INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Yufei Huang,Xiaowen Zhang,Xiao Luo,Hongxia Gao,Zain Ali Saleh Bairq,Paitoon Tontiwachwuthikul,Zhiwu Liang
The huge energy consumption of rich amine solution regeneration severely restricts the large-scale application and promotion of the CO2 capture process by the amine method. In order to reduce the operating energy consumption during the CO2 capture process using amines, especially the energy consumption of absorbent regeneration, zeolite β/SBA-15 (BS) has been synthesized in this work using the hydrothermal method with zeolite beta (β) as the silicon source; β was used to prepare the novel Zr@BS and Fe–Zr@BS catalysts for amine regeneration. Experiments for CO2 stripping were performed at 370.15 K using amine solvent [monoethanolamine (MEA)] with an initial CO2 loading of 0.50 mol CO2/mol amine. Additionally, all the materials were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, N2 adsorption–desorption experiment, ammonia temperature-programmed desorption, and pyridine adsorption infrared spectroscopy. Also, the catalytic CO2 desorption performances of seven different catalysts (β, SBA-15, three BS catalysts, Zr@BS, and Fe–Zr@BS) were investigated and assessed from the aspects of the cyclic capacity, desorption rate, and energy consumption. Experimental results indicated that the Fe–Zr@BS catalysts exhibited superior catalytic behaviors than other catalysts studied in this work, improving the desorption factor of MEA solution by 212% and bringing down the energy heat by 33% compared with 5 M MEA solution without catalysts. Furthermore, the Fe–Zr@BS catalysts show good stability and easy regeneration and do not influence absorption performance of the amine solution. Moreover, the possible catalytic mechanism for amine regeneration was proposed, and the stability of the material in terms of the structure of the material and the regeneration heat duty were also studied.
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
APPLIED ENERGY
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2018
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IF 7.9
Xiaowen Zhang,Helei Liu,Zhiwu Liang,Raphael Idem,Paitoon Tontiwachwuthikul,Mohammed Jaber Al-Marri,Abdelbaki Benamor
The aim of this work is to find a potential way for great decrease in CO 2 capture energy requirement. Here, for the first time, a series of bifunctional Al 2 O 3 /HZSM-5 catalysts (Al-ZSM) were prepared by the combined precipitation ultrasound method and used for the CO 2 desorption process. All the investigated catalysts were characterized by X-ray diffraction (XRD), Fourier transform infrared spectrometry (FT-IR), N 2 adsorption–desorption, ammonia and CO 2 temperature programmed desorption (NH 3 /CO 2 -TPD) and pyridine-adsorption infrared spectroscopy (Py-IR). The regeneration behaviors of a 5 M monoethanolamine (MEA) solvent with four Al-ZSM catalysts were studied at an initial CO 2 loading of 0.5 mol CO 2 /mol amine and the temperature of 96 °C. The results reveal that all the catalysts improve the CO 2 desorption performance, the Al-ZSM catalysts show higher catalytic performance than the single catalysts Al 2 O 3 and HZSM-5, and the Al-ZSM can reduce the heat duty by 23.3–34.2% as compared with the catalyst-free test. The use of Al-ZSM in the MEA regeneration process improves the desorption performance by 2–3 times in comparison with the blank run. A possible dual sites mechanism of CO 2 desorption with Al-ZSM is suggested. The excellent performance of Al-ZSM can be attributed to their enhanced Brϕnsted acid sites (BAS), mesopore surface area (MSA) and basic sites, which resulted from the good synergistic reaction between the Al 2 O 3 and HZSM-5, and the base treatment for HZSM-5. Besides, the stability test of the Al-ZSM was conducted. Based on the results, the Al-ZSM demonstrate a superior catalytic performance for the rich amine regeneration process, and present an excellent cyclic stability, explicitly have the potential to be a promising industrial catalyst for CO 2 capture. Furthermore, the dual sites catalytic CO 2 desorption over bifunctional catalysts will open a new path to design better catalysts for the rich amine solution regeneration process to increase the desorption performance, reduce the regeneration energy consumption, and thus further decreasing the operation costs of 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
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Qiang Sun,Hongxia Gao,Teerawat Sema,Zhiwu Liang
