyuan Cui,Juntao Huang,Elenica Shiko,Yefeng Zhou,Zhaogang Zeng,Yang Liu,Rui Zhang
The main issue for the development of CO2 capture in industry is its high energy cost. In this work, the regeneration of the chemical solvent 3-(diethylamino)propylamine (DEAPA) with or without catalyst was studied to further reduce the energy consumption. Three different catalysts (SAPO-34, MCM-41, and SO42–/TiO2) were applied into the DEAPA system to enhance the energy efficiency by lowering the heat cost per mole of CO2 released in a CO2 stripping process. The results show that solely DEAPA (without catalyst) can increase the CO2 desorption rate by 37.28%, increase the cyclic capacity by 38.02%, and reduce the heat duty by 14.85% compared to 5 M monoethanolnamine (MEA). In addition, for the catalyst–DEAPA systems, DEAPA-SAPO-34, DEAPA-MCM-41, and DEAPA-SO42–/TiO2 could lower the heat duty by 33.08%, 27.79%, and 22.41%, respectively, relative to 5 M MEA. The SAPO-34 catalyst also shows a better efficiency for increasing the CO2 desorption rate and cyclic capacity compared to the other two catalysts used. Moreover, a possible catalytic mechanism for CO2 desorption from the DEAPA–catalyst system is proposed based on the results from catalyst characterization. Through comparing the parameters of each catalyst, it can be inferred that the mesopore surface area (MSA) and the total acid sites (TAS) are the critical factors for an efficient catalyst. The combination of MAS*TAS could especially act as a key value to evaluate the performance of a catalyst for catalytic CO2 desorption.
研究领域:
化学工程
·
环境科学
·
催化
✓ 已验证
DOI
高影响因子
International Journal of Greenhouse Gas Control
·
2016
·
IF 4.064
Shufeng Shen,Yangyang Bian,Yue Zhao
High energy consumption for aqueous amine-based CO 2 capture process is still a major drawback limiting its commercial deployment. Most of heat is used for water vaporization during solvent regeneration for CO 2 stripping. Development of phase-changing solvents is an attractive energy-efficient method to reduce energy requirement. In this work, we have proposed potassium prolinate (ProK)/ethanol solution as a novel non-aqueous absorbent. Its physical properties and the rate of CO 2 absorption were investigated and compared with the aqueous ProK systems. Phase behaviours during CO 2 absorption and partition of CO 2 absorbed between liquid and solid phases were characterized. The main species in solid precipitates were identified as bicarbonate and proline salts by 13 C NMR and XRD. Moreover, the regenerated absorbents can remain relatively stable after absorption-desorption cycles.
研究领域:
化学工程
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Xiayi Hu,Juntao Huang,Xinwei He,Qi Luo,Chao'en Li,Changbo Zhou,Rui Zhang
The challenge for the carbon dioxide (CO 2 ) capture by using amine solution is the huge energy cost in solvent regeneration process, this work combined the advantages of three conventional amines, monoethanolamine (MEA), 1-Dimethylamino-2-propanol (1DMA2P), and piperazine (PZ) to formulate an effective trio-amine blend to capture CO 2 , and the results demonstrate that the blends could reduce the energy consumption by 29.4–55.4%, increase the average desorption rate by 60–140%, and increase the cyclic capacity by 40–120%, relative to 5 M MEA solution. Through analysis the regeneration mechanism in detail, it is found that more proton provider in the trio-amine blends could help to reduce the energy consumption by lower the reaction activation energy in the deprotonation process of the protonated amines. Finally compared to the reported amine systems in considering of the energy cost, it is found that the MEA-1DMA2P-PZ could be a potential candidate for capturing CO 2 in industrial.
研究领域:
化学工程
·
环境科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiaming Mao,Chang Li,Yanbin Yun,Jia Liu,Wenjuan Yang,Meng Li,Lihua Wang,Chunli Li,Wenli Liu
To reduce the energy consumption for solvent regeneration and mitigate the corrosiveness of saturated solvents, dual-functionalized ionic liquid (IL) [DMAPA][TZ] was synthesized as a primary absorbent, and mixed with a phase separation accelerator poly (ethylene glycol) dimethyl ether (NHD) or propylene carbonate (PC) as biphasic solvents, to achieve high efficiency, energy savings, and corrosion inhibition of post-combustion CO 2 capture. The results demonstrated a transition from a homogeneous solvent to a biphasic system upon CO 2 absorption, with the majority of CO 2 being concentrated in the rich phase, which is related to the formation of hydrogen bonds. Molecular dynamics analysis showed that interaction between the IL and PC is significantly stronger than that with NHD, resulting in a reduced absorption capacity of IL-PC relative to IL-NHD, while NHD effectively suppressed the formation of HCO 3 − /CO 3 2− . At 373 K, both solvents exhibited efficient regeneration of their respective rich phases within 10 min. The calculated absorption enthalpies for IL-NHD and IL-PC are remarkably low at 0.662 and 0.772 GJ·t −1 , respectively, and the regeneration energy consumption of IL-NHD was lower to 1.387 GJ·t −1 . Notably, the phase separation accelerator exerts a significant influence on the phase-transition behavior and absorption products of biphasic solvents. Furthermore, ILs effectively inhibited corrosion through the adsorption-passivation mechanism; specifically, the corrosion rate of the CO 2 -rich phase in IL-NHD relative to 20# carbon steel was only 0.1896 mpy, which is only 1/865 of the rate of the saturated 5 M MEA solution.
研究领域:
化学工程
·
环境科学
·
材料科学
✓ 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）