Efficient SF6/N2 separation at high pressures using a zirconium-based mesoporous metal–organic framework

The capture and separation of CF 4 , C 2 F 6 , and SF 6 and their mixtures containing nitrogen is a challenging process. To solve this, we propose the use of saccharose coke-based carbons as membranes for the adsorption and separation of these gases. By means of advanced techniques of Monte Carlo and molecular dynamics simulations, we have studied the adsorption and diffusion of CF 4 , C 2 F 6 , and SF 6 as well as their mixtures with nitrogen in three HRMC carbon models, namely, CS400, CS1000, and CS1000a. We have computed the adsorption isotherms of the single components and the heat of adsorption as a function of the adsorbed concentration. We have also calculated the competitive adsorption of fluoride molecules and nitrogen at two different molar fractions, 0.1 and 0.9. We have computed the transport properties of the adsorbed gases in terms of the self-diffusivities and corrected diffusivities. The performance of the membranes for the targeted separations has been characterized by the calculation of the permselectivity. Our results indicate that the activated amorphous carbon CS1000a is an efficient adsorbent for the capture of the fluoride adsorbates as well as their purification from nitrogen-based mixtures.

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“…More recently, Kim M.B. et al55 studied SF 6 /N 2 separation in UIO-66 and UIO-67 MOFs and NaX zeolite, which was also reported by Dunne et al…”

supporting

confidence: 57%

“…More recently, Kim M.B. et al studied SF 6 /N 2 separation in UIO-66 and UIO-67 MOFs and NaX zeolite, which was also reported by Dunne et al The adsorption capacity of UIO-66 and NaX is about 2 mol/kg of SF 6 , while UIO-67 shows the highest adsorption capacity reaching 9 mol/kg. This is attributed to the very large pores of about 23 Å.…”

Section: Resultsmentioning

confidence: 58%

Separation of CF₄/N₂, C₂F₆/N₂, and SF₆/N₂ Mixtures in Amorphous Activated Carbons Using Molecular Simulations

Peng

Vicent-Luna

Jin

2020

ACS Appl. Mater. Interfaces

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“…Over the past decades, metal–organic frameworks (MOFs) have attracted great attention owing to their highly tunable structural and chemical features. − In contrast to the prototypical greenhouse gas CO 2 , − only a few studies have been reported on MOFs for the selective SF 6 capture over N 2 . ,,− So far, UiO-66-Br 2 is the best selective MOF under industrially relevant working conditions (SF 6 :N 2 = 10:90 and room temperature), showing an ideal adsorbed solution theory (IAST)-predicted SF 6 /N 2 selectivity of 220; however, its SF 6 uptake at 1.0 bar as single component is extremely low (0.93 mmol g –1 ) . Meanwhile, MOF-74(Mg) exhibits the highest pure SF 6 uptake (6.42 mmol g –1 ) at 1.0 bar associated with a low IAST SF 6 /N 2 selectivity (19.0) and relatively low SF 6 uptake (1.82 mmol g –1 ) in the mixture case at 1.0 bar .…”

Section: Introductionmentioning

confidence: 99%

Computer-Aided Discovery of MOFs with Calixarene-Analogous Microenvironment for Exceptional SF₆ Capture

et al. 2021

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Finding optimal adsorbents to achieve an efficient capture and recovery of sulfur hexafluoride (SF 6 ) from SF 6 /N 2 mixture is of great industrial importance. To address this key challenge, here we present a materials-genomics-accelerated strategy by integrating high-throughput computational screening with subsequent synthesis and adsorption/separation testing of the identified promising material. From over 10140 metal−organic frameworks (MOFs), those with calixarene-analogous pore feature were computationally identified as optimal adsorbents with exceptional SF 6 /N 2 selectivity and SF 6 uptake. The separation mechanism was revealed to be thermodynamically driven owing to the synergistic contribution of multiple hydrogen-bond and van der Waals-type SF 6 /MOF pore wall interactions. As a proof-ofconcept, one of the discovered MOFs was further synthesized, and equilibrium adsorption measurements demonstrated both record SF 6 adsorption capacity as a single component at 0.1 bar (3.39 mmol g −1 ) and SF 6 /N 2 IAST-predicted selectivity (∼266) under ambient conditions. Besides its excellent regeneration and cycling performance, dynamic breakthrough experiments further confirmed the attractiveness of this MOF for SF 6 capture under working conditions.

