CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Xitong Yang,Guowei Liu,Ruifeng Zhou,Zhengzheng Xie,Yamin Cheng,Muhammad Shuaib Khan,Qiuye Li
Catalytic desorption can reduce the activation energy of the reaction and increase the desorption reaction rate, and is one of the most promising technologies to solve energy consumption problems of CO 2 capture technology for organic amine solutions. In order to further reduce desorption energy consumption, we propose a new method of utilizing the photothermal effect of catalysts to increase desorption temperature and accelerate reaction kinetics, and coupling the proton transfer ability of the catalyst itself to form multifunctional catalysis. In this work, we synthesized Ru x Mn 1-x OOH catalyst by introducing Ru atoms at the Mn vacancies on the MnOOH surface, grasping the advantages of the photothermal and proton transfer ability of Ru-dopants. The results showed that the CO 2 desorption capacity increased by 43.1% with adding MnOOH compared to without a catalyst. The Ru-doped catalyst demonstrated a 54.7% increase in CO 2 desorption efficiency, with an additional 98.2% surge attributed to the in-situ photothermal effect generated by the catalyst under light irradiation. Characterization and density functional theory (DFT) calculations revealed that Ru doping significantly enhanced the proton transfer ability while simultaneously weakens the adsorption capacity of monoethanolamine (MEA) on the catalyst surface. Moreover, the stronger photothermal effect introduced by Ru leads to an increase in the surface temperature of the catalyst, which is key to the faster and efficient desorption of CO 2 . This work provides a new approach to improve the proton transfer ability of catalysts and offers a novel photothermal coupled catalytic scheme for CO 2 desorption in organic amine carbon capture technology.
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
AICHE JOURNAL
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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
APPLIED ENERGY
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2024
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IF 10.1
Yingjie Niu,Ting Li,Ali Hassan Bhatti,Jiaqi Qu,Xin Zhou,Li Luo,Francesco Barzagli,Chao'en Li,Rui Zhang
The use of solid acid catalysts for sorbent regeneration is an emerging approach to improve the energy efficiency of CO 2 capture processes. In this study, fly ash (FA), an industrial byproduct rich in acid/base sites, was chosen as a support material for the solid acid SO 4 2− /ZrO 2 (SZ) in the preparation of SZ@FA composite catalysts. Three catalysts with different mass ratios between SZ and FA were synthesized and evaluated in the regeneration process at 88 °C of a CO 2 -saturated MEA solution. Their desorption performance, expressed as CO 2 desorption rate, amount of CO 2 desorbed , and heat duty, was then compared with that obtained with unmodified FA, ZrO 2, and in the absence of catalysts (blank), under identical operating conditions. Compared to the uncatalyzed system, the SZ@FA composite catalysts showed significantly better desorption performance. In particular, SZ@FA-1/2 provided the highest values of desorption rate and cyclic capacity while reducing energy consumption by 45.4% compared to the blank system. It also demonstrated stability over 20 consecutive absorption-desorption cycles. Comparison with other reported catalysts highlighted the high performance of SZ@FA-1/2, particularly in terms of relative heat duty reduction, positioning it as a cost-effective and environmentally friendly choice for post-combustion capture applications.
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Qiang Sun,Tianhao Li,Yu Mao,Hongxia Gao,Teerawat Sema,Shengyu Wang,Libin Liu,Zhiwu Liang
Amine-based CO2 capture is a promising method to limit global CO2 emissions. However, large thermal energy consumption for CO2 desorption during amine regeneration has limited large-scale worldwide applications. Here, we show that an efficient MCM-41-SO3H-0.6 catalyst presented a superior catalytic performance, decreasing the relative heat duty by one-third and enhancing the instantaneous desorption rate by up to 195% in comparison with the monoethanolamine (MEA) regeneration without catalysts. The excellent catalytic activity is related to the combination of the properties of mesopore surface area × total acid sites, and a possible catalytic mechanism is proposed for the MCM-41-SO3H catalysts. Furthermore, the experimental results in the MEA solution regeneration process were consistent with density functional theory calculations in revealing the catalytic desorption mechanism. This work demonstrated that MCM-41 functionalized with sulfonic acid group catalysts could play an essential role in the post-combustion CO2 capture technology using aqueous MEA for industrial applications.
