Selective extraction of methane from C1/C2/C3 on moisture-resistant MIL-142A with interpenetrated networks

Yuan, Yinuo; Wu, Houxiao; Xu, Yuzhi; Lv, Daofei; Tu, Shi; Wu, Ying; Li, Zhong; Xia, Qibin

doi:10.1016/j.cej.2020.125057

Cited by 56 publications

(39 citation statements)

References 36 publications

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“…Until now, to design and synthesize MOFs with balanced properties of high gas adsorption uptakes at ultralow pressures, high C 3 H 8 /CH 4 , C 3 H 8 /C 2 H 6 , and C 2 H 6 /CH 4 adsorption selectivities, moderate adsorption enthalpies, high water or chemical stability, etc., are still a great challenge for efficient pipeline NG upgrading, although many MOFs have been reported for the selective C 3 H 8 and C 2 H 6 gas adsorptions over CH 4 gas with some high performances (Tables S3 and S4). ,, Furthermore, the understanding of the mechanisms for the selective adsorptions of C 3 H 8 and C 2 H 6 over CH 4 in MOFs is also crucial for the future development of the new promising potential MOFs. − …”

Section: Introductionmentioning

confidence: 99%

Formation of a N/O/F-Rich and Rooflike Cluster-Based Highly Stable Cu(I/II)-MOF for Promising Pipeline Natural Gas Upgrading by the Recovery of Individual C₃H₈ and C₂H₆ Gases

Cheng

Wang

Meng

et al. 2021

ACS Appl. Mater. Interfaces

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Due to the ultralow amounts of C 3 H 8 and C 2 H 6 gases, to design and synthesize water-stable MOFs that are promising for real-world efficient pipeline natural gas (NG) upgrading by the recovery of individual C 3 H 8 and C 2 H 6 gases is still a great challenge. Here, a N/O/F heteroatom-rich and rooflike [Cu(II) 4 Cu(I) 2 (COO) 4 (tetrazolyl) 6 ] cluster-based ultra-microporous tsi-MOF (SNNU-Bai68) was afforded as a multiple heteroatom-rich and curved-surface-shaped cluster-based ultramicroporous MOF and the first porous MOF based upon such rooflike [Cu(II) x Cu(I) y (tetrazolyl) z ] (2x+y−z)+ cluster. In SNNU-Bai68, the rooflike cluster was further assembled into a 1D chain secondary building block (SBB), which led to a high density of accessible potential adsorptive sites. Very interestingly, it exhibited the most promising balance of high gas adsorption uptakes at 0.01, 0.03, and 0.05 bar, high C 3 H 8 /CH 4 , C 3 H 8 /C 2 H 6 , and C 2 H 6 /CH 4 adsorption selectivities, moderate adsorption enthalpies, and high water and chemical stability for pipeline natural gas upgrading by the recovery of individual C 3 H 8 and C 2 H 6 gases, which was further confirmed by the breakthrough experiments of the gas mixtures with/without 74% RH. Furthermore, the SC-XRD and GCMC studies revealed that the successful separation of C 3 H 8 , C 2 H 6 , and CH 4 gases in SNNU-Bai68 is due to different synergistic effects of H-bonds between the frameworks at three adsorptive sites around each rooflike cluster and those different gas molecules, which were initially described systematically by the number of H atoms from the gas molecules, the total number of H-bonds within the synergistic H-bonds, and the binding energy of the framework at an adsorption site toward the gas molecules. In addition, this work may provide a method for the construction of a multiple heteroatom-rich and curved-surface-shaped cluster-based ultra-microporous MOF as a novel approach to build MOFs with polar pore surfaces, suitable pore sizes, and unique pore shapes to maximize the synergistic H-bonds between the framework and guests. KEYWORDS: N/O/F-rich MOF, rooflike cluster, chemically stable, pipeline natural gas upgrading, C 3 H 8 and C 2 H 6 recovery

