CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Zhen-Jie Yu,Hao-Nan Li,Kexin Man,Jia-Hui Xin,Chao Zhang,Zhi-Kang Xu
Holey graphene oxide nanosheets enables uniform hydrogel filling in lamellar membranes • Metal ions densify gel network to increase selectivity and facilitate CO 2 transport • Zn 2+ balances CO 2 adsorption and desorption for rapid transport • Optimized membranes achieve CO 2 permeance of 27 GPU and CO 2 /CH 4 selectivity of 142 • The metal-ion regulation strategy demonstrates general applicability Exploiting efficient CO 2 /CH 4 separation membranes has emerged as indispensable platform for natural gas upgrading. Two-dimensional lamellar membranes offer immense opportunities in boosting CO 2 /CH 4 separation performance by introducing polar groups as facilitated transport carriers capable of forming strong interactions with CO 2 . Nevertheless, these lamellar membranes are largely restricted by inferior CO 2 /CH 4 selectivity of below 100, owing to the lack of efficient facilitated transport carriers to distinguish comparable kinetic diameter and polarizability of two gases. Herein, we bypass conventional carriers and discover a powerful and universal transition metal ion-modulated strategy to formulate holey graphene oxide/hydrogel lamellar membranes, rendering exceptional CO 2 /CH 4 selectivity over previously-reported lamellar membranes. In our strategy, transition metal ions play dual functions: performing high-efficient and tailorable CO 2 carriers via π-complexation for sustaining rapid permeance; and densifying hydrogel network within nanochannels via coordination for improving selectivity. By regulating the type and concentration of transition metal ions, our lamellar membranes yield a considerable CO 2 permeance of 27 GPU and a superior CO 2 /CH 4 selectivity of 142, which is about 3.7-folds of that without transition metal ions. This approach is broadly applicable to various metal ions, offering a paradigm shift in exploiting new lamellar membranes towards specific gas separation and beyond. Download: Download high-res image (187KB) Download: Download full-size image
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Yuchen Zhang,Xiaowei Zhou,ManMan Huo,Junfen Li,Yanfang Fan,Rong Zhang,Nanwen Li
Evaporation-rate control regulates kinetic trapping during polyimide membrane formation. • Stronger kinetic trapping preserves loosely packed nonequilibrium chain configurations with increased free volume. • Decarboxylative cross-linking amplifies structural gains, enhancing CO 2 permeability with modest selectivity loss. • This simple processing strategy improves CO 2 /CH 4 separation without polymer-backbone redesign or additional reagents. Kinetic trapping, the arrest of polymer chains in non-equilibrium configurations during rapid solvent evaporation, provides a deliberate route to engineer free-volume architecture in gas separation membranes. By controlling the solvent evaporation rate through casting temperature, faster evaporation from two solvents of contrasting volatility (DMAc and THF) systematically traps 6FDA-TFDB-DABA polyimide chains in more loosely packed configurations. This produces enlarged free volume, evidenced by expanded interchain spacing (5.33 to 5.49 Å, DMAc; 5.40 to 5.58 Å, THF), decreased density, enhanced birefringence, and increased surface roughness. This looser chain packing contributes to a substantial increase in CO₂ permeability, from 25.7 to 41.1 Barrer for DMAc-cast membranes and from 33.8 to 49.0 Barrer for THF-cast membranes, corresponding to increases of approximately 60% and 45%, respectively. These permeability gains arise from concurrent improvements in both CO₂ diffusivity and solubility, while the CO₂/CH₄ selectivity decreases only modestly. After thermal decarboxylation cross-linking at 340 °C, the rapidly evaporated THF-based membrane reaches 89.9 Barrer and surpasses the 1991 Robeson upper bound, withstanding feed pressures up to 600 psi without plasticization. This kinetic-trapping strategy requires no new reagents, monomer synthesis, or complex processing, offering a scalable, industrially compatible route to high-performance polyimide gas-separation membranes. Download: Download high-res image (280KB) Download: Download full-size image
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120850
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IF 7.2
Xiaohua Tong,Enyang Zhang,Guangran Shao,Ming Yuan,Boyi Song,Wangqing Zhang
