Hydrolytically stable fluorinated metal-organic frameworks for energy-efficient dehydration

Cadiau, Amandine; Belmabkhout, Youssef; Adil, Karim; Bhatt, Prashant M.; Pillai, Renjith S.; Shkurenko, Aleksander; Martineau‐Corcos, Charlotte; Maurin, Guillaume; Eddaoudi, Mohamed

doi:10.1126/science.aam8310

Cited by 326 publications

(268 citation statements)

References 44 publications

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“…Anion‐pillared ultramicroporous materials are 3D Cu/Ni/Zn coordination networks containing 2D nets of a metal node and an organic linker that are bridged by the anions, like SiF 6 2− , NbOF 5 2− , TiF 6 2− , or AlF 5 2− , which have showed their great potential in gas separation . Three SiF 6 2− (SIFSIX) pillared porous materials with different organic linkers and net interpenetration, SIFSIX‐1‐Cu (1 = 4,4′‐bipyridine), interpenetrated SIFSIX‐2‐Cu‐i (2 = 4,4‐dipyridylacetylene, i = interpenetrated), and SIFSIX‐3‐Ni (3 = pyrazine) were synthesized for C 3 H 4 capture.…”

Section: Methodsmentioning

confidence: 99%

A Single‐Molecule Propyne Trap: Highly Efficient Removal of Propyne from Propylene with Anion‐Pillared Ultramicroporous Materials

et al. 2018

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Propyne/propylene (C H /C H ) separation is a critical process for the production of polymer-grade C H . However, optimization of the structure of porous materials for the highly efficient removal of C H from C H remains challenging due to their similar structures and ultralow C H concentration. Here, it is first reported that hybrid ultramicroporous materials with pillared inorganic anions (SiF = SIFSIX, NbOF = NbOFFIVE) can serve as highly selective C H traps for the removal of trace C H from C H . Especially, it is revealed that the pyrazine-based ultramicroporous material with square grid structure for which the pore shape and functional site disposition can be varied in 0.1-0.5 Å scale to match both the shape and interacting sites of guest molecule is an interesting single-molecule trap for C H molecule. The pyrazine-based single-molecule trap enables extremely high C H uptake under ultralow concentration (2.65 mmol g at 3000 ppm, one C H per unit cell) and record selectivity over C H at 298 K (>250). The single-molecule binding mode for C H within ultramicroporous material is validated by X-ray diffraction experiments and modeling studies. The breakthrough experiments confirm that anion-pillared ultramicroporous materials set new benchmarks for the removal of ultralow concentration C H (1000 ppm on SIFSIX-3-Ni, and 10 000 ppm on SIFSIX-2-Cu-i) from C H .

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Section: Methodsmentioning

confidence: 99%

A Single‐Molecule Propyne Trap: Highly Efficient Removal of Propyne from Propylene with Anion‐Pillared Ultramicroporous Materials

et al. 2018

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“…Although the stability of these MOFs has not been commonly studied, they are expected to show relatively weaker stability compared to the MOFs with only one linker, which is similar to the trend of mixed donor linkers based MOFs. However, some stable mixed ligand MOFs based on +2 metal cations, pyridyl ligands and coordinating anions were documented . For example, a series of isoreticular MOFs, SIFSIX‐ n ‐Cu ( n = 1, 2, and 3), NbOFFIVE‐1‐Ni, and AlFFIVE‐1‐Ni, have shown great potentials toward gas storage and separation.…”

Section: Stable Metal–organic Frameworkmentioning

confidence: 99%

Stable Metal–Organic Frameworks: Design, Synthesis, and Applications

et al. 2018

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Metal-organic frameworks (MOFs) are an emerging class of porous materials with potential applications in gas storage, separations, catalysis, and chemical sensing. Despite numerous advantages, applications of many MOFs are ultimately limited by their stability under harsh conditions. Herein, the recent advances in the field of stable MOFs, covering the fundamental mechanisms of MOF stability, design, and synthesis of stable MOF architectures, and their latest applications are reviewed. First, key factors that affect MOF stability under certain chemical environments are introduced to guide the design of robust structures. This is followed by a short review of synthetic strategies of stable MOFs including modulated synthesis and postsynthetic modifications. Based on the fundamentals of MOF stability, stable MOFs are classified into two categories: high-valency metal-carboxylate frameworks and low-valency metal-azolate frameworks. Along this line, some representative stable MOFs are introduced, their structures are described, and their properties are briefly discussed. The expanded applications of stable MOFs in Lewis/Brønsted acid catalysis, redox catalysis, photocatalysis, electrocatalysis, gas storage, and sensing are highlighted. Overall, this review is expected to guide the design of stable MOFs by providing insights into existing structures, which could lead to the discovery and development of more advanced functional materials.

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“…The scientific community has intensified its efforts over the last decades to develop novel porous adsorbents able to address societal issues including air purification, wastewater treatment, natural gas upgrading, etc. [1][2][3] . Among them, metal-organic frameworks (MOFs) appear as a promising family of custom-designed adsorbents able to efficient capture strategic gases of utmost importance in diverse energy and environment-related applications.…”

mentioning

confidence: 99%

Peculiar Molecular Shape and Size Dependence of the Dynamics of Fluids Confined in a Small-Pore Metal–Organic Framework

Skarmoutsos

Eddaoudi

Maurin

2018

J. Phys. Chem. Lett.

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Force-field-based molecular dynamics simulations were deployed to systematically explore the dynamics of confined molecules of different shapes and sizes, that is, linear (CO and N) and spherical (CH) fluids, in a model small pore system, that is, the metal-organic framework SIFSIX-2-Cu-i. These computations unveil an unprecedented molecular symmetry dependence of the translational and rotational dynamics of fluids confined in channel-like nanoporous materials. In particular, this peculiar behavior is reflected by the extremely slow decay of the Legendre reorientational correlation functions of even-parity order for the linear fluids, which is associated with jump-like orientation flips, while the spherical fluid shows a very fast decay taking place on a subpicosecond time scale. Such a fundamental understanding is relevant to diverse disciplines such as in chemistry, physics, biology, and materials science, where diatomic or polyatomic molecules of different shapes/sizes diffuse through nanopores.

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Hydrolytically stable fluorinated metal-organic frameworks for energy-efficient dehydration

Cited by 326 publications

References 44 publications

A Single‐Molecule Propyne Trap: Highly Efficient Removal of Propyne from Propylene with Anion‐Pillared Ultramicroporous Materials

A Single‐Molecule Propyne Trap: Highly Efficient Removal of Propyne from Propylene with Anion‐Pillared Ultramicroporous Materials

Stable Metal–Organic Frameworks: Design, Synthesis, and Applications

Peculiar Molecular Shape and Size Dependence of the Dynamics of Fluids Confined in a Small-Pore Metal–Organic Framework

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