INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2018
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IF 3.141
Daofei Lv,Renfeng Shi,Yongwei Chen,Yang Chen,Houxiao Wu,Xin Zhou,Hongxia Xi,Zhong Li,Qibin Xia
A water resistant zirconium–porphyrin metal–organic framework PCN-222 was synthesized for selectively separating CO2/CH4 and CO2/N2. Isotherms of CO2, CH4, and N2 on PCN-222 at low and high pressures were respectively measured. At 298 K, CO2 uptakes at 100 and 3000 kPa were 1.16 and 13.67 mmol/g, respectively. At 298 K and 100 kPa, CO2/CH4 (50:50, v/v) and CO2/N2 (50:50, v/v) adsorption selectivities separately reached 4.3 and 73.7. At 298 K and 3000 kPa, CO2/CH4 (50:50, v/v) and CO2/N2 (50:50, v/v) adsorption selectivities were 4.7 and 32.8, respectively. Importantly, breakthrough experiments confirmed that PCN-222 could achieve the effective separation of CO2/CH4 (both 50:50 and 10:90) and CO2/N2 (both 50:50 and 15:85) gas mixtures. The dynamic regeneration experiments showed that PCN-222 maintained its initial CO2 adsorption capacity after five cycles of CO2 adsorption–desorption. This work suggested that PCN-222 was a potential candidate for selectively separating CO2/N2 and CO2/CH4.
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2018
·Vol. 2018
·期 8
·1047-1052
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IF 2.507
Xiaoxia Jia,Ning Yuan,Li Wang,Jiangfeng Yang,Jinping Li
Graphical Both high selectivity and adsorption capacity in the adsorptive separation of CO 2 , CH 4 , and N 2 were achieved by means of (CH 3 ) 2 NH functionalization of the unsaturated metal sites of the MOF Ni-HKUST-1. Ni-HKUST-1, with the same topological structure as Cu-BTC (HKUST-1), was synthesized by a (CH 3 ) 2 NH-assisted method. Ni-HKUST-1 with high purity (> 90 %), yield (85 %), and BET surface area (1088 m 2 /g) was successfully synthesized for the first time by using NiCl 2 . The pure-component adsorption isotherms of CO 2 , CH 4 , and N 2 on Ni-HKUST-1 were measured by the volumetric method and the data used to estimate the separation selectivity for CO 2 /CH 4 , CH 4 /N 2 , and CO 2 /N 2 binary mixtures according to the ideal adsorbed solutions theory. At 273 K and 1 atm, the selectivities for CO 2 /CH 4 , CH 4 /N 2 , and CO 2 /N 2 were 14.49, 5.36, and 183.41, respectively, and the adsorption capacities for CO 2 and CH 4 were 223.87 and 67.89 cm 3 /g, respectively. This is a rare demonstration of both high selectivity and adsorption capacity in the separation of CO 2 , CH 4 , and N 2 .
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Xupeng Zhang,Kaiqian Li,Longxin Guo,Zhiping Xu,Shuduan Deng,Ying Liu,Gang Zhu
To effectively mitigate the global warming problem caused by excessive CO2 emissions, the implementation of direct air capture (DAC) technology has emerged as one of the most promising strategies for capturing CO2 from the atmosphere. The key to DAC technology hinges on the development of high-performance solid sorbent materials that demonstrate high CO2 adsorption capacity and gas separation selectivity, particularly under low CO2 partial pressure conditions. Herein, we have successfully developed a class of MOF@carboxylated wood sponge (MOF@CWS) hybrid sorbents, capable of efficient CO2 capture from low-concentration (less than 10,000 ppm) CO2 sources, achieved by embedding the porous MOF into carboxylated wood sponges (CWS) substrate via an in situ growth route. Within the MOF@CWS series, the CO2 uptake capacity of Mg-MOF-74@CWS is 3.61 and 2.65 mmol/g at 1 bar, 273 and 298 K, respectively, significantly higher than those of CWS and HKUST-1@CWS. Moreover, this material exhibited outstanding DAC performance, with the CO2 sorption capacity at 273 K up to 0.56 mmol/g from ambient air (ca. 400 ppm of CO2), surpassing most other solid sorbents. The obtained Mg-MOF-74@CWS also demonstrated exceptional CO2/CH4 separation performance, primarily due to the unique pore structure and augmented interaction between the CO2 molecules and the hybrid sorbents. The results of this study indicate that Mg-MOF-74@CWS has potential as an efficient solid sorbent for the DAC of CO2.
