AICHE JOURNAL
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2022
·Vol. 68
·期 8
·e17706
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IF 4.167
Qiang Sun,Hongxia Gao,Yu Mao,Teerawat Sema,Sen Liu,Zhiwu Liang
High heat duty is an urgent challenge for industrial applications of amine-based CO 2 capture. The temperature (>110°C) of carbamate breakdown in amine regeneration requires large energy consumption. In this work, we report a novel, stable, efficient, and inexpensive Ni-HZSM-5 catalyst to improve the CO 2 desorption rate and reduce the heat duty. The impregnation method was applied for varying nickel content in the catalysts from 2.16 to 9.80 wt% in HZSM-5. The catalysts were characterized by scanning electron microscope, X-ray powder diffraction, N 2 adsorption–desorption, inductively coupled plasma-optical emission spectrometry, ultraviolet-visible diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy, NH 3 -temperature programmed desorption (TPD), Infrared spectroscopy of pyridine adsorption, and Fourier transform infrared spectroscopy. The catalytic performance was evaluated by CO 2 desorption of rich amine solvent at 90°C. It was found that the introduction of nickel increased the acid sites of catalysts compared with parent HZSM-5. This phenomenon plays a key role on improving the CO 2 desorption rate. The density functional theory (DFT) calculations successfully explain the catalytic performance. The catalytic activity associates with the combined properties of MSA × B/L × Ni 2+ . The 7.85-Ni-HZ catalyst presents an excellent catalytic activity for the CO 2 desorption: it increases the amount of desorbed CO 2 up to 36%, reduces the relative heat duty by 27.07% with the same reaction time, and possesses high stability during five cyclic tests. A possible catalytic mechanism for the Ni-HZSM-5 catalysts through assisting carbamate breakdown and promoting CO 2 desorption is proposed based on experimental results and theoretical calculations. Therefore, the results present that the 7.85-Ni-HZ catalyst significantly accelerates the protons transfer in CO 2 desorption and can potentially apply in industrial CO 2 capture.
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
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
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2023
·Vol. 99
·期 1
·183-194
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IF 3.4
Zhen Wang,Zhitao Han,Gang Liu,Zelu Zhou,Xi Wu,Song Zhou,Xinxiang Pan
BACKGROUND The large-scale practical application of CO 2 capture using carbonate solutions is mainly limited by their low CO 2 absorption rate. In view of this, it is feasible to improve CO 2 capture performance of carbonate solution by adding additives. In this paper, low-cost sodium carbonate (Na 2 CO 3 ) solution was selected as the main CO 2 absorbent, and the effects of different organic additives on CO 2 capture performance of Na 2 CO 3 solutions were systematically investigated. RESULTS The results showed that 0.04 mol/L tetrabutylammonium bromide (TBAB) could achieve a better enhancement effect on CO 2 capture performance of Na 2 CO 3 solution. After addition of TBAB, the maximum CO 2 absorption rate of Na 2 CO 3 solution was improved to 2.52 × 10 −3 mol/min, which increased by 105%. And the maximum CO 2 desorption rate could also be improved by 45%. TBAB/Na 2 CO 3 system not only realized a high CO 2 absorption capacity of 0.769 mol/mol, but also maintained 82% of the initial CO 2 absorption capacity after three cyclic tests. The regeneration heat duty of TBAB/Na 2 CO 3 solution was calculated to be 1136.6 kJ/mol, which was significantly lower than that of single Na 2 CO 3 solution and conventional MEA aqueous solution. The promotion mechanism of TBAB in Na 2 CO 3 solution was explored using Fourier transform infrared spectra (FTIR) and 13 C nuclear magnetic resonance (NMR) analysis. CONCLUSION The introduction of TBAB additive could significantly improve CO 2 capture performance of Na 2 CO 3 solution and reduce regeneration heat duty, making it a possible option in the field of post-combustion CO 2 capture. © 2023 Society of Chemical Industry (SCI).
