JOURNAL OF MOLECULAR STRUCTURE
·
2025
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IF 4.7
Di-Ming Chen,Han-Dong Qiao,Pei-Feng Wang,Zi-Jun Zhao,Shao-Ming Fang
In this study, a porous Ni-MOF formulated as {(H 2 NMe 2 )[Ni 3 (μ 3 OH)(TPT)(TZB) 3 ](H 2 O) 6 (DMA) 7 } n (TZB = 4-(1H-tetrazol-5-yl)benzoate, TPT = 2,4,6-tri(4-pyridyl)-1,3,5-triazine, and DMA = N,N-dimethylacetamide) was prepared and its C 2 H 2 and CO 2 adsorption performances were systemically studied both experimentally and computationally. The structural analysis by single crystal X-ray diffraction studies reveals that the prepared Ni-MOF crystallizes in the space group P6 3 mc and features a porous pacs -type network composed of trigonal bipyramidal and octahedral cages. The activated Ni-MOF (Ni-MOF-a) shows a high C 2 H 2 uptake capacity of 157 cm 3 /g with a moderate C 2 H 2 /CO 2 IAST selectivity of 3.3 at 298 K and 1 bar. More importantly, Ni-MOF-a shows a low adsorption heat for C 2 H 2 ranging from 24.6 to 27.1 kJ/mol at 298 K with a high separation potential of 2.85 mol/kg. In the computational simulation section, six sets of point charge derived from different approaches (Qeq, Mulliken, PACMOF, mCBAC, Mepoml, PACMAN) and two different force-fields (UFF and Dreiding) were used to calculate the C 2 H 2 and CO 2 adsorption isotherms and then compared with the experimental values. Our results reveal that great care should be taken in the selection of point charges and force fields, and the unsuitable combinations might result in an inappropriate C 2 H 2 /CO 2 selectivity which is against the experimental results.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Ihtisham Ul Haq,Shen Hui Li,Hong-Gang Zhen,Rehan Khan,Ao-Shuai Zhang,Zhi-Ping Zhao
For separating 1, 3-butadiene (BD) from BD/N 2 mixture, among numerous studied metal–organic frameworks-based adsorbents, Ni-ZIF-8 was comparatively selected here based on intelligent gravimetric analysis, simulation studies, facile synthesis, and very good IAST selectivity. Experimental results showed good butadiene uptake capacity of Ni-ZIF-8 of 7.41 mol/kg, which is 42% higher than pure ZIF-8. Additionally, Ni-ZIF-8 exhibits IAST selectivities of 2826 and 3302 at 0.1 bar, at 25 and 45 °C respectively, for 20% BD/N 2 adsorption. The molecular simulation results showed that Ni-ZIF-8 has binding energies of 65.25, 9.54 kJ/mol, while ZIF-8 has 56.07, 15.03 kJ/mol for butadiene, and nitrogen, respectively. This strongly supported the experimental results. To the best of our knowledge, Ni-ZIF-8 showed the best working capacity of 5.91 mol/kg for butadiene among all the reported adsorbents. Moreover, dynamic adsorption experiments revealed that butadiene could be recovered from BD/N 2 mixtures at room temperature, suggesting great potential for industrial BD/N 2 separation.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jingyun Qian,Wenna Zhang,Xue Yang,Kexin Yan,Meikun Shen,Hongyue Pan,Hongjun Zhu,Lei Wang
Constructing the metal cation-mediated low-cost inorganic sorbent with high separation efficiency in CO 2 , N 2 , and CH 4 remains a major challenge. Herein, we developed a series of alkali metal cations (Na + , K + , Rb + , Cs + )-exchanged ERI zeolites and adopted in the separation process of CO 2 among the gas mixture. Among the ion-exchanged zeolites, the zeolite K-ERI showed a high adsorption volume of 70.84 cm 3 g −1 and an IAST selectivity of CO 2 /CH 4 : 6254, CO 2 /N 2 : 2872 at 298 K, respectively, far outweighed the reported metal cation exchanged zeolites. Combining powder X-ray diffraction crystallography and density functional theory calculations, we unequivocally unveiled that the metal cations located at s 8 r effectively tailored zeolite aperture, and metal cation-gas molecules interactions synergically restrained the pass-through capacity of CO 2 in ion-exchanged ERI framework. Such a unique host–guest interaction governed by metal cations in aluminosilicate zeolite ERI affords a general strategy for gas separation.