研究领域:
材料科学
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环境科学
·
化学工程
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MICROPOROUS AND MESOPOROUS MATERIALS
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2025
·
IF 4.7
Lili Gong,Ju Bai,Can Wang,Zhenyuan Li,Linglong Shan
Two-dimensional (2D) metal-organic framework (MOF) nanosheets are promising fillers for gas separation membranes, owing to their high aspect ratios and tunable pore architectures. Realizing their full application potential requires precise control over nanosheet morphology and sizes to optimize membrane performance. This work employs crystal growth kinetics modulation to tailor the morphology and size of ZIF-67-based nanosheets incorporated into mixed matrix membranes (MMMs) targeting superior CO 2 /CH 4 separation. Strategy (i): Adjusting early-stage nucleation kinetics yielded two distinct ZIF-L nanosheet types: disk-like (ZIF-L-I) and leaf-like (ZIF-L-II). ZIF-L-II, synthesized with higher ligand molar ratio, possessed larger lateral dimensions and more favorable pore characteristics, significantly enhancing gas separation. Strategy (ii): Amino-functionalized ionic liquid (IL) was introduced to further modulate the size of ZIF-L-II nanosheets. The IL's amino groups served as capping agents by coordinating preferentially with Co ions, restricting framework extension without altering crystallinity. The ILs loading amount dictated the final nanosheet size, but did not alter their crystalline phase. Critically, the IL also exhibits affinity for CO 2 , augmenting its transport. At 48 % IL addition, the CO 2 permeability of the 10 wt% IL-ZIF-L-II/PI membrane surged from 289 Barrer to 493 Barrer, without significant selectivity loss. The synergistic combination of kinetically-controlled synthesis (yielding larger and leaf-like nanosheets) and IL-mediated size regulation (providing both capping and CO 2 -philic functions) resulted in a 70 % enhancement in CO 2 permeability.
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POLYMER
·
2022
·
IF 4.432
Min Zhao,Caili Zhang,Yunxuan Weng,Pei Li
Thermal oxidative crosslinking results in the generation of oxygen bridges among polymer chains and helps regulate the membrane microstructure. Simultaneously, any strategy to increase the crosslinking sites of polyimide (PI) can improve the crosslinking efficiency and allow precise control of the pore structure of membranes. Phenolphthalein-based PIs are potentially suitable precursors for thermal oxidative crosslinking of membranes, since thermal treatment will result in the degradation of lactone ring leading to the generation of a pair of phenyl crosslinking sites. In this work, three phenolphthalein-based diamines with different structures were designed and synthesized. The three diamines were subsequently reacted with 3,3′,4,4′-benzophenone tetracarboxylic dianhydride (BTDA) to prepare phenolphthalein-based PIs. The original membranes were post-treated by thermal oxidation crosslinking at 400 °C and 425 °C, respectively; the lactone ring underwent decomposition, and the imide ring opened at the same time, resulting in the generation of multiple crosslinking sites and correspondingly improving the crosslinking efficiency. The effect of the side groups (−CH 3 , –CF 3 or unsubstituted) of phenolphthalein-based diamine and thermal treatment temperatures on the gas separation performance of phenolphthalein-based PI membranes were investigated. Wide-angle X-ray diffractometry (WAXD) and wide-angle X-ray scattering (WAXS) analysis demonstrated that the π-π stacking distance were improved. BTDA-FPP-425 had a CO 2 /CH 4 selectivity of 37.68. This thermal degradation along with thermal oxidative crosslinking strategy provides a promising approach for fabrication of CO 2 /CH 4 separation membrane .
