Nitrogen Removal From Natural Gas

Ringer, Marianna; Su, Tianyan; He, Zhimin; Pinnau, Ingo; Wijmans, J.G.; Morisato, Atsushi; Amo, Kazuo; DaCosta, Andre R.; Baker, Richard W.; Olsen, R.P.; Hassani, Hassan; Rathkamp, T.

doi:10.2172/780455

Cited by 21 publications

(39 citation statements)

References 6 publications

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“…These plots yield isosteric heats of adsorption for methane and dinitrogen that are both relatively low and quite similar; in particular, they are 5.3 ± 0.2 and 5.5 ± 0.2 kcal/mol, respectively, which yields an experimental difference of 0.2 ± 0.3 kcal/mol. These results differ from the previously reported values of 4.8 kcal/mol for CH 4 44 and 8.4 kcal/mol for N 2 12 both because of the lower temperature and because of the change in experimental procedure; the present results should be more accurate for the difference because they were done with isotherms at the same temperature on the exact same batch of sample. An attempt to obtain the same information for V-MOF-74 was not successful.…”

Section: ■ Theoretical Methodscontrasting

confidence: 99%

“…Table 3 shows that the M−N distance is shorter in V-MOF-74 than in Fe-MOF-74, as anticipated above; there is also a smaller difference in the M−C distances for CH 4 . Neutron powder diffraction experiments on Fe-MOF-74 at 10 K (see figure in the Supporting Information) indicate excellent agreement between the calculated and the experimentally observed structures of methane bound to Fe 2+ .…”

Section: ■ Theoretical Methodssupporting

confidence: 72%

“…One should also consider that the two models have different ligand coordination environments, and this too has an influence on the absolute binding energies. In order to further verify the validity of these predictions, isosteric heats of CH 4 and N 2 adsorption in Fe 2 (dobdc) were obtained experimentally from adsorption isotherms at 175 K. (Details of the experiment are in the Supporting Information.) As seen in Figure 2, the uptake of N 2 in Fe-MOF-74 is relatively steep and approaches one N 2 molecule per iron cation site at 1 bar and 175 K. Methane uptake, while similar at low pressure, reaches a higher value of approximately 1.5 CH 4 molecules per iron at 1 bar.…”

Section: ■ Theoretical Methodsmentioning

confidence: 99%

“…Although cryogenic distillation is currently utilized for separation of these gases, the cost-and capital-intensive nature of this separation has led to development of a number of competing processes, such as membraneor kinetics-based separations, which generally suffer from low selectivities. 4 Adsorptive separations utilizing porous solids containing transition-metal cations capable of reversibly binding dinitrogen may result in highly selective and efficient dinitrogen/methane separations. Metal−organic frameworks are particularly promising in this regard, as they offer a myriad of materials design opportunities and have already shown great potential for a number of gas separation applications.…”

Section: ■ Introductionmentioning

confidence: 99%

“…The M-MOF-74 series of compounds having formula M 2 (dobdc) (where dobdc 4− is 2,5-dioxido-1,4-benzenedicarboxylate) is an especially versatile and intensively studied structure type. 8−13 This structure features 12 Å wide hexagonal channels, lined at the vertices with helical chains of five-coordinate divalent metal ions connected through dobdc 4 4 and N 2 adsorption enthalpies of 4.4 14 and 5.0 15 kcal/mol, respectively. However, in principle, other dicationic metals could be incorporated into this structure type.…”

Section: ■ Introductionmentioning

confidence: 99%

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Design of a Metal–Organic Framework with Enhanced Back Bonding for Separation of N₂ and CH₄

et al. 2013

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Gas separations with porous materials are economically important and provide a unique challenge to fundamental materials design, as adsorbent properties can be altered to achieve selective gas adsorption. Metal−organic frameworks represent a rapidly expanding new class of porous adsorbents with a large range of possibilities for designing materials with desired functionalities. Given the large number of possible framework structures, quantum mechanical computations can provide useful guidance in prioritizing the synthesis of the most useful materials for a given application. Here, we show that such calculations can predict a new metal− organic framework of potential utility for separation of dinitrogen from methane, a particularly challenging separation of critical value for utilizing natural gas. An open V(II) site incorporated into a metal−organic framework can provide a material with a considerably higher enthalpy of adsorption for dinitrogen than for methane, based on strong selective back bonding with the former but not the latter. ■ INTRODUCTIONCoordination of dinitrogen to transition-metal cations is important both fundamentally and industrially. Dinitrogen is highly inert and generally considered to be a poor ligand. In 1965, however, it was shown that a simple coordination complex, [Ru(NH 3 ) 5 ] 2+ , could reversibly bind N 2 . 1 In subsequent years, a number of dinitrogen−transition-metal complexes have been isolated for metals in varying oxidation states with various coordination numbers. 2,3 These complexes typically feature low-valent, relatively reducing metal cations coordinated to dinitrogen in an end-on binding mode. Activating dinitrogen at a metal center to promote its reduction by hydrogen to ammonia under moderate conditions remains a critical goal for homogeneous catalysis. Somewhat weaker metal−dinitrogen binding, however, may be useful for adsorptive separation of gas mixtures. An example is provided by the need to remove dinitrogen (an omnipresent but noncombustible contaminant) from natural gas or other methane-rich gases. This is an extraordinarily difficult separation based on physical properties alone, as both gases lack a permanent dipole and have similar polarizabilities, boiling points, and kinetic diameters. Although cryogenic distillation is currently utilized for separation of these gases, the cost-and capital-intensive nature of this separation has led to development of a number of competing processes, such as membraneor kinetics-based separations, which generally suffer from low selectivities. 4