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
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2025
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IF 9
Haozhan Chu,Shaojuan Zeng,Xiangping Zhang,Guoxiong Zhan,Bo Wang,Hongyu Zhang,Sheng Zhong,Wei Liu
Ionic liquids (ILs) show great application potentials in CO 2 capture due to extremely low vapor pressures, tunable structures, and strong CO 2 affinity. Up to date, many efforts have been focused on the design and absorption performance of novel functionalized ILs, rather than desorption performance. In our previous work, the IL solvent [Cho][Triz]/TMS exhibited exceptional CO 2 absorption performance. As a successive study on decreasing regeneration energy consumption, this work focused on the design and synthesis of novel metal-modified MCM-41 catalysts with multiple acidic sites to enhance CO 2 catalytic desorption in the nonaqueous [Cho][Triz]/TMS (80 wt%/20 wt%) absorbent under lower temperatures. Among all the composite MCM-41 catalysts, the CoM-1/4 catalyst exhibits superior catalytic performance because of the increase of Brønsted acid sites by 232.3 % and Lewis acid sites by 56.2 % compared with pristine MCM-41, which promote CO 2 desorption by accelerating C-N bond breaking. The CO 2 desorption rate and amount increased by 180.2 % and 95.7 %, and the activation energy reduced by 46.7 % compared to the non-catalysis. Therefore, the theoretical regeneration energy consumption of the catalyst-added system was 0.88 GJ/t CO 2 , representing a 76.7 % reduction compared with the 30 wt% MEA solution. Furthermore, the CoM-1/4 catalyst maintained high catalytic activity after 20 cycles. This work indicated that the CoM-1/4 catalyst effectively enhanced the regeneration performance of IL absorbent, facilitating the development of an energy-efficient CO 2 capture process for industrial applications.
研究领域:
化学工程
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环境科学
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催化材料
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DOI
高影响因子
APPLIED ENERGY
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2019
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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
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环境科学
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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
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DOI
高影响因子
APPLIED ENERGY
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2018
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IF 7.9
Xiaowen Zhang,Rui Zhang,Helei Liu,Hongxia Gao,Zhiwu Liang
To enhance the energy efficiency of the CO 2 desorption process, the regeneration behaviors of the CO 2 -loaded 6 M MEA-AMP-PZ (monoethanolamine, 2-amino-2-methyl-1-propanol and piperazine) tri-solvent blends with different AMP/PZ molar ratios with four different solid acid catalysts (H-ZSM-5, γ-Al 2 O 3 , SAPO-34 and SO 4 2− /TiO 2 ) and a blank at 96 °C were investigated in terms of CO 2 desorption rate, cyclic capacity and relative heat duty. For the no-catalytic runs, the results showed that all the tri-solvent blended amines greatly increased CO 2 desorption rate, cyclic capacity and decreased the relative heat duty in comparison with 5 M MEA. The 13 C NMR analysis indicated that the 3 M MEA-2.5 M AMP-0.5 M PZ blend with the highest AMP/PZ ratio produced the largest amount of bicarbonate and less carbamate, which resulted in the best desorption performance. With regard to catalyst, when the solid acid catalysts were introduced, the regeneration performance of the blend was further improved. The best of the blends along with H-ZSM-5 provided the combination with the best performance in CO 2 desorption, and reduced the relative heat duty by 61.6% as compared to 5 M MEA without catalyst (100%). Five relevant physicochemical properties of the catalyst were obtained and used to better understand the catalytic regeneration process. A possible catalytic CO 2 desorption mechanism was analyzed. The results revealed that the mesopore surface area coupled with total acid sites of the catalyst had the most positive influence on improving the CO 2 desorption performance. Findings from this work imply that the combination of solid acid catalyst with tri-solvent blended amines is a promising alternative method for further reduction of solvent regeneration energy requirement.
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
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yao Shen,Ke Wang,Lu Li,Jingkai Zhao,Jiexu Ye,Ping Chen,Xiang Gao,Shihan Zhang
Catalyst-aided CO 2 desorption offers a promising reduction in the energy penalty of amine scrubbing, but faces the challenges of slow mass transfer, sluggish desorption kinetics, and susceptibility to deactivation. In this work, a hollow composite catalyst C@ZrO 2 was developed to simultaneously realize rapid electron, proton and mass transfer for CO 2 desorption via facilitating proton-coupled electron transfer (PCET) effect. The CO 2 desorption rate of benchmark MEA solution increased by 126% and relative heat duty decreased by 69.9% in presence of C@ZrO 2 , and its catalytic performance didn’t noticeably decline after 10 cycles. Additionally, the desorption rate of biphasic solvents with a high viscosity increased by 112% and relative heat duty decreased by 57.3% with C@ZrO 2 . Based on theoretical calculation, the facilitated PCET efficiency of carbon layer increased the binding energy of carbamate to enhance its mass transfer rate from the liquid phase to the C@ZrO 2 surface, and stretched the C-N bond to reduce the proton transfer energy barrier by 66.8%. This work provided a novel insight to design catalysts for energy-efficient and stable CO 2 capture.