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
ENERGY & FUELS
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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
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环境科学
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催化
✓ 已验证
DOI
高影响因子
ENERGY
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2025
·
IF 9.4
Kefei Li,Yue Wu,Yiming Bai,Hai Yan,Yiming Wang,Yuzhe Guan,Liang Li,Guicheng Liu
Reducing the energy consumption of CO 2 regeneration is crucial for enhancing the economic feasibility of CO 2 capture processes. While most studies have focused on developing novel absorbents, the influence of operating parameters on gas-liquid mass transfer behavior and their subsequent impact on energy consumption has received limited attention. This study experimentally investigates the regeneration heat duty (Q reg ) for CO 2 desorption from a 1-(Dimethylamino)-2-propanol (1DMA2P)/2-Methylaminoethanol (MAE) aqueous blend in a lab-scale stripper equipped with high-efficiency Sulzer DX structured packing. The effects of key operating parameters, including rich CO 2 loading, lean CO 2 loading, solution flow rate, amine concentration, and synergistic parameters (Δ α × L and C × L ), on Q reg were systematically analyzed. The experimental results showed that all these factors greatly influenced Q reg . For example, the Q reg decreases as the lean CO 2 loading (α lean ) , rich CO 2 loading (α rich ) , and 1DMA2P/MAE concentration (C) increase, indicating that the Q reg can be reduced by optimizing these operating parameters. Additionally, compared with MEA, 1DMA2P/MAE reduces energy consumption by 51.5 % and decreases the stripper height by 35 %. This study underscores the critical role of operating parameters in reducing CO 2 regeneration energy consumption. The findings provide valuable insights into optimizing stripper performance and demonstrate the advantages of the 1DMA2P/MAE blend as an energy-efficient alternative to MEA-based solvents in industrial CO 2 capture applications.
研究领域:
化学工程
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环境工程
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能源技术
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过程优化
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2020
·
IF 7.632
Zhibiao Chen,Guohua Jing,Bihong Lv,Zuoming Zhou
A nonaqueous, phase-change absorbent of 2-amino-2-methyl-1-propanol (AMP)/piperazine (PZ) and environmentally friendly solvent dipropylene glycol dimethyl ether (DME) fixes a number of issues suffered by a solid–liquid biphasic solvent, such as high viscosity of the saturated solution and difficult separation and regeneration of the viscous solid. The solid phase occupies 43% of the total volume while attributes about 94% of the total loading (0.87 mol mol–1) of the solution. Beside the formation of AMP-carbamate and PZ-carbamate according to zwitterions mechanism, the coupling products of AMP/PZ-carbamate are also found in the crystal, which helps to reduce the desorption temperature during the regeneration. Because of low solubility, self-aggregation, and high lattice energy in DME, the CO2 products precipitate and form a white crystalline powder in the lower phase of the solution. Meanwhile, the solid precipitation helps the bulk solution to keep a lower partial pressure and higher diffusivity of CO2, conforming a perfect performance of CO2 capture into the biphasic solvent. The regeneration heat duty of the solvent (1.61 GJ t–1 CO2) was approximately 57% less than that of the benchmark monoethanolamine (MEA) because of its perfect performance on CO2 capture, such as high absorption loading, high regeneration efficiency, and low amount of rich phase required for regeneration. The novel absorbent has a great potential for green and sustainable CO2 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
APPLIED ENERGY
·
2024
·
IF 10.1
Bingling Yuan,Zhen Chen,Qianxuan Zhang,Guoxiong Zhan,Lei Xing,Zhoulan Huang,Yuchen Li,Lidong Wang,Junhua Li
