CHEMISTRY OF MATERIALS
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2025
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IF 7
Beibei Sun,Cheng Zeng,Suyun Deng,Yuewen Gu,Lei Gan,Huajun Yang
The separation of C2H2/CO2 under highly humid conditions by using metal–organic frameworks (MOFs) is extremely challenging because water vapor would reduce the C2H2 adsorption capacity or even degrade the structure of MOFs. In this work, a zirconium zeolitic metal–organic framework (NNM-5) with a small aperture and large cavities exhibits commendable C2H2/CO2 selectivity (16.6 at 298 K and 1 bar) and a high uptake ratio (3.13 at 298 K and 1 bar). More importantly, NNM-5 could maintain at least five breakthrough cycles under highly humid conditions (around 100% RH) without performance degradation compared to that under dry conditions. Our studies indicate that the kinetic mechanism is the key to excellent separation performance under highly humid conditions based on the fact that the material is hydrophilic with a high water uptake, but the diffusion rate of H2O is 2 orders slower than that of C2H2 and CO2 in NNM-5.
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
CRYSTENGCOMM
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2019
·Vol. 22
·期 2
·275-282
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IF 3.382
Peng Yan,Jucai Yang,Xiangying Hao,Zhisheng Chen,Guanhua Shen,Yanhua Zhao,Deyun Ma,Jiaxin Zhu
A new Zn-based metal–organic framework with 8-connected hex topology constructed from bipyridine and carboxylate ligands, namely [Zn(cpna)3(tmbpy)]n·4DMF (1) (H2cpna = 6-(4-carboxyphenyl)nicotinic acid; tmbpy = 3,3′-dimethyl-4,4′-bipyridine), has been synthesized under solvothermal conditions. The Zn-MOF was structurally characterized and retained a good crystal structure after activation (1a), an indication of permanent porosity. 1a exhibits a BET surface of 770 m2 g−1 and the maximum aperture of 8.60 Å. Single component adsorption isotherm measurements of C2H2, CO2, CH4, CO and N2 on 1a were performed both at 273 K and 298 K, and the selectivities for C2H2/CH4, C2H2/CO2, CO2/CO, CO2/CH4 and CO2/N2 were estimated on the basis of the ideal adsorbed solution theory (IAST). 1a shows the uptake of C2H2 (3.89 mmol g−1) and CO2 (3.52 mmol g−1) at 273 K and 100 kPa, respectively. Due to the Lewis basic pyridyl sites inside the channel of the framework, 1a showed good adsorption selectivities for C2H2/CH4(50 : 50) and C2H2/CO2(50 : 50) at 298 K (100 kPa).
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
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Wan-Qi Sun,Jian-Bo Hu,Yun-Jia Jiang,Nuo Xu,Ling-Yao Wang,Jia-Hao Li,Yong-Qi Hu,Simon Duttwyler,Yuan-Bin Zhang
The separation of C 2 H 2 /CO 2 is an important process in industry but challenged by the trade-off of capacity and selectivity owning to their close physical properties and identical kinetic molecular size. Herein, we reported a new metal organic framework ZNU-3 (ZNU = Zhejiang Normal University) with flexibility controlled by abundant hydrogen-bonds for highly selective molecular sieving of C 2 H 2 from CO 2 , CH 4 , C 2 H 4 and C 2 H 6 using commercially available cost-effective ligands. At 1.0 bar and 298 K, the uptake capacity of C 2 H 2 is 81.0 cm 3 (STP) g −1 , while the CO 2 , C 2 H 4 , C 2 H 6 , CH 4 , N 2 uptake capacities are only 5.4, 5.3, 1.0, 1.1, 1.1 cm 3 (STP) g −1 , respectively. Such high uptake ratios of C 2 H 2 over other C2 and C1 gases have rarely been achieved. Particularly, the C 2 H 2 /CO 2 uptake ratio of 14.9 is only secondary to that of the benchmark UTSA-300a and much higher than those of all other porous materials. Dynamic breakthrough experiments with equimolar C 2 H 2 /CO 2 mixtures showed that the retaining time of C 2 H 2 is nearly 2 fold of that of CO 2 , indicating the excellent practical separation performance of ZNU-3 for C 2 H 2 /CO 2 mixtures. Modeling studies indicated that C 2 H 2 is mainly trapped by two opposite carboxylic groups with additional small contribution from π···π packing between pyridine ring and planar C≡C moiety.