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Section: ■ Theoretical Methodscontrasting

confidence: 99%

Section: ■ Theoretical Methodssupporting

confidence: 72%

Section: ■ Theoretical Methodsmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

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Design of a Metal–Organic Framework with Enhanced Back Bonding for Separation of N₂ and CH₄

et al. 2013

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Nanostructured Poly(styrene‐b‐butadiene‐b‐styrene) (SBS) Membranes for the Separation of Nitrogen from Natural Gas

Buonomenna

Golemme

Tone

et al. 2012

Adv Funct Materials

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The preparation and characterization of new, tailor-made polymeric membranes using poly(styrene-b -butadiene-b -styrene) (SBS) triblock copolymers for gas separation are reported. Structural differences in the copolymer membranes, obtained by manipulation of the self-assembly of the block copolymers in solution, are characterized using atomic force microscopy, transmission electron microscopy, and the transport properties of three gases (CO 2 , N 2 , and CH 4 ). The CH 4 /N 2 ideal selectivity of 7.2, the highest value ever reported for block copolymers, with CH 4 permeability of 41 Barrer, is obtained with a membrane containing the higher amount of polybutadiene (79 wt%) and characterized by a hexagonal array of columnar polystyrene cylinders normal to the membrane surface. Membranes with such a high separation factor are able to ease the exploitation of natural gas with high N 2 content. The CO 2 /N 2 ideal selectivity of 50, coupled with a CO 2 permeability of 289 Barrer, makes SBS a good candidate for the preparation of membranes for the post-combustion capture of carbon dioxide.

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CH₄‐Selective Mixed‐Matrix Membranes Containing Functionalized Silica for Natural Gas Purification

et al. 2020

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Mixed-matrix membranes were prepared by incorporating functionalized silica nanoparticles (SNPs) into the poly(ether-block-amide). The gas permeation properties of membranes were investigated for the separation of N 2 and CO 2 from CH 4. Results revealed that chemical modification of SNPs and incorporation of the carboxylic groups on its surface had a strong interaction with the polymer matrix and improved the distribution of the nanofiller in the membrane matrix. According to the gas permeation experiments at various SNPs loadings and feed pressures, different trends were observed for the permeability and selectivity. Incorporation of the modified-SNPs nanofiller into the membrane enhanced the CH 4 permeability, as well as the CH 4 /N 2 and CO 2 /N 2 selectivities.

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Nitrogen Removal From Natural Gas

Cited by 21 publications

References 6 publications

Design of a Metal–Organic Framework with Enhanced Back Bonding for Separation of N₂ and CH₄

Design of a Metal–Organic Framework with Enhanced Back Bonding for Separation of N₂ and CH₄

Nanostructured Poly(styrene‐b‐butadiene‐b‐styrene) (SBS) Membranes for the Separation of Nitrogen from Natural Gas

CH₄‐Selective Mixed‐Matrix Membranes Containing Functionalized Silica for Natural Gas Purification

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Nitrogen Removal From Natural Gas

Cited by 21 publications

References 6 publications

Design of a Metal–Organic Framework with Enhanced Back Bonding for Separation of N2 and CH4

Design of a Metal–Organic Framework with Enhanced Back Bonding for Separation of N2 and CH4

Nanostructured Poly(styrene‐b‐butadiene‐b‐styrene) (SBS) Membranes for the Separation of Nitrogen from Natural Gas

CH4‐Selective Mixed‐Matrix Membranes Containing Functionalized Silica for Natural Gas Purification

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Design of a Metal–Organic Framework with Enhanced Back Bonding for Separation of N₂ and CH₄

Design of a Metal–Organic Framework with Enhanced Back Bonding for Separation of N₂ and CH₄

CH₄‐Selective Mixed‐Matrix Membranes Containing Functionalized Silica for Natural Gas Purification