PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2024
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IF 6.9
You-yun Gong,Zi-ang Jia,Yiwen Fan,Jin-ping Cheng
Rational chemical modification engineering of metal-organic frameworks (MOFs) is an effective means to improve their CO 2 capture efficiency. In this study, we prepare UiO-66 MOF impregnated with different types of aliphatic amines using solvothermal and impregnation techniques, respectively, and investigated their performances in CO 2 adsorption and CO 2 /N 2 separation using the isothermal adsorption method. Aliphatic amines successfully chemically modifies UiO-66, and their molecules effectively occupied the pores of the UiO-66 framework, which has been confirmed by material characterization, experiments, and DFT-FMO calculations. There are significant improvements in the ability to capture CO 2 when aliphatic amines were added to UiO-66 compared to pure UiO-66 (1.39 mmol/g up to 2.11 mmol/g-2.53 mmol/g), attributed to the different types and numbers of amines, and there were also differences in the Zr metal clusters and BDC ligands. Meanwhile, The material has better CO 2 /N 2 adsorption IAST selectivity(98) because its surface area is changed and N 2 does not interact specifically with the adsorbent. Furthermore, the CO 2 adsorption capacity remains constant across multiple adsorption cycles, highlighting the adsorbent's stability and reliability during repetitive CO 2 capture. This study provides new ideas and perspectives for improving the CO 2 capture efficiency of UiO-66.
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高影响因子
APPLIED CLAY SCIENCE
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2024
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IF 5.3
Xiaoyu Li,Kang Peng,Xueqi Zhao,Keping Zhao,Haoran Li,Yanrong Zhao,Bo Zhang
Amine-functionalized mesoporous silica is considered as one of the most promising solid amine adsorbents for post-combustion carbon dioxide (CO 2 ) capture due to their high specific surface area, large pore volume and adjustable pore structure . However, the high costs associated with silica precursors and synthesis techniques of amine-functionalized mesoporous silica have extremely limited their practical applications. In this work, a facile and feasible approach was proposed to construct polyethyleneimine (PEI)-impregnated of Al-MCM-41 derived from natural flake-like kaolinite (FK) clay. The effect of PEI loadings and adsorption temperature on CO 2 uptakes, adsorption/desorption kinetics and stability for Al-MCM-41/PEI x adsorbents were specifically discussed. The optimal Al-MCM-41/PEI (AP30) adsorbent exhibited a high CO 2 uptake of 1.27 mmol/g at 75 °C and stable cyclic stability with a mere 1.1% decline per cycle over 10 adsorption-regeneration cycles, resulting from the unique ordered porous structure and spatial confinement effect of as-prepared Al-MCM-41 support to suppress excess PEI agglomeration and avoid blocking CO 2 adsorption in the resultant adsorbents. The good PEI dispersions provided abundant CO 2 affinity sites, which is beneficial to efficient CO 2 diffusion and adsorption, and thus greatly improving the CO 2 capture performances. This approach has enormous potential for cost-effective large-scale practical applications for CO 2 capture and separation processes.
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JOURNAL OF MOLECULAR STRUCTURE
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2024
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IF 4
Miao Jiang,Peng-Li Zhao,Yong-Ning Yue,Xue-Qin Song,Li Wang
With the acceleration of industrialization and energy consumption, global concerns for the safety of ecological system and sequent human health have attracted consideration attention increasingly in view of the severe contamination both in aqueous environment and aerosphere. Therefore, the development of multifunctional species for efficient adsorption of pollutants and chemical fixation of CO 2 receives increasing attention. Herein, an anionic Er III metal organic framework ( Er-MOF ) with large hexagonal channels, is obtained based on a benzene-spaced tetracarboxylate ligand, H 4 L (H 4 L = 1,4-bis(2′,2′′,6′,6′′-tetracarboxy-1,4′:4,4′′-pyridyl) benzene). Adsorption analysis indicates that Er-MOF behaves as an excellent adsorbent for selectively absorbing MB in water with a maximum adsorption capacity of 494.1 mg·g ‒1 . The adsorption mechanism could be a combination of size matching, electrostatic interaction, π···π stacking and hydrogen bonding. In addition, Er-MOF is demonstrated to be an efficient catalyst in the cycloaddition of CO 2 with epoxides under mild conditions due to its excellent stability, substantial specific surface area, confined space and well-exposed Lewis acid/base sites. The findings presented herein had great significance for enriching the multifunctional lanthanide MOFs in environmental applications.