Polymer blending is a simple and cost-effective method to improve the gas separation performance of polyimide membranes, thereby potentially overcoming the inherent permeability/selectivity trade-off effect. However, its application still faces challenges, since only a few polymers are miscible with polyimides, and the mechanical property of the membranes usually reduces significantly after polymer blending. Herein, we prepare membranes by blending polyimide containing bulky isopropyl substituents with a small amount of polar polymers such as polyacrylonitrile (PAN). The resultant blend membranes using PAN as additive not only possess excellent gas separation performance but also maintain good mechanical property. For example, when 0.8 wt% PAN is added, the corresponding blend membrane displays a high CO 2 permeability of 632.2 Barrer and a high CO 2 /CH 4 selectivity of 23.4 under humidified condition, close to the 2008 Robeson upper bound, which is attributed to the formation of micro-phase separation structure within the blend membranes. Moreover, the tensile strength of the blend membranes using 0.8 wt% PAN as additive is only 12 % lower than that of the pure polyimide membrane. In addition, the blend membranes using PAN as additive show remarkable stability against physical aging and outstanding long-term operation stability, suggesting their great prospect for natural gas purification and biogas upgrading.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
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IF 3.764
Xiaonan Zhao,Wei Liu,Xiufeng Liu,Baoquan Zhang
Mixed matrix membranes (MMMs) are challenged by the poor compatibility between fillers and a polymer matrix that leads to the weakened performance for gas separation. The surface modification of fillers with aminosilane should be an effective approach to improve their compatibility within the polymer matrix. 3-(2-Aminoethylamino)propyl-dimethoxymethylsilane (APDS) was used as a silane coupling agent for modification of sheet-like silicoaluminophosphate-34 (SAPO-34) crystal grains, and novel MMMs were fabricated by incorporating APDS-modified SAPO-34 crystal grains into a Pebax MH 1657 polymer. Based on characterization using scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, and mechanical tests, the incorporation of an APDS-modified SAPO-34 into Pebax matrix led to much enhanced interfacial adhesion within the MMM. In addition, the effect of the filler content in the MMM on the separation performance of a CO2/CH4 gas mixture and pure gases (CO2 and CH4) was investigated. Compared with available Pebax-based MMMs in the literature, the prepared MMM containing 8 wt % APDS-modified SAPO-34 exhibited the satisfactory CO2 permeability of ca. 137 Barrer and the highest selectivity of 34.7 for the CO2/CH4 gas mixture. It was believed that the excellent separation performance and good stability of the prepared MMM in this study should be due to the good interfacial compatibility of APDS–SAPO-34 fillers together with their strong affinity for CO2 within the MMM.
研究领域:
材料科学
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化学工程
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膜技术
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高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
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2020
·Vol. 138
·期 20
·50424
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IF 2.52
Junfeng Qian,Tingting Wu,Jianqun Shi,Hao Chang,Donghui Liu,Yichang Pan
Membrane-based technology is an attractive alternative in terms of CO 2 separation. Pebax-based membranes are regarded as potential candidates for CO 2 separation due to the favorable interaction between its poly (ethylene oxide) chains with CO 2 molecules and inorganic fillers. However, the separation performance for CO 2 /CH 4 mixture is still suffered from the moderate gas permeability and selectivity. To overcome this problem, in this work, amino-functionalized zeolite imidazolate framework (ZIF-7-NH 2 ) nanocrystals were used as fillers to blend with Pebax 1657 for fabricating mixed-matrix membranes (MMMs). XRD, Brunauer–Emmett–Teller (BET), scanning electron microscope, and 1 H nuclear magnetic resonance characterization indicated that ZIF-7-NH 2 with the highest crystallinity was synthesized. Fourier transform infrared spectroscopy, thermogravimetric analysis, differential scanning calorimetry (DSC), and Young's modulus showed that it has good interfacial interaction. Gas separation test results showed that both the CO 2 permeability and CO 2 /CH 4 selectivity of the 31 wt% ZIF-7-NH 2 /Pebax MMMs increased by 80 and 170%, respectively. The improved performance is attributed to the addition of ZIF-7-NH 2 nanocrystals and the favorable interfacial interactions between the polymer and ZIF-7-NH 2 nanocrystals. Furthermore, the polyvinylidene fluoride supported hollow fiber composite membranes also exhibit the long-term stability for CO 2 /CH 4 separation.
