Immobilization of N-oxide functionality into NbO-type MOFs for significantly enhanced C2H2/CH4 and CO2/CH4 separations

Xu, Tingting; Fan, Lihui; Jiang, Zhenzhen; Zhou, Ping; Li, Ziruo; Lu, Huangyan; He, Yabing

doi:10.1039/d0dt01081b

Cited by 73 publications

(43 citation statements)

References 56 publications

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“…Among the three compounds, the ortho ‐dimethyl functionalized compound ZJNU‐96 exhibited the highest gravimetric C 2 H 2 uptake capacity, which is 6.2 % higher than those of its counterpart ZJNU‐95 functionalized with meta ‐methyl group at 298 K and 1 atm. The C 2 H 2 uptake capacity of ZJNU‐96 is at a high level among the C 2 H 2 adsorptive values reported for porous materials under the same conditions [2b,17a] . The density of C 2 H 2 stored in the bulk ZJNU‐96 material at 298 K and 1 atm is 0.154 g cm −3 , which is equivalent to the value corresponding to an imaginary storage condition of 146.7 atm and room temperature, and is 73.3 times the compression limit for safe C 2 H 2 storage at ambient conditions.…”

Section: Resultsmentioning

confidence: 70%

An Isomeric Copper‐Diisophthalate Framework Platform for Storage and Purification of C₂H₂and Exploration of the Positional Effect of the Methyl Group

et al. 2021

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Three isostructural metal-organic frameworks (MOFs) based on dicopper paddlewheels and dimethyl-functionalized linear diisophthalate ligands were solvothermally constructed, with the aim to investigate their performance regarding acetylene (C 2 H 2 ) storage as well as separation and purification and to further understand the positional effect of the weakly polarized methyl functionality. Isotherm measurements and IAST selectivity analyses revealed that the three compounds exhibited the promising potential for storing C 2 H 2 and recovering C 2 H 2 from carbon dioxide (CO 2 ) and methane (CH 4 ) at ambient conditions. Furthermore, their C 2 H 2 adsorption properties can be tailored and optimized by altering the relative position of the methyl substituents immobilized in the organic linkers. At 298 K and 1 atm, the C 2 H 2 uptake capacities vary from 173.0 to 183.6 cm 3 (STP) g À 1 , while the C 2 H 2 /CH 4 and C 2 H 2 /CO 2 adsorption selectivities are in the range of 24.5-26.6 and 4.34-4.70 for the equimolar gas mixtures. The ortho-dimethyl-modified MOF outperformed better than the other two MOF isomers. The results indicate that rational arrangement of functional groups can to some extent improve gas adsorption properties. Although the property discrepancy caused by the less-polar methyl group is not as large as that by Lewis-basic nitrogen atoms, this is the first experimental demonstration of the positional effect of methyl group on C 2 H 2 adsorption.

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Section: Resultsmentioning

confidence: 70%

An Isomeric Copper‐Diisophthalate Framework Platform for Storage and Purification of C₂H₂and Exploration of the Positional Effect of the Methyl Group

et al. 2021

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“…Obviously, the total adsorption volume of MoP@C‐14.1 is increased compared with the unmodified MoP, indicating that the effect of absorbent cotton on MoP is strengthened. Moreover, the hysteresis loop of MoP@C‐14.1 in the isotherm shift to P/P 0 values of 0.7–1.0, and the adsorption amount on the high‐pressure side is larger than unmodified MoP , . It hints that the slit pores may be formed by the accumulation of flake particles .…”

Section: Resultsmentioning

confidence: 95%

MoP@C Supported on Absorbent Cotton as a Highly Efficient Catalyst towards Hydrodechlorination Reaction

Zhang

Yuan

Bai

et al. 2020

Zeitschrift anorg allge chemie

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This paper reports a method for preparing MoP@C synthesized from absorbent cotton. While the influence of the amount of absorbent cotton on its composition and morphology are also explored. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) confirmed that MoP@C and unmodified MoP exhibit completely different microscopic morphologies. With the gradual increase in the quality of absorbent cotton, the morphology of catalysts