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
JOURNAL OF MOLECULAR STRUCTURE
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2023
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IF 3.8
Di-Ming Chen,Xue-Jing Zhang
Acetylene is an important industrial material for the production of acetaldehyde, acetic acid, benzene, synthetic rubber, synthetic fiber, etc., and its separation from the gas mixtures of C 2 H 2 /CO 2 is of great importance but a challenging task due to their similar physical properties and molecular sizes. In this study, taking the advantage of open-donor sites on the pore surface as the nano-traps for C 2 H 2 molecules, a new microporous metal-organic framework (MOF) formulated as {[C o 3 (OH) 2 (HCOO) 2 (CPT) 2 ](NMF) 2 (MeOH) 3 (H 2 O)} n ( 1 , NMF = N - methylformamide) has been prepared by virtue of a bifunctional organic ligand 4-(4H-1,2,4-triazol-4-yl)benzoic acid (HCPT), which showed discriminating sorption performance toward C 2 H 2 (113 cm 3 /g at 298 K and 1 bar) over CO 2 (33 cm 3 /g) under the same conditions. The different sorption behavior of {[C o 3 (OH) 2 (HCOO) 2 (CPT) 2 ]} n between C 2 H 2 and CO 2 results in a high uptake ration (3.4:1) and IAST selectivity (13) at 298 K and 1 bar. Furthermore, the force-field based grand canonical Monte Carlo (GCMC) simulation results demonstrate that the large electronegativity and polarizability of open O donor sites on the pore surface contribute to its high C 2 H 2 /CO 2 separation performance, leading to its more favorable C 2 H 2 uptakes than CO 2 .
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Shuangqing Shang,Pengxiang Wang,Hanting Xiong,Xing Liu,Junhui Liu,Hua Shuai,Lingmin Wang,Zhenglong Zhu,Zhiwei Zhao,Yong Peng,Jingwen Chen,Shixia Chen,Zhenyu Zhou,Jun Wang
The efficient separation of C 2 H 2 /CO 2 mixtures is critical yet and remains challenging owing to their closely similar physical properties and molecular sizes. Herein, we report a novel flexible microporous adsorbent, Zn-SDBA-bpy (SDBA=4,4′-sulfonyldibenzoic acid, bpy = 4,4′-bipyridine), for molecular sieving of C 2 H 2 from CO 2 . Zn-SDBA-bpy features contracted interlayer cavities with a highly negative electro-environment arising from abundant exposed oxygen atoms of SDBA. Charge transfers between C 2 H 2 and the framework result in strong C 2 H 2 -host interactions that induce a selective gate-opening effect towards C 2 H 2 . Therefore, Zn-SDBA-bpy exhibits substantial C 2 H 2 capture at low pressure (20.7 cm 3 g −1 at 0.1 bar) while excluding CO 2 , demonstrating high C 2 H 2 /CO 2 selectivity (490.2). Notably, Zn-SDBA-bpy features the lowest C 2 H 2 gate-opening threshold ( ca. 0.01 bar) among reported flexible adsorbents for C 2 H 2 /CO 2 separation. Dynamic breakthrough experiments confirm its excellent C 2 H 2 /CO 2 separation yielding high-purity C 2 H 2 (>99.5 %) products. Modeling studies reveal the strong host-C 2 H 2 interactions and underlying mechanisms of molecular sieving within Zn-SDBA-bpy.
研究领域:
化学
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材料科学
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环境科学
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高影响因子
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