研究领域:
材料科学
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化学工程
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高影响因子
Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 15
·4519-4525
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IF 7
Chaoran Wang,Xiao Li,Shiyue Liu,Tingting Wang,Puxu Liu,Xiaowei Song,Zhiqiang Liang
Silicoaluminophosphate (SAPO) zeolites with small pores (8-ring window), such as SAPO-34, SAPO-17, and SAPO-RHO, have attracted a lot of attention due to their unique structural features, and their applications in the field of small-molecule gas adsorption and separation. However, the fast, efficient and green synthesis of SAPO zeolites remains a great challenge. In this work, SAPO-17 zeolites were synthesized within 1 min for the first time by a seed-assisted microwave method, and the resulting samples possessed excellent performance in the application of CO2 adsorption and separation for flue gas and natural gas. The microwave-assisted route can shorten the crystallization time of traditional hydrothermal methods from a few hours to 30 min. Furthermore, the crystallization time could be drastically shortened to 1 min with the addition of seeds, which represents the shortest time for the preparation of a SAPO-17 zeolite up to now. SAPO-17 synthesized within 1 min (SAPO-17-S-1) possessed the smallest crystal size, and the largest micropore volume and specific surface area among all the samples, which enhanced mass transfer and exposed more active sites, and thus it possessed prominent performance for CO2 adsorption (3.47 mmol g−1 at 273 K and 1 bar) and gas separation. At 298 K and 100 kPa, SAPO-17-S-1 exhibited the highest gas selectivity for CO2/N2 (276) and CO2/CH4 (63) over the other samples, which were synthesized in a relatively long time. Transient binary breakthrough experiments on SAPO-17-S-1 further verified the highly-efficient gas separation performance. This work proposes a green and ultrafast strategy for the synthesis of SAPO-17 zeolites with highly selective CO2 adsorption over N2 and CH4.
研究领域:
材料科学
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环境科学
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化学工程
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Yuke Zhang,Yi Huang,Shangqing Chen,Lijuan Shi,Jiancheng Wang,Qun Yi,Feng Pei
The high-efficiency capture of CO 2 from biogas by adsorption is highly desirable, which, yet faces the challenges regards of the unsatisfactory adsorption efficiency, selectivity, and regeneration performance. Herein, ionic ultramicroporous metal organic frameworks (IUM-MOFs) with high CO 2 affinity are constructed by one-step in-situ coordination strategy and used for CO 2 /CH 4 separation. The phenoxylate anion-functionalized ionic liquid (FIL) serves as competitive ligands in the formation of IUM-MOFs. The oxyl group exhibits high affinity with CO 2 as the Lewis basic center, while the rigid counterion occupies the adsorption space of CH 4 in the cavities of IUM-MOFs, thus bringing about superior CO 2 adsorption capacity of 149 cm 3 g −1 (150% higher than that of Cu-BTC) and high IAST predicted selectivity with CH 4 of 22 under atmospheric condition. Mechanism analysis demonstrated that the formation of hydrogen bonds between CO 2 with coordinated IL and H 2 O and IL-enhanced polarity of MOFs benefit to the CO 2 adsorption. In addition, the IUM-MOFs could be facilely regenerated at 120 °C with favorable recycling stability. This work provides facile strategy for the rational design of IUM-MOFs and lays useful insights for structural tuning to promote their applications.