Chemisorption with biphasic solvents is a promising low-energy strategy for separating CO 2 from industrial flue gas, however, amine degradation and changes in water content can considerably impede the phase-splitting performance. To the issues, tetramethylene sulfone (TMS) was selected as separating agent to prepare a biphasic solvent with polyamine triethylenetetramine (TETA) with a TETA:TMS:H 2 O ratio of 2:6:2 (denoted as 20 T-60TMS). The CO 2 loading of the blended phase and the volume fraction of the rich phase were 2.56 mol/L and 35.4%, respectively; the total regeneration heat duty was 2.36 GJ/tCO 2 . The proposed biphasic solvent exhibited better resistance to oxidative degradation and thermal degradation than did previously reported solvents, attributed to the beneficial effect of TMS. Additionally, the degradation products did not substantially reduce the phase separation performance after a 360 h thermal degradation test. A dynamic phase-splitting evaluation revealed that the 20 T-60TMS solvent was robust to changes in water content. Theoretical calculations confirmed that the introduction of TMS weakened the hydrogen bond between TETACOO − /TETAH + and H 2 O, engendering enhanced TETACOO − and TETAH + self-aggregation, forming a strong hydrogen bond network, and achieving fast phase separation. This work provides a novel biphasic solvent with excellent tolerance and stability for CO 2 capture from flue gas.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2023
·
IF 4.7
Qiang Sun,Jia Xiong,Hongxia Gao,Wilfred Olson,Zhiwu Liang
Catalytic CO 2 desorption from rich amine solution is a practical approach to reducing energy consumption for amine regeneration. In this study, for the first time, the catalytic effect of environmentally friendly, imidazole series ionic liquids ([Bmim]PF 6 , [Bmim]BF 4 , [Bmim]HSO 4 , [Bmim]NO 3 , [Bmim]CH 3 COOH, [Bmim]Cl, [Bmim]Br, and [Bmim]I) is evaluated in terms of CO 2 desorption rate, amount of CO 2 released, and heat duty. Overall, the [Bmim]PF 6 catalyst shows excellent catalytic activity for CO 2 desorption, increasing the quantity of CO 2 released by 21.35% and reducing the relative heat duty by 17.59%. In addition, the catalytic applicability of [Bmim]PF 6 for secondary and tertiary amine systems was evaluated. Of note, the homogeneous [Bmim]PF 6 catalyst presents good stability during 5 cycles. The catalyst/MEA (monoethanolamine) solution ratio of 3 wt% retained about 94% of the catalytic performance after five cycling tests without any reactivation step, showing the potential application of this desorption technology for CO 2 capture with lower heat duty.
研究领域:
化学工程
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环境科学
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催化
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碳捕集与封存
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
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IF 7.864
Chenkai Jiang,Han Chen,Junliang Wang,Yao Shen,Jiexu Ye,Shihan Zhang,Lidong Wang,Jianmeng Chen
A biphasic solvent features high absorption capacity and low heat duty for CO2 capture. Phase separation behavior is essential to cut down energy penalty. Four phase splitting agents with different hydrophobicities, such as 1,3-dimethyl-2-imidazolidinone (DMI), 1-methyl-2-pyrrolidinone (NMP), N,N-dimethylformamide, and sulfolane, were dosed to biphasic solvents, triethylenetetramine and 2-(diethylamino)ethanol. Experimental results revealed that they can tune the phase separation behavior during CO2 absorption. Generally, under the same CO2 loading, the volume ratio of the rich phase increased with their hydrophobicity (log P), which accounts for over 50%. Moreover, their influences on absorption capacity, kinetics, and thermodynamics were also investigated. After dosing NMP, the heat duty was decreased by 22%. Furthermore, a phase splitting agent with a positive log P was more conducive to reducing the heat duty, and one with a negative log P enhanced the absorption rate. With DMI, the absorption rate was 114% higher than that of MEA at rich loading. The 13C NMR analysis showed that the agents were not involved in CO2 absorption and did not affect the reaction mechanism. Furthermore, quantum calculation was used to verify the reaction mechanism, confirming that the phase splitting agent increases the reaction equilibrium constant and makes it proceed more thoroughly.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）