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Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 47
·24975-24984
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IF 14.511
Lili Gong,Zhili Cai,Qi Wu,Lu Liu,Can Wang,Linglong Shan,Xianghai Meng,Shuangjiang Luo,Zhichang Liu,Suojiang Zhang
Mixed matrix membranes (MMMs) are highly promising for natural gas sweetening due to their high microporosity and outstanding gas separation performance. However, MMMs are frequently challenged by the polymer/filler interfacial incompatibility, leading to the deterioration of gas separation performance. In this study, the mixed-linker ZIF-7-8 was employed as a filler by finely tuning the molecular sieving for CO2/CH4 separation. An amino-functionalized ionic liquid ([C3NH2Mim][Cl]) was introduced for constructing the interface connection between the ZIF-7-8 filler and polymer matrix through coordination and hydrogen bonding, which was verified by extended X-ray absorption fine structure (EXAFS) and electron paramagnetic resonance (EPR). The design of interface interaction through an IL is crucial to improve the interface compatibility and the CO2/CH4 separation performance. The newly developed 20% ZIF-7-8-IL (1%)/PI and 25% ZIF-7-8-IL (1%)/PI MMMs displayed a dramatic improvement of CO2 permeability by 244.2% and 291.6%, from 308 to 1060 and 1206 barrer, respectively, for pure-gas separation, compared to the pristine polyimide matrix. Moreover, the 25% ZIF-7-8-IL (1%)/PI MMM also demonstrated outstanding low-temperature mixed-gas CO2/CH4 separation performance in the temperature range of −45–35 °C, far beyond the 2018 mixed-gas CO2/CH4 upper bound.
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ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Peng Hu,Hao Wang,Chao Xiong,Hao Liu,Jun Han,Jie Zhou,Zhenxia Zhao,Yongqing Wang,Hongbing Ji
We demonstrate a novel microwave-assisted strategy to in situ functionalize the node chemistry of Zr-based metal–organic frameworks (Zr-MOFs) with a 2-aminobenzimidazole (2-AMI) agent. The novel strategy can concomitantly weaken the Lewis acidity of Zr6O8 nodes of Zr-MOFs through bonding with 2-AMI, contributing to admirable surface hydrophobicity with an ultrahigh water contact angle of 151.7° and enhanced stability. The successful coordination process was jointly verified by thermogravimetry analysis, 1H nuclear magnetic resonance spectroscopy , and X-ray photoelectron spectroscopy analyses. Meanwhile, the tailor-made pore microenvironment enabled highly efficient CO2/CH4 separation via a synergetic equilibrium-kinetic effect. Gas adsorption isotherms and time-dependent kinetic profiles cooperatively reveal that UiO-66(N10%-Zr) exhibits an advanced ideal adsorbed solution theory selectivity of 326, an excellent diffusion selectivity of 60.7, and a dynamic selectivity of 195 for CO2/CH4 separation, confirming the unwanted equilibrium-kinetic effect. Breakthrough experiments and modeling simulations further confirm the enhanced hydrophobic nature and high CO2/CH4 separation performance of UiO-66(N10%-Zr) even under humid conditions. The node-based engineering strategy is here demonstrated to be highly effective for CO2/CH4 separation, providing a new direction to achieve advanced MOF structures with sustainable advantages including high adsorption capacity, high selectivity, and hydrophobicity, which are of crucial significance for industrial applications.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Ke Chen,Linhan Ni,Xin Guo,Chengming Xiao,Yue Yang,Yujun Zhou,Zhigao Zhu,Junwen Qi,Jiansheng Li