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Section: Introductionmentioning

confidence: 99%

Formation of a N/O/F-Rich and Rooflike Cluster-Based Highly Stable Cu(I/II)-MOF for Promising Pipeline Natural Gas Upgrading by the Recovery of Individual C₃H₈ and C₂H₆ Gases

Cheng

Wang

Meng

et al. 2021

ACS Appl. Mater. Interfaces

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“…At 298 K and 1 bar, the adsorption capacity of C 2 H 6 reached 4.04 mmol·g –1 in MIL-160(Al), while it only adsorbed 0.87 mmol·g –1 of CH 4 . Interestingly, the C 2 H 6 capacity of MIL-160(Al) was over twice larger than that of the PCN-233 series and also higher than the majority of MOFs reported, such as MIL-142A, UiO-67, and UTSA-33 (3.82, 3.00, and 2.77 mmol·g –1 , respectively) under the same condition. − We then evaluated the isosteric heat of adsorption ( Q st ) for the gases applying the Clausius–Clapeyron equation on the basis of their adsorption isotherms at different temperatures. The isotherms were well-fitted with the dual-site Langmuir–Freundlich (DSLF) model …”

Section: Resultsmentioning

confidence: 99%

Fructose to Sorbents: Synthesis of Metal–Organic Frameworks Directly from Biomass for Humid Shale Gas Separation

Qadir

et al. 2021

ACS Sustainable Chem. Eng.

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The synthesis of metal–organic frameworks (MOFs) directly starting from biomass, making the most of renewable feedstocks and allowing for coupled or continuous processing, is intriguing. The interference of water (vapor) greatly hinders the wide utilization of MOFs in, e.g., recovering ethane from humid shale gas, which is a critical process for purifying natural gas in practical scenarios. Here, we propose a concept of direct ligand and MOF synthesis in a continuous routine, i.e., a linear synthesis of a bioderived ligand (furan-2,5-dicarboxylic acid), starting from a biomass source (fructose), followed by the in situ synthesis of a series of different MOFs. This strategy is also exempt from the tedious and energy-intensive processes of filtering, purifying, or drying intermediate products. The obtained renewable MOFs, particularly MIL-160(Al), reveal superior ethane capture abilities from shale gas mixtures under ambient conditions compared to most of the MOF materials reported to date. MIL-160(Al) also demonstrates a remarkable cycling nature and facile sorption regenerability to selectively capture ethane even under high-humidity conditions, as verified by static gas sorption measurement, experimental breakthrough tests, and in-depth theoretical studies, further conferring it with great potential for industrial applications.

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“…Considerable research efforts have been contributed to develop excellent adsorbents for light hydrocarbon separation. Adsorbents like zeolites, − metal–organic frameworks (MOFs), − and porous carbon materials − have been intensively developed for gas mixture separation. MOFs have garnered wide interest as a promising adsorbent material because of their ultrahigh specific surface area, tunable pore properties, and controllable functionality .…”

Section: Introductionmentioning

confidence: 99%

“…MOFs have garnered wide interest as a promising adsorbent material because of their ultrahigh specific surface area, tunable pore properties, and controllable functionality . They have been employed for various light hydrocarbon separation. − Li et al investigated an oxalamide-decorated strontium-based MOF for CH 4 /C 2 H 6 separation and revealed a high C 2 H 6 /CH 4 selectivity of 22.5 at 298 K and 1 atm. Yuan et al reported an Fe-MOF with interpenetrated networks, MIL-142A, and at 298 K, its ethane/methane selectivity reached 13.7 with an ethane uptake of 3.82 mmol/g.…”

Section: Introductionmentioning

confidence: 99%

“…They have been employed for various light hydrocarbon separation. − Li et al investigated an oxalamide-decorated strontium-based MOF for CH 4 /C 2 H 6 separation and revealed a high C 2 H 6 /CH 4 selectivity of 22.5 at 298 K and 1 atm. Yuan et al reported an Fe-MOF with interpenetrated networks, MIL-142A, and at 298 K, its ethane/methane selectivity reached 13.7 with an ethane uptake of 3.82 mmol/g. Wu et al synthesized a robust pillared-layer MOF Ni(TMBDC)(DABCO) 0.5 , and its C 2 H 6 /CH 4 selectivity reached up to 29 at 298 K and 1 bar.…”

