Browse
Submit Data
Databases
API
Help

Dataset Information

0 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Docking rings in a solid: reversible assembling of pseudorotaxanes inside a zirconium metal-organic framework.

ABSTRACT: An unprecedented zirconium metal-organic framework featuring a T-shaped benzimidazole strut was constructed and employed as a sponge-like material for selective absorption of macrocyclic guests. The neutral benzimidazole domain of the as-synthesized framework can be readily protonated and fully converted to benzimidazolium. Mechanical threading of [24]crown-8 ether wheels onto recognition sites to form pseudorotaxanes was evidenced by solution nuclear magnetic resonance, solid-state fluorescence, and infrared spectroscopy. Selective absorption of [24]crown-8 ether rather than its dibenzo counterpart was also observed. Further study reveals that this binding process is reversible and acid-base switchable. The success of docking macrocyclic guests in crystals via host-guest interactions provides an alternative route to complex functional materials with interpenetrated structures.

SUBMITTER: Li X

PROVIDER: S-EPMC9159108 | biostudies-literature | 2022 Jun

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Publications

Docking rings in a solid: reversible assembling of pseudorotaxanes inside a zirconium metal-organic framework.

Li Xia X Xie Jialin J Du Zhenglin Z Jiang Long L Li Guangqin G Ling Sanliang S Zhu Kelong K

Chemical science 20220502 21

An unprecedented zirconium metal-organic framework featuring a T-shaped benzimidazole strut was constructed and employed as a sponge-like material for selective absorption of macrocyclic guests. The neutral benzimidazole domain of the as-synthesized framework can be readily protonated and fully converted to benzimidazolium. Mechanical threading of [24]crown-8 ether wheels onto recognition sites to form pseudorotaxanes was evidenced by solution nuclear magnetic resonance, solid-state fluorescence ...[more]

PMID: 35733896

Similar Datasets

A reversible photochromic covalent organic framework.

Project description:Covalent organic frameworks are a type of crystalline porous materials that linked through covalent bond, and they have numerous potential applications in adsorption, separation, catalysis, and more. However, there are rarely relevant reported on photochromism. Fortunately, a hydrazone-linked DBTB-DETH-COF is rapidly generated through ultrasound method. The DBTB-DETH-COF is found to exhibit reversible photochromism (at least 50 cycles) from yellow to olive in the presence of light and air, and subsequently back to the original color upon heating. In addition, the structure of DBTB-DETH-COF remains unchanged after 15 days of light illumination. Furthermore, the reason of photochromic process is discussed by electron paramagnetic resonance, X-ray photoelectron spectroscopy, electrochemistry characterizations and transient absorption measurements. The reversible photochromic DBTB-DETH-COF can be used as anti-counterfeiting ink and optical switch in the presence of air. This work expands a stable organic photochromic material and broadens the applications of COFs.

| S-EPMC11448497 | biostudies-literature

Facile and reversible digestion and regeneration of zirconium-based metal-organic frameworks

Project description:The digestion/regeneration of metal-organic frameworks (MOFs) has important applications for catalysis, drug delivery, environmental decontamination, and energy storage, among other applications. However, research in this direction is limited and very challenging. Here, we develop a facile method to digest and regenerate a series of zirconium-based metal-organic frameworks (Zr-MOFs) by bicarbonate or carbonate salts. As an example, UiO-66 demonstrates well the mechanism of reversible digestion/regeneration processes. By analyzing the digested zirconium species via X-ray diffraction, Fourier transform infrared spectroscopy and Raman scattering spectroscopy, a digestion mechanism based on the formation of dissoluble complexes [Zr2(OH)2(CO3)4]2− is proposed. Impressively, ultrafine Pd nanoparticles can be extracted from Pd@PCN-224 via this strategy. This work, thus, may provide new insight for the development of renewable MOFs and their practical applications. The ability to digest and regenerate metal-organic frameworks is valuable for their application in catalysis and drug delivery, but challenging to achieve. Here, the authors develop a facile method to digest and regenerate a series of zirconium-based metal-organic frameworks using bicarbonate or carbonate salts.

| S-EPMC9812265 | biostudies-literature

Zirconium-based metal-organic framework gels for selective luminescence sensing.