The performance of mixed matrix membranes (MMMs) substantively depends on the intrinsic structure and composition of the introduced nanofillers. In this work, pyrazole-based metal-organic frameworks (termed as MOF-303) were introduced into polymer of intrinsic microporosity (PIM-1) through a physical blending approach. Thanks to the well CO 2 -philic capability, high porosity, and appropriate pore structure of the incorporated MOF-303, the obtained MMMs exhibited remarkable separation performance. The improved CO 2 permeability and well-maintained CO 2 /CH 4 selectivity were achieved. Specifically, MMMs introducing 30 wt% MOF-303 loading exhibited a CO 2 /CH 4 selectivity of 27.6 and a high-CO 2 permeability of 7528.2 Barrer, which were 2.2 and 1.9 times greater than those of the unfilled PIM-1 membranes, respectively. Furthermore, a 33-h continuous separation test verified the excellent stability of the manufactured MMMs. More importantly, the MMMs showed significant resistance against physical aging, retaining up to 92.8% of their original CO 2 permeability after 150 days, compared to just 33.0% for control PIM-1 over the same period. Meanwhile, the plasticization resistance of the MMMs was reinforced compared to the unfilled PIM-1 membrane. This study potentially provides a novel approach for the rational design of MMMs in CO 2 separation applications.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Daofei Lv,JiaYu Chen,Kexin Yang,Houxiao Wu,Yongwei Chen,Chongxiong Duan,Ying Wu,Jing Xiao,Hongxia Xi,Zhong Li,Qibin Xia
Using porous materials to selectively adsorb CO 2 from flue gas or natural gas is a promising method for mitigating CO 2 emission and purifying methane. Here, we synthesized an L-aspartic acid based microporous metal-organic framework (MIP-202) and studied its adsorptive separation performance for CO 2 /CH 4 and CO 2 /N 2 mixtures. Results show that MIP-202 had ultrahigh CO 2 /CH 4 (72.9 and 241.5 for CO 2 /CH 4 = 50/50 and 10/90, respectively) and CO 2 /N 2 (1,950,000 and 2129.1 for CO 2 /N 2 = 50/50 and 15/85, respectively) IAST selectivities at 298 K and 100 kPa. The high selectivity was verified by the calculations of Henery’s law selectivity and breakthrough experiments. Metropolis Monte Carlo simulation calculations show that CO 2 with greater polarizability and quadruple moment tends to occupy the pore walls of large cages with higher polarity, while the less polar CH 4 or N 2 majorly being adsorbed in the pore walls of small cages with lower polarity, resulting in the ultrahigh CO 2 /CH 4 and CO 2 /N 2 separation selectivities. MIP-202 exhibits low CO 2 adsorption enthalpy (17.2–30.7 kJ/mol), superior persistent reusability after five cyclic adsorption experiments, easy desorption performance at 298 K, moderate water and moisture stability, good stability under dry and humid SO 2 atmosphere, and low ligand cost ($36/kg). MIP-202 extrudates were prepared by an extrusion molding method using hydroxypropyl cellulose (HPC) as the binder and they retained 97.35% CO 2 uptake of MIP-202 powder at room temperature and pressure. This work shows that MIP-202 is an industrially promising material for the separation of CO 2 /CH 4 and CO 2 /N 2 mixtures.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2026
·Vol. 71
·期 8
·3669-3680
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IF 2.4
Wu Shasha,Li Wenyu,Yang Li,Chen Zhen,Qin Yuanhang,Yuan Lunyong,Sun Wei
This study systematically investigates the influence
of lithium
nitrate (LiNO 3 ) modification on the gas adsorption characteristics
of UiO-66. The adsorption isotherms for carbon dioxide (CO 2 ), methane (CH 4 ), and nitrogen (N 2 ) were acquired
within a pressure range of 0 to 20 bar. The results from the cyclic
testing indicate that the UiO-66–0.05LiNO 3 variant
exhibits commendable stability. Notably, the incorporation of LiNO 3 enhances the CO 2 adsorption capacity by 29.48%,
reaching 2.24 mmol·g –1 at a pressure of 1 bar.
This is attributed to the introduction of lithium ions, which enhance
the electrostatic interaction between CO 2 and the MOF.
Analysis of the high-pressure data reveals that the Langmuir–Freundlich
model provides the most robust fit, whereas the Langmuir and Dual-site
Langmuir models demonstrate increased discrepancies as pressure escalates.