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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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
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IF 3.141
Yongwei Chen,Houxiao Wu,Zewei Liu,Xuejiao Sun,Qibin Xia,Zhong Li
Mechanochemical synthesis, driven the chemical transformation by mechanical force, has been a rapid and efficient strategy to prepare metal–organic frameworks (MOFs). In this work, a liquid-assisted mechanochemical method has been successfully applied to the synthesis of copper based MOF-505. The crystallinity and porosity of MOF-505 were investigated by adjusting the synthesis parameters, such as added solvent (type and amount) and grinding time. Results showed that the type and amount of added solvent were crucial parameters for the mechanochemical synthesis of MOF-505. Furthermore, the optimizations of MOF-505 synthesis were carried out: grinding Cu(OAc)2·H2O and H4bptc as starting materials for 80 min with 0.4 mL of DMF assisted, giving MOF-505-K with Brunauer–Emmett–Teller (BET) surface area of 977 m2/g. Meanwhile, MOF-505-K had moderate CO2 adsorption capacity of 2.01 mmol/g at 298 K and 100 kPa. The adsorptive selectivity determined from ideal adsorbed solution theory (IAST) indicated that MOF-505-K had high CO2/N2 and CO2/CH4 selectivities (26.6 and 5.5) at 298 K. Highly efficient mechanochemical synthesis of MOF-505 provides the promise to facilitate the industrial application of CO2 capture.
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
POLYMER ENGINEERING AND SCIENCE
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2020
·Vol. 61
·期 3
·662-668
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IF 1.917
Jinghu Chen,Lingchang Jiang,Chengyun Li,Wenying Fu,Qineng Xia,Yangang Wang,Yuandong Huang
Light hydrocarbon separation is a crucial process associated with high energy expenditure in the petrochemical industry. The utilization of porous organic materials as solid porous adsorbents for light hydrocarbon separation has found widespread attention because of the advantages of low cost, excellent stability, and good recyclability. Here, we present the facile synthesis of a porous organic material, constructed from pyridine-triphenylborane by using a Friedel-Crafts alkylation coupling reaction, affording the hyper-cross-linked polymer, HCP-B. HCP-B features significant thermal stability, and high surface area. Gas adsorption experiments show that this material adsorbs much larger amounts of ethane, ethylene, and acetylene than that of methane. Ideal adsorbed solution theory (IAST) calculations also predict that HCP-B selectively adsorbs ethane, ethylene, and acetylene over methane. Both are indicative of the great potential of HCP-B in light hydrocarbon separation.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2018
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IF 3.927
Houxiao Wu,Yongwei Chen,Daofei Lv,Renfeng Shi,Yang Chen,Zhong Li,Qibin Xia
The purification of ethylene (C 2 H 4 ) from the cracking gas ethane/ethylene mixture (1:15, v / v ) is a typical energy-intensive process in the chemical industry. As an alternative, adsorptive separation with much lower energy consumption and operational cost has attracted escalating attention. In this work, we reported an interesting C 2 H 6 -trapping adsorbent, In-soc-MOF-1, an indium-based metal-organic framework exhibiting the preferential adsorption of C 2 H 6 over C 2 H 4 . Single-component adsorption isotherms showed that the C 2 H 6 adsorption capacities were higher than those of C 2 H 4 under measured temperatures (288, 298 and 308 K). For example, the uptakes of C 2 H 6 and C 2 H 4 were 4.04 and 3.72 mmol/g at 298 K and 100 kPa, respectively. The calculated IAST selectivity of C 2 H 6 /C 2 H 4 (1:15) on In-soc-MOF-1 was in the range of 1.4–4.8. Moreover, the dynamic separation performance of In-soc-MOF-1 toward the C 2 H 6 /C 2 H 4 binary mixture was evaluated by the breakthrough experiments, the result of which suggests that In-soc-MOF-1 could achieve efficient separation by trapping the impurity C 2 H 6 molecules out of the C 2 H 6 /C 2 H 4 binary mixture. Notably, In-soc-MOF-1 not only showed good water and moisture stability but also exhibited excellent recyclability, where negligible decrease in C 2 H 6 adsorption capacity was observed during five cycles of adsorption-desorption tests. These properties suggest that In-soc-MOF-1, as a C 2 H 6 -trapping adsorbent, could be considered as a potential candidate in the practical application of separating the cracking gas mixture.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Huiyuan Cheng,Jingwei Hu,Zihan Liu,Guangping Lei,Guojun Xi,Yayun Zhang,Hantao Liu,Xuhuan Guo,Huiyun Ren
Developing novel adsorbents for CO 2 capture and separation offers an efficient approach to relieving global environmental problems. To promote CO 2 capture from flue gas, novel Cr 3 O@MIL-101(Cr) composites was synthesized through packing [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 into MIL-101(Cr) cages. The resultant composite Cr 3 O@MIL-101(Cr) presents higher CO 2 uptakes at lower pressure ranges, benefiting from the increased content of unsaturated Cr(III) ions and micropores relative to MIL-101(Cr). Meanwhile, IAST selectivity for CO 2 /N 2 mixture reached 50.2 under standard temperature and pressure, outperforming most of the reported materials. Further GCMC simulations reveal that the synergistic effect of [Cr 3 O(HCOO) 6 (H 2 O) 3 ] + , NO 3 − and MIL-101 (Cr) could effectively facilitate the interactions with CO 2 molecules and hinder N 2 molecules from approaching the optimal adsorption sites. Thus the [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 encapsulated MIL-101(Cr) can be recommended as a promising adsorbent for superior CO 2 /N 2 separation.
