SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Hang Yu,Tieyan Li,Xingda Yang,Chunxi Li,Jianguo Mi,Hong Meng,Junsu Jin
In order to improve the heat transfer efficiency of the shaped activated carbon in CO 2 adsorption, we proposed a rapid CO 2 adsorption–desorption approach by coating the outer surface of the metal tube with a hydrophobic carbon layer. The coating layer was prepared by carboxylated cellulose nanofibers (CNF) as the binder, coconut shell-activated carbon as the carrier, and methyltrimethoxysilane (MTMS) as the hydrophobic modifier. The oxygenated groups can increase its surface polarity and adsorptivity for the weakly polar small molecules like carbon dioxide. The equilibrium adsorption capacity of SAC-6-1.0 for CO 2 in dry (15 vol% CO 2 ) and wet flue gas (15 vol% CO 2 + 4.7 vol% H 2 O) is 39.4 mg/g and 34.3 mg/g, respectively, at 40 °C and 1.0 bar, which is 54.5% and 382.4% higher than that of the original activated carbon. After 10 cycled reuses, over 97% of its adsorption capacity can be retained. The CO 2 adsorption performance of SAC-6-1.0 is better than most of the oxygenated and sulfur-doped activated carbons, albeit slightly worse than that of nitrogen-doped ones. The present hydrophobic carbon coating approach is of great industrial application in the field of CO 2 capture and other gas separation.
研究领域:
材料科学
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环境工程
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2023
·Vol. 25
·期 4
·1513-1521
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IF 9.8
Zhe Wang,Zhuo Li,Liying Liu,Peizhi Cao,Shupeng Li,Gang Kevin Li
Post-combustion carbon capture from fossil fuels for concentrated sources such as power plants is considered as one of the efficient ways to mitigate CO2 emissions. However, conventional adsorbents in physical adsorption processes have faced challenges in the presence of moisture in flue gases. Here, we successfully synthesized polypyrrole (PPy) adsorbent using Fenton's reagent and demonstrated that the filtrate could be recycled for the synthesis of PPy. The single-component gas-adsorption capacities of PPy were measured to obtain CO2, CH4, and N2 adsorption amounts of 16.73, 5.19, and 1.06 cm3 g−1 at 303 K and 101 kPa, respectively. Calculations by the IAST method demonstrated that PPy had excellent gas selectivities for CO2/N2 and CO2/CH4 of 46 and 4.0, which could be utilized for CO2 separation in flue gases and biogas. To simulate flue gas carbon capture, we investigated the dynamic adsorption capacity of PPy on CO2 in the presence of water vapor using a breakthrough device in the laboratory. The CO2 adsorption capacity was twice higher in moisture than in dry conditions, which was attributed to the presence of water vapor-formed hydrogen bonds that enhance its adsorption capacity through electrostatic and acid–base interactions of CO2 with PPy. This green and facilely synthesized polypyrrole adsorbent has great potential for carbon capture in high humidity flue gases.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Shanshan Shang,Chao Yang,Mingzhe Sun,Zeyu Tao,Aamir Hanif,Qinfen Gu,Jin Shang
CO 2 capture from large point sources is indispensable for achieving 1.5 degree target as long as fossil fuels are still in use. Selective adsorption of CO 2 from flue gas constitutes a promising CO 2 capture technology, thanks to the development of numerous fascinating solid adsorbents in the past three decades. However, very few adsorbents can retain their required performance in the presence of moisture which is unfortunately always the case in reality. In this study, we elevated the CO 2 adsorption and separation performance of a water-stable aluminum-based porphyrin metal-organic frameworks (Al-PMOF) by inserting transition metals as adsorption sites. Compared with the pristine Al-PMOF and other four transition metals (TMs) incorporated PMOFs (Al-PMOF(M)), the Co-inserted Al-PMOF (Al-PMOF(Co)) exhibited the highest CO 2 adsorption capacity (3.32 mmol/g) and highest CO 2 /N 2 and CO 2 /CH 4 selectivity (87 and 20, respectively) at 273 K and 1.0 bar. After three consecutive cyclic moisture treatments, the CO 2 adsorption capacity of Al-PMOF(Co) remained almost unchanged. More importantly, the dynamic binary CO 2 /N 2 breakthrough adsorption of Al-PMOF(Co) exhibited negligible differences in CO 2 adsorption capacities between dry and wet flue gas conditions, suggesting that TMs incorporated Al-PMOF possess excellent moisture-resistant properties. Mechanistic studies using the combined in situ synchrotron infrared spectroscopic and powder X-ray diffraction together with density functional theory calculations unambiguously revealed the inserted metals are the dominant CO 2 adsorption sites. This study materializes the rational design of efficient adsorbents for CO 2 capture and contributes to mitigating climate change.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Journal of the American Chemical Society
·
2025
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IF 15.6
Deyun Sun,Shangqing Chen,Miao He,Hongxue Xu,Yongxiang Sun,Lijuan Shi,Hongbo Zeng,Qun Yi
Efficient extraction of high-purity CO2 from humid flue gas via adsorptive separation offers a promising and sustainable solution for carbon reduction and downstream applications. However, the coadsorption of H2O vapor and N2 from humid flue gas remains a persistent challenge that limits separation efficiency. To overcome this issue, this work introduces a novel concept of ionic hydrophobic gates on porous adsorbents, which enables one-step separation of high-purity CO2 directly from humid flue gas. By assembling hydrophobic ionic liquids and fluorine-rich terephthalaldehyde onto the surface of a metal–organic framework (MOF), this design establishes H2O barriers and CO2 channels on the outer shell while maintaining pore integrity in the core. The resulting core–shell material demonstrates exceptional CO2 adsorption capacity and an extraordinary CO2/N2 selectivity of 1780 (15/85, v/v), surpassing conventional adsorbents. Notably, dry CO2 with 99.999% purity is successfully extracted from humid flue gas (relative humidity, RH = 100%) in a single breakthrough experiment. In situ diffuse reflectance Fourier transform infrared spectroscopy (in situ DRIFTS) and density functional theory calculations reveal that fluorine-rich hydrophobic sites act as effective H2O barriers, while ionic liquid segments facilitate the transport of CO2 through hydrogen bonding and electrostatic interactions. Owing to its excellent scalability and broad compatibility with diverse MOF platforms, this ionic hydrophobic gating strategy offers a robust and versatile approach for constructing advanced gas separation materials, holding great promise for industrial applications in carbon capture, clean energy, and sustainable chemical processes.