High energy consumption during the carbon dioxide (CO 2 ) desorption process in amine-based CO 2 capture technology is a crucial hindrance to achieving carbon neutrality. HZSM-5 is one of the most widely reported solid acid catalysts used in primary amine regeneration. This work compared a series of HZSM-5 zeolites with different Si/Al ratios in terms of CO 2 desorption performance. To further enhance catalytic activity, hierarchical HZSM-5 was synthesized by the dealumination and desilication re-assembly method with different acid and alkali concentrations. The experimental results suggested that desilication by modification in sodium hydroxide resulted in a significant improvement of mesoporous surface area. The NaOH-0.4 catalyst could improve the amount of desorbed CO 2 by 40.3% and decrease the relative heat duty by 28.5%. And the cyclic tests revealed that catalytic activity was well preserved in the recycling process. Moreover, the structure and acidity of modification samples were characterized by X-Ray diffraction (XRD), Fourier transforms infrared (FT-IR), Nitrogen adsorption–desorption experiment, temperature programmed desorption of ammonia (NH 3 -TPD), Pyridine-adsorption infrared spectroscopy (Py-IR), and scanning electron microscopy (SEM). The characterization results suggested that the synergistic effect of larger mesoporous surface area and total acid sites was important to enhance catalytic CO 2 desorption performance. These results showed a new understanding of catalyst design for CO 2 capture technology by modifying the structure of the catalyst support.
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
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
YiRong Yao,Bing Xing,Jianbing Chen,YanLun Ren,YuJia Ma,Ying Zhang,Li Zhang
This study proposes an advanced method to tackle CO 2 emissions by enhancing solid acid catalysts, aiming to reduce the high energy consumption and low economic efficiency typically associated with chemical absorption processes. The research involves modifying commercial HZSM-5 zeolites through Cu ion exchange, with the optimal performance observed at a Cu ion content of 2.86 % and a Cu salt concentration of 0.2 M. This modification significantly minimizes the loss of copper ions—a common issue in the impregnation method—resulting in a 76.62 % reduction in the loss of active components. To further improve CO 2 gas-liquid mass transfer, mesoporous MCM-41 zeolites were introduced. Experimental results demonstrate that, at a regeneration temperature of 86°C and a mass ratio of 2:1 for HZSM-5 to MCM-41, the combined catalyst achieves a 61.28 % reduction in relative heat duty compared to the blank sample. Moreover, the energy consumption is 12.33 % and 16.45 % lower than that of HZSM-5 and MCM-41 used individually. Characterization analysis reveals that, under comparable acidic active site densities, catalysts with superior physical pore structures exhibit enhanced catalytic performance. The introduction of mesoporous structures notably improves the bidirectional mass transfer efficiency between carbamate macromolecules and CO 2 molecules. This work successfully demonstrates the synergistic effect of combining Cu ion-modified HZSM-5 zeolites with mesoporous MCM-41, leveraging the abundant active sites of HZSM-5 while harnessing the enhanced mass transfer properties of MCM-41.
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
AICHE JOURNAL
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2025
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IF 4
Jia Xiong,Qiang Sun,Hongxia Gao,Zhiwu Liang
Catalytic amine–based solution regeneration has attracted considerable attention due to its potential to reduce energy consumption in carbon dioxide (CO 2 ) separation. However, the limited catalytic activity and cycling stability of catalysts under high–temperature alkaline conditions hinder their industrial application. Herein, zirconium hydrogenphosphate (ZrHP) catalysts, featuring abundant acidic sites, were first utilized for amine solution regeneration. By leveraging its proton donation and acceptance mechanism, efficient monoethanolamine solution regeneration was achieved. The ZrHP–4 catalyst demonstrated a 526% increase in the instantaneous CO 2 desorption rate compared to the non–catalytic test, reducing the relative heat duty by 48%. Moreover, ZrHP–4 exhibited remarkable stability over 10 cycles without requiring regeneration. Density functional theory calculations revealed that ZrHP promotes CO 2 desorption by elongating the C—N bond of carbamate and lowering the proton transfer energy barrier. Therefore, this study offers novel insights into the design and mechanistic understanding of efficient and stable catalysts for amine solution regeneration.