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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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2013
·
IF 2.206
Jiangfeng Yang,Junmin Li,Wei Wang,Libo Li,Jinping Li
Three hydrophobic microporous high-silica zeolites, DDR (with an 8-membered ring), silicalite-1 (a 10-membered ring), and beta (a 12-membered ring) were synthesized. The Si/Al ratios were 230, 1350, and 35, respectively. The samples were characterized by X-ray diffraction, scanning electron microscopy, thermal gravimetric analysis, water vapor adsorption, and volumetric nitrogen adsorption. They were tested for their CO2, CH4, and N2 adsorption properties at pressures of up to 10 bar at 288–313 K after activation, and the results were correlated with the Langmuir model. The heat of adsorption was calculated using the Clausius–Clapeyron equation based on the adsorption isotherms. These data were used to estimate the separation selectivities for CO2/CH4 and CH4/N2 binary mixtures at 298 K, using the ideal adsorbed solution theory (IAST) model. Experimental results showed that DDR and beta have good selectivities for CO2/CH4, because they have narrow pores (DDR) or more balance metal ions (relatively low Si/Al ratios beta) effect separately. The synthesized silicalite-1 has the lowest SCO2/CH4 but has the most suitable orifices for methane adsorption and the highest SCH4/N2. In addition, the breakthrough data for CH4/N2 mixtures further indicates that silicalite-1 is more suitable for the CH4 enrichment than the commercially used sorbents zeolite-5A and 13X. From the reproducibility of CH4 and N2 adsorption isotherms on silicalite-1, we can infer that which has the potential to be a commercial sorbent by the stable adsorption properties.
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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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xun Wang,Zewei Liu,Jian Yan,Daofei Lv,Xin Chen,Feng Xu,Xin Zhou,Zhong Li
Developing adsorbents with exceptional CH 4 /N 2 selectivity under high pressure is a crucial commercial requirement and a significant technical challenge for the industrial high-pressure swing adsorption (HPSA) in CH 4 /N 2 separation. Only a few adsorbents were reported to address this issue. In this work, we aimed to explore two microporous MOFs with low-polarity channels for high-pressure CH 4 /N 2 separation. The Ni(BDC)(DABCO) 0.5 and its isostructural analog Ni(TMBDC)(DABCO) 0.5 were synthesized, characterized, and examined for high-pressure CH 4 /N 2 adsorption property. Due to the lower polarity channel originating from tetramethyl groups, Ni(TMBDC)(DABCO) 0.5 exhibited an exceptional methane capacity of 4.23 mmol/g and an IAST selectivity of 5.1 for the CH 4 /N 2 binary mixture at a pressure of 10 bar, surpassing the majority of previously reported materials. The GCMC simulation revealed that the low-polarity pore surfaces in both materials exhibited a higher affinity for CH 4 molecules compared to N 2 molecules, under both ambient and high pressures. The breakthrough experiments showed that Ni(TMBDC)(DABCO) 0.5 exhibited excellent dynamic separation towards CH 4 /N 2 under both 1 bar and 5 bar, indicating great potential as an emerging candidate for the recovery of CH 4 from coal-mine methane in industrial PSA processes.