研究领域:
材料科学
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环境科学
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高影响因子
JOURNAL OF POROUS MATERIALS
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2025
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IF 3.2
Qian Yi,Jiang Qingqing,Xiang Shimeng,Lu Zhenhao,Xu Xiaowen,Yang Jing,Dai Guoliang,Song Ruifeng,Jiang Ji
Separating CO 2 and N 2 from CH 4 is crucial for energy production and environmental protection. This study showed the rapid synthesis of CHA zeolites with different morphologies using an in situ growth method, without the assistance of organic structure directing agents (OSDA) or fluoride media. The crystallization behavior of CHA zeolites was studied in terms of synthesis gel composition (including water content, silicon and aluminum content, alkalinity and Sr 2+ concentration), synthesis temperature and duration. The results suggested that pure phase CHA zeolite nano-aggregates could be synthesized with broad precursor conditions at 150 °C for only 4 h. Then, K-CHA zeolite was ion-exchanged to Na-CHA and Ca-CHA and the adsorption properties of CHA zeolites with different morphologies and ions were studied. The results suggested that Na-CHA exhibited highest CH 4 , CO 2 and N 2 adsorption capacity and showed higher ideal selectivity for N 2 /H 2 ; Although Ca-CHA zeolites exhibited relative lower CO 2 and CH 4 adsorption capacity, it exhibited the highest ideal selectivity for CO 2 /CH 4 ; Simultaneously, K-CHA zeolite exhibited high CH 4 adsorption capacity and high adsorption separation ability of CH 4 /N 2 . Furthermore, breakthrough experiments have confirmed the practical feasibility of separating CO 2 from CH 4 .
研究领域:
材料科学
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化学工程
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吸附与分离
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分子筛合成
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气体分离
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
·
IF 9.1
Ke Chen,Ruishan Li,Chengming Xiao,Xin Guo,Junwen Qi,Jiansheng Li
Efficient gas separation is essential for sustainable energy generation and industrial applications; however, membrane materials often encounter an intrinsic trade-off between permeability and selectivity. In this work, we overcome this limitation by incorporating phenolate-based metal-organic frameworks (termed as SU-102) into polyimides (6FDA-Durene) via a physical blending method. Attributable to the strong CO 2 affinity, significant porosity, and distinctive pore size of SU-102, the resulting mixed matrix membranes (MMMs) demonstrate a synergistic enhancement in both CO 2 permeability and selectivity. Specifically, MMMs with 30 wt% SU-102 amounts achieved a CO 2 /CH 4 selectivity of 33.6 and a CO 2 permeability of 1572.3 Barrer, representing increases by 1.8 and 2.2 times, respectively, compared to the pristine 6FDA-Durene membranes. Furthermore, the MMMs exhibited remarkable long-term stability over 72 h of continuous operation. Importantly, hydrogen-bonding interactions between the carboxyl and hydroxyl groups on SU-102 and the imide groups on 6FDA-Durene significantly enhanced the plasticization resistance of the MMMs, which withstood CO 2 pressures up to 12 bar. This work provides a feasible strategy for the design of high-performance gas separation membranes for practical applications.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2020
·
IF 4.551
Junjie Zhou,Hao Liu,Yichao Lin,Chen Zhou,Aisheng Huang
A well-shaped Ce (IV)-based metal organic framework (Ce-BDC) is prepared under solvothermal method. The influence of synthesis time, temperature and the amount of acetic acid (HAc) as a modulator is studied to develop a new strategy for the synthesis of well-shaped Ce-based MOF. The relationship between the synthesis parameters and morphology as well as crystallinity of Ce-BDC is investigated by XRD and SEM. Furthermore, the obtained well-shaped Ce-BDC shows a CO 2 uptake capacity of 2.28 mmol g −1 at 0 °C and 1.0 bar. Meanwhile, the breakthrough curve behaviors of Ce-BDC are investigated for a CO 2 /CH 4 and CO 2 /N 2 mixture gas . It is found that the Ce-based MOF adsorbs CO 2 under ambient temperature and pressure, but completely excludes CH 4 and N 2 , suggesting that it is a promising adsorbent for efficient separation of CO 2 from natural gas.