Section: Introductionmentioning

confidence: 99%

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Adsorption Property of Starch-Based Microporous Carbon Materials with High Selectivity and Uptake for C1/C2/C3 Separation

Xiao

Wen

et al. 2021

Ind. Eng. Chem. Res.

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Recovering light hydrocarbons from natural gas is of great significance in the petrochemical industry. In this work, starch-based microporous carbon materials (SMCs) were prepared using starch as a carbon source and characterized for their pore structure and surface chemistry. CH4, C2H6, and C3H8 isotherms of SMCs were determined using a volumetric method. The breakthrough experiments were carried out to evaluate the dynamic separation performance. A grand canonical Monte Carlo simulation was conducted to reveal the adsorption mechanism of these light hydrocarbons on the SMCs. Results showed that the resulting SMCs exhibited a high specific surface area of 1999 m2/g and a narrow pore size distribution within 0.5–2.0 nm. Particularly, SMCs displayed extremely high ethane and propane uptakes at 298 K and 100 kPa, reaching 5.28 mmol/g for C2H6 and 8.39 mmol/g for C3H8. Moreover, SMCs showed an ultrahigh selectivity of 27.1 for C2H6/CH4 mixtures under ambient conditions, which exceeded that of many metal–organic frameworks. Thus, SMCs have the potential for recovering light hydrocarbons from natural gas.

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Selective extraction of methane from C1/C2/C3 on moisture-resistant MIL-142A with interpenetrated networks

Cited by 56 publications

References 36 publications

Formation of a N/O/F-Rich and Rooflike Cluster-Based Highly Stable Cu(I/II)-MOF for Promising Pipeline Natural Gas Upgrading by the Recovery of Individual C₃H₈ and C₂H₆ Gases

Formation of a N/O/F-Rich and Rooflike Cluster-Based Highly Stable Cu(I/II)-MOF for Promising Pipeline Natural Gas Upgrading by the Recovery of Individual C₃H₈ and C₂H₆ Gases

Fructose to Sorbents: Synthesis of Metal–Organic Frameworks Directly from Biomass for Humid Shale Gas Separation

Adsorption Property of Starch-Based Microporous Carbon Materials with High Selectivity and Uptake for C1/C2/C3 Separation

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Selective extraction of methane from C1/C2/C3 on moisture-resistant MIL-142A with interpenetrated networks

Cited by 56 publications

References 36 publications

Formation of a N/O/F-Rich and Rooflike Cluster-Based Highly Stable Cu(I/II)-MOF for Promising Pipeline Natural Gas Upgrading by the Recovery of Individual C3H8 and C2H6 Gases

Formation of a N/O/F-Rich and Rooflike Cluster-Based Highly Stable Cu(I/II)-MOF for Promising Pipeline Natural Gas Upgrading by the Recovery of Individual C3H8 and C2H6 Gases

Fructose to Sorbents: Synthesis of Metal–Organic Frameworks Directly from Biomass for Humid Shale Gas Separation

Adsorption Property of Starch-Based Microporous Carbon Materials with High Selectivity and Uptake for C1/C2/C3 Separation

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Formation of a N/O/F-Rich and Rooflike Cluster-Based Highly Stable Cu(I/II)-MOF for Promising Pipeline Natural Gas Upgrading by the Recovery of Individual C₃H₈ and C₂H₆ Gases

Formation of a N/O/F-Rich and Rooflike Cluster-Based Highly Stable Cu(I/II)-MOF for Promising Pipeline Natural Gas Upgrading by the Recovery of Individual C₃H₈ and C₂H₆ Gases