Project description:Metal-organic gelation represents a promising approach to fabricate functional nanomaterials. Herein a series of Zr-carboxylate gels are synthesized from rigid pyrene, porphyrin and tetraphenyl ethylene-derived tetracarboxylate linkers, namely Zr-TBAPy (H4TBAPy = 1,3,6,8-tetrakis(4-carboxylphenyl)pyrene), Zr-TCPE (H4TCPE = 1,1,2,2-tetra(4-carboxylphenyl)ethylene), and Zr-TCPP (H4TCPP = 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin). The gels are aggregated from metal-organic framework (MOF) nanoparticles. Zr-TBAPy gel consists of NU-901 nanoparticles, and Zr-TCPP gel consists of PCN-224 nanoparticles. The xerogels show high surface areas up to 1203 m2 g-1. MOF gel films are also anchored on the butterfly wing template to yield Zr-MOF/B composites. Zr-TBAPy and Zr-TCPE gels are luminescent for solution-phase sensing and vapour-phase sensing of volatile organic compounds, and exhibit a significant luminescence quenching effect for electron-deficient analytes. Arising from the high porosity and good dispersion of luminescent MOF gels, rapid and effective vapour-sensing of nitrobenzene and 2-nitrotoluene within 30 s has been achieved via Zr-TBAPy film or Zr-TBAPy/B.

| S-EPMC9058640 | biostudies-literature

A porous, electrically conductive hexa-zirconium(iv) metal-organic framework.

Project description:Engendering electrical conductivity in high-porosity metal-organic frameworks (MOFs) promises to unlock the full potential of MOFs for electrical energy storage, electrocatalysis, or integration of MOFs with conventional electronic materials. Here we report that a porous zirconium-node-containing MOF, NU-901, can be rendered electronically conductive by physically encapsulating C60, an excellent electron acceptor, within a fraction (ca. 60%) of the diamond-shaped cavities of the MOF. The cavities are defined by node-connected tetra-phenyl-carboxylated pyrene linkers, i.e. species that are excellent electron donors. The bulk electrical conductivity of the MOF is shown to increase from immeasurably low to 10-3 S cm-1, following fullerene incorporation. The observed conductivity originates from electron donor-acceptor interactions, i.e. charge-transfer interactions - a conclusion that is supported by density functional theory calculations and by the observation of a charge-transfer-derived band in the electronic absorption spectrum of the hybrid material. Notably, the conductive version of the MOF retains substantial nanoscale porosity and continues to display a sizable internal surface area, suggesting potential future applications that capitalize on the ability of the material to sorb molecular species.

| S-EPMC5956983 | biostudies-literature

A robust zirconium amino acid metal-organic framework for proton conduction.

Project description:Proton conductive materials are of significant importance and highly desired for clean energy-related applications. Discovery of practical metal-organic frameworks (MOFs) with high proton conduction remains a challenge due to the use of toxic chemicals, inconvenient ligand preparation and complication of production at scale for the state-of-the-art candidates. Herein, we report a zirconium-MOF, MIP-202(Zr), constructed from natural α-amino acid showing a high and steady proton conductivity of 0.011 S cm-1 at 363 K and under 95% relative humidity. This MOF features a cost-effective, green and scalable preparation with a very high space-time yield above 7000 kg m-3 day-1. It exhibits a good chemical stability under various conditions, including solutions of wide pH range and boiling water. Finally, a comprehensive molecular simulation was carried out to shed light on the proton conduction mechanism. All together these features make MIP-202(Zr) one of the most promising candidates to approach the commercial benchmark Nafion.

| S-EPMC6250719 | biostudies-literature

Survival of Zirconium-Based Metal-Organic Framework Crystallinity at Extreme Pressures.

Project description:Recent research on metal-organic frameworks (MOFs) has shown a shift from considering only the crystalline high-porosity phases to exploring their amorphous counterparts. Applying pressure to a crystalline MOF is a common method of amorphization, as MOFs contain large void spaces that can collapse, reducing the accessible surface area. This can be either a desired change or indeed an unwanted side effect of the application of pressure. In either case, understanding the MOF's pressure response is extremely important. Three such MOFs with varying pore sizes (UiO-66, MOF-808, and NU-1000) were investigated using in situ high-pressure X-ray diffraction and Raman spectroscopy. Partial crystallinity was observed in all three MOFs above 10 GPa, along with some recovery of crystallinity on return to ambient conditions if the frameworks were not compressed above thresholds of 13.3, 14.2, and 12.3 GPa for UiO-66, MOF-808, and NU-1000, respectively. This threshold was marked by an unexpected increase in one or more lattice parameters with pressure in all MOFs. Comparison of compressibility between MOFs suggests penetration of the pressure-transmitting oil into MOF-808 and NU-1000. The survival of some crystallinity above 10 GPa in all of these MOFs despite their differing pore sizes and extents of oil penetration demonstrates the importance of high-pressure characterization of known structures.

| S-EPMC10324312 | biostudies-literature

An efficient modulated synthesis of zirconium metal-organic framework UiO-66.