研究领域:
材料科学
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无机化学
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多孔材料
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气体分离
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环境催化
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DOI
高影响因子
PETROLEUM CHEMISTRY
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2025
·
IF 1.1
Jiang Ning,Mao Min,Wang Qingyin,Wang Gongying
MOF-5 is a classic metal-organic framework (MOF) crystal. However, synthesis of high-quality crystals usually requires an expensive N , N ′-diethylformamide (DEF) solvent, and a high molar ratio of a raw material (Zn 2+ : BDC 2– = 3‒5 : 1). More critically, its extreme instability against water vapor has caused researchers to do not use it. In this study, we achieved some important breakthroughs by using inexpensive N , N ′-dimethylformamide (DMF) solvent and meticulously optimizing synthesis parameters combined with a specialized micro-open solvothermal method. With a reduced molar ratio of a raw material (1.47 : 1), we successfully synthesized crystals exhibiting excellent phase structure and morphology, high surface area, out standing water vapor stability, and strong CO 2 adsorption capacity. The results show that the DEF replacement with DMF and reduction of the raw material molar ratio from 3 : 1 to 1.47 : 1 provides an increase of the BET surface area from ~935 to 2388 m 2 /g, and an improvement of the CO 2 adsorption capacity from ~0.8 to 2.5 mmol/g (298 K, 100 kPa). Breakthrough curves reveal that in simulated separation experiments for the flue gas and natural gas containing low CO 2 concentrations (10‒20%), the dynamic separation selectivity for CO 2 /N 2 reaches 22, while that for CO 2 /CH 4 remains stable at 4. Notably, the selectivity remained nearly unaffected by the pressure variation; this phenomenon is promising for enhancing the capture and purification of a low-concentration CO 2 from the flue gas and natural gas. It is important that the improved MOF-5 crystals prepared under optimal synthetic conditions maintained the stable phase structure and morphology even after 14-day exposure to humid air (relative humidity >70%), successfully overcoming the challenge posed by a water vapor.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zucheng Cheng,Weiguo Liu,Shaohua Li,Sijia Wang,Yingying Liu,Xiang Sun,Cong Chen,Lanlan Jiang,Yongchen Song
Hydrate technology with high gas storage capacity and excellent safety features has attracted much attention for capturing CO 2 from biogas to produce purified CH 4 . When considering operational efficiency, it is desirable to overcome technical barriers such as slow hydrate generation and low separation efficiency. Therefore, based on the properties of surfactant-enhanced hydrate generation kinetics, this work first systematically evaluated the performance of 500 ppm SDS on the separation efficiency of 40 mol% CO 2 and 60 mol% CH 4 simulated biogas. The experimental results show a significant increase in gas capture at higher driving forces, with the rise being dominated by the CH 4 component, indicating that larger driving forces reduce hydrate selectivity to CO 2 -CH 4 and weaken gas separation efficiency, with a maximum CO 2 recovery of 84.24 ± 1.19% at 275.15 K and 8 MPa. Interestingly, hydrate growth mainly occurred in the liquid phase, leading to the separation factor being positively correlated with the induction time with sufficient CO 2 dissolution. In comparison, the gas capture per unit volume of solution could be improved by more than a factor of 2 at higher gas–liquid ratios. The best separation factor of 7.84 ± 0.73 was achieved, and separation factors in general gradually decreased with increasing gas–liquid ratio; however, there was high-pressure failure behavior. Furthermore, the impact of the defoamer on separation efficiency was deeply investigated for SDS decomposition foaming, with results showing that the defoamer would alleviate hydrate decomposition foaming behaviour while having no significant effect on hydrate generation kinetics and separation efficiency.
研究领域:
能源工程
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环境科学
·
化学工程
·
气体分离技术
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DOI
高影响因子
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