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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产品关联
DOI
高影响因子
Greenhouse Gases-Science and Technology
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2021
·Vol. 11
·期 5
·974-987
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IF 2.013
Shunji Kang,Zhi Shen,Xizhou Shen,Liuya Fang,Li Xiang,Wenze Yang
The carbon dioxide discharged from fossil fuels combustion products is considered as a major contributor to global warming. The current investigation aimed at CO 2 desorption kinetics in 3.25 mol L –1 methyldiethanolamine (MDEA)–0.1 mol L –1 piperazine (PZ) rich amine aqueous solution with thermo-gravimetric analysis (TGA) method under different heating rates of 2.5, 5, 10, and 20 °C min –1 . The kinetics parameters were determined by comparison of 40 mechanism functions with thermal analysis kinetic method. The average activation energy E was 59.16 kJ mol –1 , preexponential factor A was 5.54 × 10 8 , and the most probable mechanism function was G( α ) = [–ln(1 – α )] 3/2 . In addition, the kinetic parameters of CO 2 desorption process from three rich amine aqueous solutions (MDEA, MDEA + diethanolamine(DEA), MDEA + PZ) were compared and the influence of kinetic parameters was further discussed. The desorption rate models of three rich amine aqueous solutions were established and desorption rates were well predicted. The order of desorption rate inferred from desorption rate model was MDEA > MDEA + DEA > MDEA + PZ. The results indicated that TGA combined with thermal analysis kinetics was an effective and quick method with high accuracy, easy operation, and good repeatability for screening absorbents preliminarily in laboratory. © 2021 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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热分析
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
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2025
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IF 9.5
Ze Li,Youbin Zheng,Yuze Wang,Zhenjie Hao,Yuhui Huang,Rui Zhu,Dinghao Zheng,Ruixia Zhong,Liang Dong,Jianbing Zang,Pengfei Li,Zheng-Jun Wang
To address the kinetic limitations of CO2 desorption in the urea oxidation reaction (UOR), we develop a urotropine-induced strategy to engineer NiS–Ni3S2@g-C3N4 electrocatalysts. Urotropine, serving as both a structure-directing agent and g-C3N4 precursor, forms a dandelion-like architecture with narrowed columnar fluffs to maximize the surface area. The electronegativity difference between g-C3N4 and NiS–Ni3S2 induces local electron interactions, converting inactive sites to electron-enriched active sites and reducing adsorption energy barriers for CO2 desorption, the rate-limiting step. This catalyst exhibits outstanding UOR performance with a 1.24 V onset potential, 1.34 V to reach 100 mA cm−2, and 90% activity retention over 40 hours, while also demonstrating superior trifunctional activity rivaling IrO2 (OER: η10 = 90.9 mV) and Pt/C (HER: η10 = 13 mV). The urea electrolyzer requires only 1.26 V for 10 mA cm−2 with 48-hour stability. This work provides a breakthrough in designing efficient electrocatalysts through synergistic structural and electronic regulation.
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DOI
高影响因子
ELECTROCHIMICA ACTA
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2025
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IF 5.6
Dongya Liu,Shaohan Xing,Xiuping Chen
Interface engineering via the construction of heterojunctions to accelerate electron transfer is an effective strategy for enhancing electrocatalytic activity. This study designed and synthesized a NiFe 2 O 4 /CeO 2 Mott–Schottky (M–S) heterojunction for efficient urea oxidation reaction (UOR), which exhibits exceptional activity with a current density of 50 mA cm −2 at 1.40 V (vs. RHE). Spectroscopic analyses validate the formation of the M–S heterojunction, where a significant work function difference drives spontaneous electron transfer from NiFe 2 O 4 to CeO 2 through Ni–O–Ce bridge, thereby establishing a strong built-in electric field. This interfacial charge rearrangement precisely modulates the electronic structure of the Ni sites, enhancing initial urea adsorption and lowering the d -band center. Such modulation weakens intermediate binding and reduces the energy barrier for the rate-determining CO 2 desorption step. The utility of NiFe 2 O 4 /CeO 2 is demonstrated through reduced energy consumption in hybrid water electrolysis along with improved efficiency and longevity in urea-assisted zinc–air batteries. This study elucidates the effectiveness of M–S heterojunction engineering for developing highly efficient catalysts for advanced energy conversion and storage.
研究领域:
电化学
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催化
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材料科学
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能量转换
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纳米技术
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表面科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）