研究领域:
化学工程
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催化科学
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环境科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Lijie Fu,Juanjuan Gong,Hengyu Li,Jinhua Xiao,Bihong Lv,Xiaomin Wu,Zhiwei Huang,Zuoming Zhou,Guohua Jing
The regeneration of catalytic amine-based solvents using solid acid offers a promising approach to reduce energy consumption in CO 2 capture processes. Nickel-based solid acid catalysts, endowed with multiple Lewis acid sites, could enhance the efficiency of regeneration reactions. Nevertheless, the irregular pore structure of NiO and the deficiency in Brønsted acid sites posed significant challenges to the practical use of amine solvent regeneration in CO 2 vapor stripping processes. A highly effective solid acid catalyst, nickel-modified H-β (Ni/β), were synthesized to enhance CO 2 desorption from MEA solutions saturated with CO 2 . The catalyst with 1.25% Ni (1.25% Ni/β) exhibited the highest activity and stability, with a 43.19% increase in the amount of desorbed CO 2 and a 30.16% reduction in relative heat duty. The catalyst maintained excellent stability, enhancing the desorption performance of MEA after ten cyclic absorption–desorption experiments. According to theoretic calculations and experimental analyses, the incorporation of H-β zeolite significantly enhanced the specific surface area of the composite and introduced a substantial number of Brønsted acid sites. Concurrently, the introduction of metal nickel substituted the hydrogen proton on the hydroxyl groups of the H-β molecular sieve, increasing the Lewis acid sites and modulating the Brønsted-to-Lewis acid site ratio. The Brønsted acid sites functioned as proton donors, while the Lewis acid sites facilitated N-C bond cleavage, promoting carbamate decomposition and the deprotonation of protonated amines. This work presents a valuable solid acid catalyst for amine-based CO 2 capture and offers insights for developing innovative solid acids for various catalytic processes.
研究领域:
化学工程
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环境科学
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Aicheng Song,Zhitao Han,Xiao Yang,Mengjing Zhang,Xi Wu,Zelu Zhou,Dong Liu,Dong Ma
The high energy consumption associated with solution regeneration in amine-based CO 2 capture processes remains a major challenge for large-scale carbon capture and storage (CCS) applications. However, the addition of solid acid catalyst accelerates the slow CO 2 desorption process while reducing the energy consumption for regeneration of the amine-rich solution. Herein, we innovatively developed Mn 3 O 4 -modified SAPO-34 catalysts via impregnation, demonstrating exceptional efficacy in reducing energy consumption for CO 2 -rich monoethanolamine (MEA) solution regeneration. Mn 15 -SAPO catalyst exhibited excellent performance in catalytic desorption tests using a 5 M CO 2 -rich MEA solution at 90 °C, achieving a 31.0 % increase in CO 2 desorption rate, a 133.3 % increase in CO 2 desorption amount, and a 57.1 % reduction in solution regeneration heat duty compared to the non-catalytic process. Comprehensive characterization revealed that the optimized Mn 15 -SAPO catalyst featured abundant strong acidic sites, optimal mesoporous structure, and the redox activity of Mn 3+ /Mn 4+ species. FTIR and 13 C NMR analysis confirmed the catalytic accelerating effect of catalysts on the conversion of intermediates. A possible reaction mechanism for the catalytic desorption of CO 2 over Mn x -SAPO catalysts was discussed. Additionally, the cycling stability of Mn 15 -SAPO catalyst was also evaluated. This work demonstrated the potential of Mn 15 -SAPO catalyst in enhancing the efficiency of the amine CO 2 capture process and reducing energy consumption, which was conducive to the application of industrial CO 2 capture.
研究领域:
能源与燃料
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环境科学
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催化
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化学工程
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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）