研究领域:
材料科学
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化学工程
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环境科学
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产品关联
DOI
PubMed
高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2018
·Vol. 35
·期 8
·1642-1649
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IF 2.199
Wang Yushun,Du Tao,Fang Xin,Meng Da,Li Gang,Liu Liying
CO 2 capture from humid flue gas is always costly due to the irreplaceable pretreatment of dehydration in current processes, which creates an urgent demand for moisture-insensitive adsorbents with considerable CO 2 uptakes as well as remarkable H 2 O tolerances. In the present work, the microporous titanium silicate molecular sieve ETS-10 was synthesized with coal fly ash as the only silica source. The as-synthesized ETS-10 was characterized by X-ray diffraction, scanning electronic microscopy and infrared spectroscopy to verify its crystal morphology, in which neither impurity nor aggregation was observed. The following CO 2 adsorption experiments on the thermal gravimetric analyzer demonstrated its similar CO 2 adsorption capacity yet dramatical adsorption kinetics among some other microporous materials, e.g., potassium chabazite. These specific properties consequently guaranteed its favorable CO 2 adsorption capacity even at high temperatures (1.35 mmol/g at 393 K) and shortened the breakthrough time of single CO 2 flow to less than 20 s. In CO 2 /H 2 O binary breakthrough experiments, the as-obtained ETS-10 still maintained excellent CO 2 uptake of 0.81 mmol/g at 323 K, regardless of the presence of water vapor, making it a promising substitute for direct CO 2 separation from humid flue gases at practical conditions of post-combustion adsorption.
研究领域:
材料科学
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环境工程
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
J.Y. Yong,R.Y. Xie,Q. Huang,X.J. Zhang,B. Li,P.F. Xie,C.F. Wu,L. Jiang
Due to the superior CO 2 adsorption capacity and selectivity, amine-functional solid adsorbents have received increasing attention. Nevertheless, amine-functionalized polyporous materials have a large performance deviation when considering carbon removal capacity under wet flue gas. Therefore, a variety of metal–organic frameworks (MOFs) with amine functionality are synthesized in this work by appending diamine with a propylene linker to Mg 2 (dobpdc) (dobpdc 4- = 4,4′-dioxido-3,3′-biphenyldicarboxylate) and screened under the simulated flue gas environment with a high water content (7 v%). The results indicate that ndmpn-grafted Mg 2 (dobpdc) (ndmpn = N,N-dimethyl-1,3-propanediamine) has a high CO 2 adsorption capacity of 1.72 mmol/g at 60 °C with an extremely low regeneration heat (2.26 GJ/ton CO 2 at the desorption temperature of 145 °C). Adsorption property of ndmpn-Mg 2 (dobpdc) at high humidity is even more excellent than that of another well-reported diaminopropene-appended MOF, dmpn-Mg 2 (dobpdc) (dmpn = 2,2-dimethyl-1,3-propanediamine). Herein, van der Waals (vdW)-corrected density functional theory (DFT) calculations are used to quantitatively analyze binding strengths and water effects on it between diamine-appended Mg 2 (dobpdc) and CO 2 . It is revealed that the addition of water makes ammonium carbamate chains produced in ndmpn-Mg 2 (dobpdc) more stable. These chemisorption structures under humid conditions have also been disclosed by using 15 N solid-state nuclear magnetic resonance (NMR) spectroscopy experiments and DFT calculation. To conclude, we unveil the binary adsorption characteristics and mechanism of ndmpn-Mg 2 (dobpdc). It enables a thorough understanding of this compound and highlights its potential as a promising adsorbent under humid conditions for post-combustion applications.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
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IF 6.7
Xin-Yue Wang,Yi-Ming Gu,Xu-Peng Zong,Sheng-Sheng Zhao,Shu-Dong Wang
The inevitable combustion of fossil fuels in human industrial activities results in significant greenhouse gas emissions, leading to the pressing challenge of CO 2 /N 2 separation in humid flue gas. Iron-based Metal-organic frameworks (MOFs) have proven to be cheap, robust against water vapor attack due to the enhanced coordination bonds. In this study, we present two distinct MOFs i.e., DNL-9(Fe) and PCN-233(FeM II ), constructed by Fe clusters and 2,5-furandicarboxylic acid ligands. Static adsorption experiments revealed that DNL-9(Fe), featuring an exclusive Fe-F-Fe spiral packing structure, exhibited higher surface areas and enhanced CO 2 adsorption performance that outcompeted PCN-233 candidates. DNL-9(Fe) demonstrated a high IAST selectivity of CO 2 /N 2 at 247 (15/85, v/v, P/P 0 = 0.01), superior to the most of state-of-the-art Fe-MOFs reported up to date. The further theoretical calculations elucidated the binding sites of the framework with CO 2 molecules. Importantly, DNL-9(Fe) showed sufficient water stability and cyclic separation, as confirmed by dynamic breakthrough tests, indicating it as a promising candidate for practical CO 2 capture from humid flue gas.
研究领域:
化学
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材料科学
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环境科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）