A metal-organic framework for C2H2/CO2 separation under highly humid conditions: Balanced hydrophilicity/hydrophobicity

Xie, Xiao‐Jing; Zeng, Heng; Xie, Mo; Chen, Wei; Hua, Gui-Fang; Lü, Weigang; Li, Dan

doi:10.1016/j.cej.2021.132033

Cited by 67 publications

(25 citation statements)

References 39 publications

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“…Metal–organic frameworks (MOFs), as an emerging and burgeoning class of adsorbent materials, have drawn extensive attention, because of their tunable pore structures and surface functionalities. − These features enable MOFs with great potential in the application of light hydrocarbon separations, especially for C 2 H 6 /C 2 H 4 , − C 2 H 2 /C 2 H 4 , , CH 4 /N 2 , C 2 H 2 /CH 4 , 1-butene/2-butene, and C 2 H 2 /CO 2 − mixtures. With respect to the separation of C 2 H 2 /CH 4 and C 2 H 2 /CO 2 , considerable progress has been made in the usage of MOFs to promote the C 2 H 2 binding affinity and separation selectivity through the introduction of open metal sites (OMSs) .…”

Section: Introductionmentioning

confidence: 99%

Efficient C₂H₂ Separation from CO₂ and CH₄ within a Microporous Metal–Organic Framework of Multiple Functionalities

Zhang

Zhao

et al. 2022

Ind. Eng. Chem. Res.

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The separation of acetylene (C 2 H 2 ) from carbon dioxide (CO 2 ) and methane (CH 4 ) is of great significance, but remains challenging, because of their similar physicochemical properties, and it currently has received substantial research interest by using adsorptive separation based on metal−organic frameworks (MOFs). Herein, a new microporous Cu-MOF, [Cu(5-OH-IPA 2− )-(DPYA)(H 2 O)] (BUT-318, where 5-OH-IPA 2− = 5-hydroxyisophthalate and DPYA = 4,4′-dipyridylamine) has been synthesized successfully under solvothermal conditions, which exhibits excellent separation performance for C 2 H 2 /CO 2 and C 2 H 2 /CH 4 gas mixtures. The presence of Cu(II) open metal sites and different Lewis base sites (−OH and −NH) make the activated BUT-318 efficiently bind C 2 H 2 and exhibit high adsorption capacity under low pressure (24.52 and 9.1 cm 3 g −1 under 0.01 bar, at 273 and 298 K, respectively). The corresponding IAST (ideal adsorbed solution theory) selectivity was 9.8 and 244.3 at 273 K and 1 bar for an equimolar C 2 H 2 /CO 2 and C 2 H 2 /CH 4 mixture. The separation performance and reusability under dynamic conditions were also confirmed by column breakthrough experiments, making BUT-318a a promising candidate for the practical C 2 H 2 separation.

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Section: Introductionmentioning

confidence: 99%

Efficient C₂H₂ Separation from CO₂ and CH₄ within a Microporous Metal–Organic Framework of Multiple Functionalities

Zhang

Zhao

et al. 2022

Ind. Eng. Chem. Res.

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“…In short, the adsorption capacity of C 2 H 2 (2.25 mmol g −1 ) is modest for NUM-11a at 298 K and 1.0 bar, higher than or comparable to many well-known MOFs, such as Cu-FINA-2 (approximately 1.79 mmol g −1 ), 33 CPL-1 (1.84 mmol g −1 ) and CPL-1-NH 2 (2.01 mmol g −1 ), 34 M'MOF-3a (1.90 mmol g −1 ), 35 UiO-66-(COOH) 2 (2.16 mmol g −1 ), 36 JNU-1 (2.67 mmol g −1 ), 37 Ni 3 (pzdc) 2 (7Hade) 2 (2.36 mmol g −1 ), 38 NKMOF-1-Cu (2.27 mmol g −1 ), 8 and Cu I @UiO-66-(COOH) 2 (2.31 mmol g −1 ). 36 NUM-11a shows relatively small CO 2 adsorption amounts (1.27 mmol g −1 ) under the same situations, resulting in a well C 2 H 2 /CO 2 uptake ration of 1.78, higher than or comparable to those of UiO-66-(COOH) 2 (1.29), 36 JNU-2 (2.1), 39 etc. In addition, the small adsorption amount for C 2 H 4 also causes a modest C 2 H 2 /C 2 H 4 uptake ratio of 1.3, comparable to that of NKMOF-1-Ni (1.28), 8 FeMOF-74 (1.11), 40 and NOTT-300…”

Section: ■ Results and Discussionmentioning

confidence: 91%

Two-Dimensional Metal–Organic Framework with Ultrahigh Water Stability for Separation of Acetylene from Carbon Dioxide and Ethylene