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Nature Communications
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2024
·Vol. 15
·期 1
·1-13
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IF 14.7
Liu Qinglu,Tang Tang,Tian Ziyu,Ding Shiwen,Wang Linqin,Chen Dexin,Wang Zhiwei,Zheng Wentao,Lee Husileng,Lu Xingyu,Miao Xiaohe,Liu Lin,Sun Licheng
Ion-solvating membranes have been gaining increasing attention as core components of electrochemical energy conversion and storage devices. However, the development of ion-solvating membranes with low ion resistance and high ion selectivity still poses challenges. In order to propose an effective strategy for high-performance ion-solvating membranes, this study conducted a comprehensive investigation on watermelon skin membranes through a combination of experimental research and molecular dynamics simulation. The micropores and continuous hydrogen-bonding networks constructed by the synergistic effect of cellulose fiber and pectin enable the hypodermis of watermelon skin membranes to have a high ion conductivity of 282.3 mS cm −1 (room temperature, saturated with 1 M KOH). The negatively charged groups and hydroxyl groups on the microporous channels increase the formate penetration resistance of watermelon skin membranes in contrast to commercially available membranes, and this is crucial for CO 2 electroreduction. Therefore, the confinement of proton donors and negatively charged groups within three-dimensional microporous polymers gives inspiration for the design of high-performance ion-solvating membranes.
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PubMed
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2011
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IF 2.089
Jun Li,Yinmei Ye,Lifang Chen,Zhiwen Qi
The solubilities of CO2 in solvent poly(ethylene glycols) (PEGs) with molecular weights of 150, 200, 300, and 400 were measured over the range of pressure from (100 to 1200) kPa and temperature from (303.15 to 333.15) K. Henry's constant was obtained by linear fitting of the experimental data, and thermodynamic properties of solutions were calculated from the correlation of Henry's constant. It indicates that the solubility of CO2 increases with increasing molecular weights of PEGs. Henry's constant based on mole fraction and the molality of CO2 in PEG400 vary from (4.78 to 7.09) MPa and (1.56 to 2.48) MPa·kg·mol–1 from (303.15 to 333.15) K, respectively.
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ChemNanoMat
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2017
·Vol. 3
·期 8
·560-568
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IF 2.937
Xinglong Pan,Jianqiang Zhang,Qingzhong Xue,Xiaofang Li,Degong Ding,Lei Zhu,Tianchao Guo
Graphical As a novel filler , 1 D multi-walled carbon nanotube/graphene oxide nanoribbons (MWCNT@GONRs) with low oxidation degree can enhance the gas-separation performance of mixed matrix membranes (MMMs) due to the synergistic effect of the MWCNTs core and GONRs shell. 1 D multi-walled carbon nanotube/graphene oxide nanoribbon (MWCNT@GONRs) hybrids were prepared using a chemical method as fillers for Pebax-based mixed matrix membranes (MMMs) with excellent CO 2 separation performance. Herein, the GONRs shell provided a selective barrier and large gas adsorption area, which contributed to enhancement of gas selectivity, while MWCNTs core with smooth internal surface acted as a rapid transport channel, which improved the gas permeability. It is found that MMMs with 1 wt % loading showed the highest separation factor (80 for CO 2 /N 2 and 23 for CO 2 /CH 4 ) and high CO 2 permeability, far surpassing the upper bound line. Therefore, the synergistic effect of the MWCNTs core and GONRs shell in MWCNT@GONRs nanohybrids can effectively enhance the gas-separation performance of MMMs at low loading. The unique microstructures, ease of synthesis and low filled loading make MWCNT@GONRs promising candidates in post-combustion and sustainable chemistry.