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“…The compounds with N-oxide groups have several advantages over the parent pyridyl-N atom due to the presence of additional lone pairs in the N-oxide moiety, which could lead to enhanced interactions with solvent/guest molecules. For example, Xu et al showed that modified metal-organic frameworks with N-oxide moieties displayed enhanced C 2 H 2 and CO 2 adsorptions [35]. Compounds with pyridine-N-oxide moieties are an excellent organocatalyst in various racemic and enantioselective reactions and act as oxidant in various oxidation reactions [36].…”

Section: Introductionmentioning

confidence: 99%

Making and Breaking of Gels: Stimuli-Responsive Properties of Bis(Pyridyl-N-oxide Urea) Gelators

2021

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The structural modification of existing supramolecular architecture is an efficient strategy to design and synthesize supramolecular gels with tunable and predictable properties. In this work, we have modified bis(pyridyl urea) compounds with different linkers, namely hexylene and butylene, to their corresponding bis(pyridyl-N-oxide urea). The gelation properties of both the parent and the modified compounds were studied, and the results indicated that modification of the 3-pyridyl moieties to the corresponding 3-pyridyl-N-oxides induced hydrogelation. The stability of the parent and modified compounds were evaluated by sol-gel transition temperature (Tgel) and rheological measurements, and single-crystal X-ray diffraction was used to analyze the solid-state interactions of the gelators. The morphologies of the dried gels were analyzed by scanning electron microscopy (SEM), which revealed that the structural modification did not induce any prominent effect on the gel morphology. The stimuli-responsive behavior of these gels in the presence of salts in DMSO/water was evaluated by rheological experiments, which indicated that the modified compounds displayed enhanced gel strength in most cases. However, the gel network collapsed in the presence of the chloride salts of aluminum(III), zinc(II), copper(II), and cadmium(II). The mechanical strength of the parent gels decreased in the presence of salts, indicating that the structural modification resulted in robust gels in most cases. The modified compounds formed gels below minimum gel concentration in the presence of various salts, indicating salt-induced gelation. These results show the making and breaking ability of the gel network in the presence of external stimuli (salts), which explains the potential of using LMWGs based on N-oxide moieties as stimuli-responsive materials.

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Immobilization of N-oxide functionality into NbO-type MOFs for significantly enhanced C₂H₂/CH₄ and CO₂/CH₄ separations

Abstract: Two NbO-type MOFs with N-oxide functionality immobilized in the pore surface display significantly enhanced C2H2/CH4 and CO2/CH4 separation performance.

Cited by 73 publications

References 56 publications

An Isomeric Copper‐Diisophthalate Framework Platform for Storage and Purification of C₂H₂and Exploration of the Positional Effect of the Methyl Group

An Isomeric Copper‐Diisophthalate Framework Platform for Storage and Purification of C₂H₂and Exploration of the Positional Effect of the Methyl Group

MoP@C Supported on Absorbent Cotton as a Highly Efficient Catalyst towards Hydrodechlorination Reaction

Making and Breaking of Gels: Stimuli-Responsive Properties of Bis(Pyridyl-N-oxide Urea) Gelators

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Immobilization of N-oxide functionality into NbO-type MOFs for significantly enhanced C2H2/CH4 and CO2/CH4 separations

Abstract: Two NbO-type MOFs with N-oxide functionality immobilized in the pore surface display significantly enhanced C2H2/CH4 and CO2/CH4 separation performance.

Cited by 73 publications

References 56 publications

An Isomeric Copper‐Diisophthalate Framework Platform for Storage and Purification of C2H2and Exploration of the Positional Effect of the Methyl Group

An Isomeric Copper‐Diisophthalate Framework Platform for Storage and Purification of C2H2and Exploration of the Positional Effect of the Methyl Group

MoP@C Supported on Absorbent Cotton as a Highly Efficient Catalyst towards Hydrodechlorination Reaction

Making and Breaking of Gels: Stimuli-Responsive Properties of Bis(Pyridyl-N-oxide Urea) Gelators

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Immobilization of N-oxide functionality into NbO-type MOFs for significantly enhanced C₂H₂/CH₄ and CO₂/CH₄ separations

An Isomeric Copper‐Diisophthalate Framework Platform for Storage and Purification of C₂H₂and Exploration of the Positional Effect of the Methyl Group

An Isomeric Copper‐Diisophthalate Framework Platform for Storage and Purification of C₂H₂and Exploration of the Positional Effect of the Methyl Group