Project description:The use of large amounts of deleterious solvents in the synthesis of metal-organic frameworks (MOFs) is one of the important factors limiting their application in industry. Herein, we present a detailed study of the synthesis of UiO-66, which was conducted with hydrobromic (HBr) acid as a modulator for the first time, at a high concentration of precursor solution (ZrCl4 and H2BDC, both 0.2 mol L-1). Powder crystals with atypical cuboctahedron structure were obtained which indicated that the HBr acid modulator played roles by competitive coordination and deprotonation modulation, thereby controlling the processes of nucleation and crystal growth. The properties of the obtained materials were systematically characterized and compared with those of materials synthesized with hydrofluoric (HF) acid and hydrochloric (HCl) acid modulators. Despite the high concentration of defectivity, the UiO-66 material synthesized with the HBr acid additive has the characteristics of larger specific surface area, excellent thermal stability and higher porosity in the structure. Besides that, the present protocol has the advantages of high reaction mass efficiency (RME), and feasibility of scalable synthesis, providing a facile and sustainable route to diverse Zr-based MOFs.

| S-EPMC8981973 | biostudies-literature

Assembling covalent organic framework membranes with superior ion exchange capacity.

Project description:Ionic covalent organic framework membranes (iCOFMs) hold great promise in ion conduction-relevant applications because the high content and monodispersed ionic groups could afford superior ion conduction. The key to push the upper limit of ion conductivity is to maximize the ion exchange capacity (IEC). Here, we explore iCOFMs with a superhigh ion exchange capacity of 4.6 mmol g-1, using a dual-activation interfacial polymerization strategy. Fukui function is employed as a descriptor of monomer reactivity. We use Brønsted acid to activate aldehyde monomers in organic phase and Brønsted base to activate ionic amine monomers in water phase. After the dual-activation, the reaction between aldehyde monomer and amine monomer at the water-organic interface is significantly accelerated, leading to iCOFMs with high crystallinity. The resultant iCOFMs display a prominent proton conductivity up to 0.66 S cm-1, holding great promise in ion transport and ionic separation applications.

| S-EPMC8866435 | biostudies-literature

Superior removal of arsenic from water with zirconium metal-organic framework UiO-66.

Project description:In this study, water stable zirconium metal-organic framework (UiO-66) has been synthesized and for the first time applied as an adsorbent to remove aquatic arsenic contamination. The as-synthesized UiO-66 adsorbent functions excellently across a broad pH range of 1 to 10, and achieves a remarkable arsenate uptake capacity of 303 mg/g at the optimal pH, i.e., pH = 2. To the best of our knowledge, this is the highest arsenate As(V) adsorption capacity ever reported, much higher than that of currently available adsorbents (5-280 mg/g, generally less than 100 mg/g). The superior arsenic uptake performance of UiO-66 adsorbent could be attributed to the highly porous crystalline structure containing zirconium oxide clusters, which provides a large contact area and plenty of active sites in unit space. Two binding sites within the adsorbent framework are proposed for arsenic species, i.e., hydroxyl group and benzenedicarboxylate ligand. At equilibrium, seven equivalent arsenic species can be captured by one Zr6 cluster through the formation of Zr-O-As coordination bonds.

| S-EPMC4642326 | biostudies-other

Host-Guest Interactions of Zirconium-Based Metal-Organic Framework with Ionic Liquid.

Project description:A metal-organic framework (MOF) is a three-dimensional crystalline compound made from organic ligands and metals. The cross-linkage between organic ligands and metals creates a network of coordination polymers containing adjustable voids with a high total surface area. This special feature of MOF made it possible to form a host-guest interaction with small molecules, such as ionic liquid (IL), which can alter the phase behavior and improve the performance in battery applications. The molecular interactions of MOF and IL are, however, hard to understand due to the limited number of computational studies. In this study, the structural parameters of a zirconium-based metal-organic framework (UiO-66) and 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, [EMIM][TFSI] were investigated via a combined experimental and computational approach using the linker model approach. When IL was loaded, the bond length and bond angle of organic linkers were distorted due to the increased electron density surrounding the framework. The increase in molecular orbital energy after confining IL stabilized the structure of this hybrid system. The molecular interactions study revealed that the combination of UiO-66 and [EMIM][TFSI] could be a promising candidate as an electrolyte material in an energy storage system.

| S-EPMC10055841 | biostudies-literature

OmicsDI is part of the ELIXIR infrastructure

OmicsDI is an Elixir interoperability service. Learn more ›

Tweets

OmicsDI Databases

PRIDE
PeptideAtlas
MassIVE
JPOST Repository
Physiome Model Repository

EGA
EVA
ENA
LINCS
PAXDB
Cell Collective

MetaboLights
Metabolomics Workbench
MetabolomeExpress
GNPS
BioModels
FAIRDOMHub

ArrayExpress
dbGaP
ExpressionAtlas
GEO
NODE

Information

Databases
Help
API
Contact us
Code on GitHub
Terms of use
Submit Data