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C-Journal of Carbon Research
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2024
·Vol. 10
·期 3
·62
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IF 3.9
Xuexin Yuan,Qiqi Zhou,Yu Chen,Hai-Jian Yang,Qingqing Jiang,Juncheng Hu,Cun-Yue Guo
In the present work, inexpensive and commercially available diethyltriamine pentaacetic acid (DTPA) was used as an initiator to catalyze the N-formylation reaction of CO2with amines via the construction of C-N bonds in the presence of xanthone as the photosensitizer and PhSiH3as the reducing agent. After a systematic study of various factors, the optimal conditions for the photocatalytic reaction were obtained: 2.5 mmol of amine, 2.5 mmol of PhSiH3, 10 mol% of DTPA, 20 mol% of xanthone, 1 mL of dimethylsulfoxide (DMSO), atmospheric pressure, and 35 W UV lamp irradiation for 48 h. Under the optimal conditions, the catalyst system afforded high performance for the N-formylation of amines (primary and secondary amines) and CO2, and the yields of the N-formylated products of dialkylamines were above 70%. Further studies exhibit that the catalytic system has a wide scope of substrate applications. For various alicyclic secondary amines, heterocyclic secondary amines, aliphatic primary amines, and aromatic primary amines, the corresponding N-formylation products can be obtained efficiently. In addition, the catalyst can be recycled by simple precipitation and filtration. After five cycles of recycling, there was no significant change in the catalytic and structural properties of DTPA. Finally, a possible reaction mechanism is proposed.
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Gels
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2024
·Vol. 10
·期 7
·449
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IF 5
Huipeng Wang,Changhua Yang,Yongwei Zhang,Chen Wang
In order to solve the problem of gas channeling during CO2flooding in low-permeability reservoirs, a novel CO2responsive gel channeling system was prepared by using carrageenan, branched polyethylene imide and ethylenediamine under laboratory conditions. Based on the Box–Behnken response surface design method, the optimal synthesis concentration of the system was 0.5 wt% carrageenan, 2.5 wt% branchized polyethylenimide and 6.5 wt% ethylenediamine. The micromorphology of the system before and after response was characterized by scanning electron microscopy. The rheology and dehydration rate were tested under different conditions. The channeling performance and enhanced oil recovery effect of the gel system were simulated by a core displacement experiment. The experimental results show that the internal structure of the system changes from a disordered, smooth and loosely separated lamellae structure to a more uniform, complete and orderly three-dimensional network structure after exposure to CO2. The viscosity of the system was similar to aqueous solution before contact with CO2and showed viscoelastic solid properties after contact with CO2. The experiment employing dehydration rates at different temperatures showed that the internal structure of the gel would change at a high temperature, but the gel system had a certain self-healing ability. The results of the displacement experiment show that the plugging rate of the gel system is stable at 85.32% after CO2contact, and the recovery rate is increased by 17.06%, which provides an important guide for the development of low-permeability reservoirs.