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“…Figure 3a shows the IAST-predicted selectivity for SF 6 /N 2 (SF 6 /N 2 = 1/9) mixtures on the three MOFs. The predicted selectivity of SF 6 /N 2 for Ni(ina) 2 reached an unprecedented 375.1-higher than any other material reported to date (Table S1), including Cu-MOF-NH 2 (266.2), [12] HKUST-1 (70.4), [15] SBMOF-1 (325), [9] UiO-66 (127.8), [13] UiO-66-Br 2 (220.0), [13] UiO-66-Zr (74), [19] CAU-17 (31.0), [17] MOF-74(Zn) (46.0), [8] MOF-74(Co) (40), [8] MOF-74(Mg) (32.0), [8] MIL-100(Fe) granule (25), [11] UiO-67 (21.6) [14] and MIL-100(Fe) (24.4). [11] The IASTpredicted SF 6 /N 2 (SF 6 /N 2 = 1/9) selectivities of Ni(pba) 2 and Cu(peba) 2 samples reached 200.6 and 18.2 at 298 K and 100 kPa, respectively.…”

Section: Forschungsartikelmentioning

confidence: 99%

Pore‐Structure Control in Metal–Organic Frameworks (MOFs) for Capture of the Greenhouse Gas SF₆with Record Separation

Wang

Liu

et al. 2022

Angewandte Chemie

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In the electronics industry, the efficient recovery and capture of sulfur hexafluoride (SF6) from SF6/N2 mixtures is of great importance. Herein, three metal–organic frameworks with fine‐tuning pore structures, Cu(peba)2, Ni(pba)2, and Ni(ina)2, were designed for SF6 capture. Among them, Ni(ina)2 has perfect pore sizes (6 Å) that are comparable to the kinetic diameter of sulfur hexafluoride (5.2 Å), affording the benchmark binding affinity for SF6 gas. Ni(ina)2 exhibits the highest SF6/N2 selectivity (375.1 at 298 K and 1 bar) and ultra‐high SF6 uptake capacity (53.5 cm3 g−1 at 298 K and 0.1 bar) at ambient conditions. The remarkable separation performance of Ni(ina)2 was verified by dynamic breakthrough experiments. Theoretical calculations and the SF6‐loaded single‐crystal structure provided critical insight into the adsorption/separation mechanism. This porous coordination network has the potential to be used in industrial applications.

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Efficient SF6/N2 separation at high pressures using a zirconium-based mesoporous metal–organic framework

Cited by 41 publications

References 52 publications

Separation of CF₄/N₂, C₂F₆/N₂, and SF₆/N₂ Mixtures in Amorphous Activated Carbons Using Molecular Simulations

Separation of CF₄/N₂, C₂F₆/N₂, and SF₆/N₂ Mixtures in Amorphous Activated Carbons Using Molecular Simulations

Computer-Aided Discovery of MOFs with Calixarene-Analogous Microenvironment for Exceptional SF₆ Capture

Pore‐Structure Control in Metal–Organic Frameworks (MOFs) for Capture of the Greenhouse Gas SF₆with Record Separation

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Efficient SF6/N2 separation at high pressures using a zirconium-based mesoporous metal–organic framework

Cited by 41 publications

References 52 publications

Separation of CF4/N2, C2F6/N2, and SF6/N2 Mixtures in Amorphous Activated Carbons Using Molecular Simulations

Separation of CF4/N2, C2F6/N2, and SF6/N2 Mixtures in Amorphous Activated Carbons Using Molecular Simulations

Computer-Aided Discovery of MOFs with Calixarene-Analogous Microenvironment for Exceptional SF6 Capture

Pore‐Structure Control in Metal–Organic Frameworks (MOFs) for Capture of the Greenhouse Gas SF6with Record Separation

Contact Info

Product

Resources

About

Separation of CF₄/N₂, C₂F₆/N₂, and SF₆/N₂ Mixtures in Amorphous Activated Carbons Using Molecular Simulations

Separation of CF₄/N₂, C₂F₆/N₂, and SF₆/N₂ Mixtures in Amorphous Activated Carbons Using Molecular Simulations

Computer-Aided Discovery of MOFs with Calixarene-Analogous Microenvironment for Exceptional SF₆ Capture

Pore‐Structure Control in Metal–Organic Frameworks (MOFs) for Capture of the Greenhouse Gas SF₆with Record Separation