According to calculations based on the Ideal Adsorption Solution Theory
(IAST), the maximum selectivity of the material for the CO 2 /CH 4 and CO 2 /N 2 mixtures is 11.5
and 56.0, respectively. These results suggest that LiNO 3 modification significantly enhances both the adsorption capacity
and the selectivity for CO 2 separation.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2026
·
IF 3.5
Mi Yan,Cao Miao,Teng Cang,Xiangzhi Kong,Yan Zhang,Shuai Liu,Dan Wang,Ekkachai Kanchanatip
UiO-66 MOF was functionalized with dual ligands namely BDC-NH 2 and BDC-(OH) 2 . • Selective CO 2 /CH 4 adsorption were investigated at atmospheric and high pressures. • The highest CO 2 /CH 4 selectivity of 35.60 was achieved with 10%H-ZrMOF-A adsorbent. • CO 2 adsorption capacity of the adsorbent remained over 91.5% after five reuses. Selective CO 2 /CH 4 separation is essential for biogas valorization, yet conventional adsorbents typically face a trade-off between adsorption capacity and selectivity. In this work, a dual-ligand engineering strategy is implemented on UiO-66-NH 2 (ZrMOF-A) by co-incorporating 2,5-dihydroxyterephthalate (BDC-(OH) 2 ) to create a series of mixed-ligand MOFs denoted X %H-ZrMOF-A ( X = 5%–50% (mass)). The materials were synthesized via a solvothermal route and systematically characterized by N 2 physisorption, powder X-ray diffraction, FTIR spectroscopy, and SEM to elucidate structure-property relationships. Increasing hydroxyl content progressively modified surface area, pore volume, and morphology, with excessive BDC-(OH) 2 loading (>30% (mass)) inducing pronounced structural degradation. Among the series, 10%H-ZrMOF-A exhibited the most favorable balance between textural properties and functional site density, achieving a CO 2 uptake of 1.352 mmol·g –1 and a CO 2 /CH 4 selectivity of 35.60 at 100 kPa and 25 °C for a 40:60 CO 2 :CH 4 mixture predicted by IAST. Multi-model isotherm analysis identified the Freundlich and Elovich models as the most suitable descriptions of CO 2 adsorption, confirming a heterogeneous adsorption landscape arising from the coexistence of amine and hydroxyl sites. Complementary DFT calculations showed that dual functionalization strengthens CO 2 binding while weakening CH 4 interactions, consistent with the experimentally observed enhancement in selectivity. Pressure-dependent measurements revealed that high CO 2 /CH 4 selectivity at low pressures (≤100 kPa) diminishes at elevated pressures as non-selective pore filling becomes dominant, indicating that 10%H-ZrMOF-A is particularly suited for low-pressure biogas upgrading and post-combustion CO 2 capture. Five consecutive adsorption-desorption cycles demonstrated 91.5% capacity retention, confirming moderate short-term recyclability under mild thermal regeneration conditions. Download: Download high-res image (204KB) Download: Download full-size image
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FUEL
·
2022
·
IF 8.035
Chengming Huang,Yiming Zhang,Dingmei Han,Binbin He,Xinyu Sun,Meiyu Liu,Yi Mei,Yun Zu
Ni-based catalysts using siliceous materials as the supports have suffered from two challenging issues of sintering and carbon deposition for dry reforming of methane (DRM), resulted from a weak metal-support interaction. Given these, a novel metal–acid bifunctional Ni@S-1 zeolite catalyst is tailored from the evolution of hydroxylated nickel phyllosilicates that are formed by subtly controlling the coordination environments of Ni precursor complexes in the silicalite-1 (S-1) zeolite. The developed Ni 0.44 @S-1 catalyst renders almost equivalent CH 4 and CO 2 conversions (85.1 % and 88.7 %), high H 2 /CO molar ratio (about 1) and superb long-term stability during 100 h with no activity loss at 750 °C with a WHSV of 100 L·g cat −1 ·h −1 , outperforming other control catalysts under investigation. Such superior catalytic behavior benefits from the synergy between highly uniform Ni nanoparticles (3–5 nm) confined in the micropores of zeolite and substantially formed Lewis acid sites due to coordinatively unsaturated Ni 2+ sites located at the reduced 2:1 nickel phyllosilicate, as revealed by detailed characterizations. Meanwhile, it further discloses that a benign balance between formation and elimination of “process carbon” species is responsible for improving the carbon resistance of catalyst during the DRM reaction. The present design broadens a new insight for the development of new Ni-based catalysts with simultaneous coking- and sintering-resistant for the DRM application.
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