Yang

Zhou

et al. 2022

ACS Appl. Mater. Interfaces

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Highly selective separation and purification of acetylene (C2H2) from ethylene (C2H4) and carbon dioxide (CO2) are daunting challenges in light of their similar molecule sizes and physical properties. Herein, we report a two-dimensional (2D) stable metal–organic framework (MOF), NUM-11 ([Cu(Hmpba)2]·1.5DMF) (H2mpba = 4-(3,5-dimethyl-1H-pyrazol-4-yl)benzoic acid), with sql topology, stacked together through π–π interactions for efficient separation of C2H2 from C2H4 and CO2. The 2D-MOF material offers high hydrolytic stability and good purification capacity; especially, it could survive in water for 7 months, even longer. This stable MOF selectively captures C2H2 from mixtures containing C2H4 and CO2, as determined by adsorption isotherms. The ideal adsorbed solution theory selectivity calculations and transient breakthrough experiments were performed to verify the separation capacity. The low isosteric heat of NUM-11a (desolvated NUM-11) (18.24 kJ mol–1 for C2H2) validates the feasibility of adsorbent regeneration with low energy footprint consumption. Furthermore, Grand Canonical Monte Carlo simulations confirmed that the pore surface of the NUM-11 framework enabled preferential binding of C2H2 over C2H4 and CO2 via multiple C–H···O, C–H···π, and C–H···C interactions. This work provides some insights to prepare stable MOF materials toward the purification of C2H2, and the water-stable structure, low isosteric heat, and good cycling stability of NUM-11 make it very promising for practical industrial application.

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“…At 100 kPa and 298 K, the C 2 H 2 /CO 2 selectivity in the equimolar binary mixture is 3.3, implying the applicability of CuZn 3 (PDDA) 3 (OH) for C 2 H 2 purification (Figure c). Despite that the calculated selectivity is lower than several MOFs with high-density open metal sites (NKMOF-1-Ni, 30; UTSA-74, 9; and JNU-2, 3.5) and MOFs with fluorinated pillars (SIFSIX-Cu-TPA, 5.3; TiFSIX-2-Cu-i, 6.5), they are superior to many notable MOFs, such as FJU-36 (2.8), ST- sod -Co/Ti (1.7) and SNNU-17 (1.2) . This enhanced selectivity can be attributed to the uncoordinated pyrazyl N atoms in the MOF backbone that facilitate the strong interactions with C 2 H 2 .…”

mentioning

confidence: 81%

A Multinary Metal–Organic Framework with Divided Linkers for C₂H₂/CO₂ Separation

Zhang

Rao

Hou

et al. 2022

ACS Materials Lett.

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Developing porous solid adsorbents with strong interactions toward C2H2 is crucial to achieve C2H2/CO2 separation with high selectivity. Herein, we introduce the concept of “divided linkers” for the construction of metal–organic frameworks (MOFs) with tailored pores and well-positioned adsorption sites. A single CuI node divides the pyrazyl-carboxylate linker 4,4′-(2,6-pyrazinediyl)dibenzoic acid into two equivalent edges. Furthermore, these edges reticulate with the pseudo-octahedral Zn-based building units to afford a porous multinary framework with single crystallinity and impressive chemical stability. Its appropriate pore size (6.4 Å) and high density of interacting sites empower the MOF with high capacity in C2H2 adsorption (104 cm3 g–1) and preferential C2H2 capture over CO2 (selectivity = 3.3) at 298 K. Potential use of the robust architecture for C2H2/CO2 separation is confirmed by the dynamic gas mixture breakthrough experiment.

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A metal-organic framework for C2H2/CO2 separation under highly humid conditions: Balanced hydrophilicity/hydrophobicity

Cited by 67 publications

References 39 publications

Efficient C₂H₂ Separation from CO₂ and CH₄ within a Microporous Metal–Organic Framework of Multiple Functionalities

Efficient C₂H₂ Separation from CO₂ and CH₄ within a Microporous Metal–Organic Framework of Multiple Functionalities

Two-Dimensional Metal–Organic Framework with Ultrahigh Water Stability for Separation of Acetylene from Carbon Dioxide and Ethylene

A Multinary Metal–Organic Framework with Divided Linkers for C₂H₂/CO₂ Separation

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A metal-organic framework for C2H2/CO2 separation under highly humid conditions: Balanced hydrophilicity/hydrophobicity

Cited by 67 publications

References 39 publications

Efficient C2H2 Separation from CO2 and CH4 within a Microporous Metal–Organic Framework of Multiple Functionalities

Efficient C2H2 Separation from CO2 and CH4 within a Microporous Metal–Organic Framework of Multiple Functionalities

Two-Dimensional Metal–Organic Framework with Ultrahigh Water Stability for Separation of Acetylene from Carbon Dioxide and Ethylene

A Multinary Metal–Organic Framework with Divided Linkers for C2H2/CO2 Separation

Contact Info

Product

Resources

About

Efficient C₂H₂ Separation from CO₂ and CH₄ within a Microporous Metal–Organic Framework of Multiple Functionalities

Efficient C₂H₂ Separation from CO₂ and CH₄ within a Microporous Metal–Organic Framework of Multiple Functionalities

A Multinary Metal–Organic Framework with Divided Linkers for C₂H₂/CO₂ Separation