研究领域:
材料科学
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化学工程
·
吸附技术
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Xiao-Wei Liu,Yi-Ming Gu,Tian-Jun Sun,Ya Guo,Xiao-Li Wei,Sheng-Sheng Zhao,Shu-Dong Wang
The highly efficient separation of CH4/N2 remains a great challenge, but it is vital to make the most of diverse natural gas resources and contributes to mitigating global warming. In this work, two isostructural metal–organic frameworks (MOFs), M-MA-BPY where M is Co and Ni, were elaborately selected and synthesized to serve the purpose. These MOFs were thoroughly characterized and found to have favorable framework flexibility, endowing them with narrow and uniform pore networks suitable for the adsorptive separation of CH4/N2. Further studies revealed the M-MA-BPY MOFs’ excellent stability toward water and moist air. Pure gas adsorption experiments suggested they have decent CH4 capacities (0.92 and 1.01 mmol·g–1 for Co- and Ni-MA-BPY), prominent CH4/N2 selectivities (7.2 and 7.4 for Co- and Ni-MA-BPY, IAST selectivity with equimolar CH4/N2 gas mixture) at 298 K and 1 bar, and desirable heats of adsorption for CH4 (22.8 and 23.5 kJ·mol–1 for Co- and Ni-MA-BPY). Dynamic breakthrough experiments and multiple adsorption–desorption cycling tests for CH4/N2 binary mixtures with different gas ratios of 5:95, 15:85, 30:70, and 50:50 (v/v) confirmed the high separation performance of M-MA-BPY MOFs. Together with their relatively simple synthesis and cheap raw reagents, this work demonstrates M-MA-BPY MOFs are very promising adsorbents for the capture of methane from low-quality natural gas resources in ambient conditions.
研究领域:
化学工程
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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
JOURNAL OF RARE EARTHS
·
2024
·
IF 5.2
Chen Di-Ming,Han-Dong Qiao,Shao-Ming Fang
Introduction of porosity and fluorescent properties into lanthanide metal–organic frameworks (MOFs) with rational design to achieve multifunctional use is of great significance from the energy and environmental viewpoint. In this study, a microporous Tb(III)-based MOF with the formula of {[Tb 2 (oba) 3 (Phen) 2 ](DMF) 2 (H 2 O) 4 } n ( 1 ) was solvothermally prepared via using the mixed ligands of 1,10-phenanthroline (Phen) and 4,4′-oxybis(benzoic acid) (H 2 oba) as organic connecters. The structural evaluation results indicate that complex 1 is composed of binuclear Tb 2 (CO 2 ) 6 (Phen) 2 clusters which are extended by the oba 2− ligands to afford a two-fold interpenetrated framework with one-dimensional microporous channels along the b -axis. Gas sorption studies show that the activated 1 demonstrates a high ideal adsorption solution theory (IAST) sorption selectivity of 7.4 toward C 2 H 2 in a C 2 H 2 /CO 2 gas mixture, which are further supported by the dynamic breakthrough experiments. The grand canonical Monte Carlo (GCMC) simulation results indicate that the synergistic effects of the H-bond interactions of C 2 H 2 with oba 2− ligands and the C–H···π interactions with Phen ligand contribute to the strong binding of the framework toward C 2 H 2 molecules. What's more, the luminescent measurements reveal that the emission of 1 features both the characteristic peaks of Phen ligand and Tb(III) ion, which could be further applied as a self-calibrating sensor for the Cr(VI) detection in water. To the best of our knowledge, complex 1 represents the first example of Tb-MOF holding such a high C 2 H 2 /CO 2 selectivity together with ratiometric Cr(VI) detection performances.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Guangping Lei,Yang Lu,Zihan Liu,Yayun Zhang,Guojun Xi,Huiyuan Cheng,Wenji Rao,Xuhuan Guo
The greenhouse effect associated with excessive CO 2 emission has led to a series of environmental issues, thus developing excellent adsorbents for CO 2 capture from flue gas offers a sustainable approach. To combine the merit of multiple functional components, novel FeTPP@MIL-101(Cr) was prepared by incorporation of 5,10,15,20-tetrakis(4-methylphenyl)porphyrinato iron (III) chloride (FeTPP) into MIL-101(Cr) cages via in-situ packaging strategy. The cage-confined FeTPP can both regulate the pore structures of MIL-101(Cr) and provide additional binding sites for CO 2 adsorption. Profiting from extra interactions for CO 2 component and the “sieving effect” for N 2 component induced by incorporation of FeTPP, the discrepancy of isosteric heat for CO 2 and N 2 was largely amplified. Notably, the CO 2 /N 2 selectivity (15/85, v / v ) calculated by ideal adsorbed solution theory (IAST) increased from 17.1 (MIL-101 (Cr)) to 41.8 (FeTPP@MIL-101 (Cr) with FeTPP loading of 4.98 wt%) at 273 K, 100 kPa, which is 2.44 times larger than that of pristine MIL-101 (Cr) and also exceeds most reported adsorbents.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
危险品化学品经营许可证（带存储）