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JOURNAL OF POLYMER SCIENCE
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2024
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IF 3.9
Xin Luo,Zhuqing Wang,Mengxia Yan,Jianhui Xin,Yongqi Yang,Longpo Zheng,Haijun Zhang
CO 2 -responsive based separation membranes are attractive in the field of membrane separation, not only for their ability to modulate the pore size of the membrane in response to CO 2 stimulation, but also for their ability to facilitate the removal of contaminants from the membrane surface. However, the introduction of CO 2 -responsive polymers by simple blending often results in membranes that are not responsive enough to last. In this study, we synthesized a hooked triblock copolymer and used it as an additive to prepare CO 2 -responsive PVDF membranes. The modified membrane combines the advantages of the PVDF material with the CO 2 response of the triblock copolymer. It not only has good CO 2 responsiveness, but also removes organic contaminants from the membrane surface well. The water flux of the hybrid membranes is 4 to 11 times higher than that of pure PVDF membranes, indicating that the triblock copolymer also has some porogenic ability. Surprisingly, the static contact angle on the membrane surface increased from 67° to 86° with the increase of the triblock copolymer content in the PVDF membrane. This suggests that modified PVDF membranes have some potential in the field of switchable oil–water separation. Graphical
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JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Jing Fan,Xin Zhang,Nan He,Fenhong Song,Xiwu Zhang
Due to the advantages of deep eutectic solvents (DESs), such as good CO 2 absorption performance, excellent biodegradability, low cost, and simple synthesis, attention has been drawn to selecting DESs with high efficiency for capturing CO 2 in a green and environmentally compatible context. In the present study, acetamide as the hydrogen bond acceptor (HBA) and diethylene glycol, 1,2-propanediol, and 1,3-propanediol as the hydrogen bond donors (HBD) for the synthesis of DESs. First, the density and viscosity of these prepared DESs were measured under standard ambient pressure and at temperatures ranging between 293 K and 343 K. Subsequently, the CO 2 solubility in DESs was ascertained by the isovolumetric saturation experimental method. The results indicated that all synthesized DESs exhibited physical absorption of CO 2 and the diethylene glycol-based DESs had the highest dissolvability for CO 2 . For the DES with diethylene glycol and 1,2-propanediol as HBD, the CO 2 solubility increased as the molar ratio of HBD decreased. On the contrary, the amount of CO 2 adsorbed by 1,3-propanediol-based DES increased with increasing 1,3-propanediol content. The semi-empirical Jou and Mather model allows for an efficient correlation to be made among experimentally determined CO 2 solubilities, temperatures, and the CO 2 partial pressures. Comparing the deviations between the experimental and fitted values, the average relative deviation is small. By estimating the Henry constants and Manuscript File Click here to view linked References comparing them with the literature, it was demonstrated that the synthesized DESs are competitive in absorbing CO 2 .
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Panpan Wang,Meiyu Shi,Yuan Shu,Qiang Niu,Pengfei Zhang
Daily discarded egg residues such as eggshells reach an astronomical figure around the world, causing severe environmental pollution and waste of Ca-based sources. CaCO 3 , especially these porous CaCO 3 nanoparticles, could role as an effective plastic stuffing, filler, ink filler, and adsorbent, having a great prospect for industrial application. Herein, based on a solid-state reaction between strong and weak acids, we successfully prepared a porous CaCO 3 -es with the BET specific surface area (SSA) up to 97.4 m 2 /g, and meanwhile with abundant mesopores and tiny small CaCO 3 primary nanoparticles about 7.4 nm. Notably, the prepared CaCO 3 -es showed significantly improved CO 2 adsorption capacity than the contrast CaCO 3 samples in both static and breakthrough tests. According to the characterization such as FTIR, Raman, XPS, TEM, and DFT calculations, the high CO 2 adsorption of CaCO 3 -es originated from its high porous structure, small nanoparticle size, and rich defective sites.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Bin Liu,Yanan Yu,Zijian Liu,Zhe Cui,Wende Tian
In this study, a quantitative structure–property relationship (QSPR) model has been designed based on machine learning (ML) to offer a new method to accurately predict carbon dioxide (CO 2 ) solubility in aqueous amine solutions. Molecular descriptors are used to denote representative features of the amine molecular structure supplemented with amine solution concentration, CO 2 partial pressure, and temperature as inputs to the model. The coefficient of determination ( R 2 ) of the well-trained ML model reaches 0.971, and the average absolute deviation (AAD) of independent experimental validation is 4.785 %, effectively demonstrating the model’s reliability and generalization performance. Finally, SHapley Additive exPlanations (SHAP) is adopted to reveal the contribution of different features to the model predictions, making the model more transparent and interpretable. Overall work provides a novel, low-cost, efficient method to predict equilibrium CO 2 solubility in aqueous amine solution and offers a new perspective in developing advanced amine for CO 2 capture.
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