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High-Quality Thin Films of UiO-66-NH₂ by Coordination Modulated Layer-by-Layer Liquid Phase Epitaxy.

ABSTRACT: We report the fabrication of macroscopically and microscopically homogeneous, crack-free metal-organic framework (MOF) UiO-66-NH₂ (UiO: Universitetet i Oslo; [Zr₆ O₄ (OH)₄ (bdc-NH₂ )₆ ]; bdc-NH₂ ^2- : 2-amino-1,4-benzene dicarboxylate) thin films on silicon oxide surfaces. A DMF-free, low-temperature coordination modulated (CM), layer-by-layer liquid phase epitaxy (LPE) using the controlled secondary building block approach (CSA). Efficient substrate activation was determined as a key factor to obtain dense and smooth coatings by comparing UiO-66-NH₂ thin films grown on ozone and piranha acid-activated substrates. Films of 2.60 μm thickness with a minimal surface roughness of 2 nm and a high sorption capacity of 3.53 mmol g^-1 MeOH (at 25 °C) were typically obtained in an 80-cycle experiment at mild conditions (70 °C, ambient pressure).

SUBMITTER: Semrau AL

PROVIDER: S-EPMC8251636 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Metal-organic framework (UiO-66 and UiO-66-NH2)-based adsorbents for bilirubin removal used in hemoperfusion.

Project description:Excessive accumulation of bilirubin in patients with hyperbilirubinemia can lead to tissue and organ damage and neurological diseases, and is even life-threatening in severe cases. Hemoperfusion is an effective method for removing bilirubin, but clinically used hemoperfusion adsorbents have unsatisfactory adsorption capacity and kinetics. In order to obtain a safe and efficient bilirubin adsorbent, Zr-based Metal-Organic Framework (MOF) material UiO-66 with high specific surface area and aqueous medium stability was prepared and modified with varying degrees of amination to improve its adsorption capacity. According to adsorption experiments in aqueous solution and simulated plasma, it was confirmed that the unsaturated coordinated zirconium in UiO-66 can effectively induce the aggregation and precipitation of free bilirubin unbound to albumin and the amino group on UiO-66-NH2 has a strong affinity for albumin bound bilirubin. The adsorption effect of UiO-66-NH2 with a high degree of amino modification is significantly stronger than that of UiO-66-NH2 with a low degree of modification. In simulated plasma with a bilirubin concentration of 40 mg dL-1, the adsorption capacities of UiO-66 and UiO-66-NH2-1.9 can reach 69.08 mg g-1 and 81.13 mg g-1. The adsorption isotherm fitting and adsorption kinetics fitting results also show that UiO-66 and UiO-66-NH2 are good adsorbents for bilirubin. In dynamic adsorption, the adsorbents also showed good performance and did not affect the protein in the plasma. The hemolysis test, coagulation time test, and cytotoxicity test confirmed that the bilirubin adsorbents based on UiO-66 and UiO-66-NH2 have good blood compatibility and biocompatibility. This study provides new ideas for the development of a novel bilirubin adsorbent and a theoretical basis for the study of bilirubin adsorption mechanisms.

| S-EPMC10691446 | biostudies-literature

All-gas-phase synthesis of UiO-66 through modulated atomic layer deposition.

Project description:Thin films of stable metal-organic frameworks (MOFs) such as UiO-66 have enormous application potential, for instance in microelectronics. However, all-gas-phase deposition techniques are currently not available for such MOFs. We here report on thin-film deposition of the thermally and chemically stable UiO-66 in an all-gas-phase process by the aid of atomic layer deposition (ALD). Sequential reactions of ZrCl4 and 1,4-benzenedicarboxylic acid produce amorphous organic-inorganic hybrid films that are subsequently crystallized to the UiO-66 structure by treatment in acetic acid vapour. We also introduce a new approach to control the stoichiometry between metal clusters and organic linkers by modulation of the ALD growth with additional acetic acid pulses. An all-gas-phase synthesis technique for UiO-66 could enable implementations in microelectronics that are not compatible with solvothermal synthesis. Since this technique is ALD-based, it could also give enhanced thickness control and the possibility to coat irregular substrates with high aspect ratios.

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Mixed-Matrix Membranes Formed from Imide-Functionalized UiO-66-NH2 for Improved Interfacial Compatibility.

Project description:Mixed-matrix membranes (MMMs) formed by dispersing metal-organic framework (MOF) particles in polymers have attracted significant attention because these composite systems can potentially surpass the separation performance of pure polymers alone. However, performance improvements are often unrealized because of poor interfacial compatibility between the MOF and the polymer, which results in interfacial defects. From a practical perspective, strategies are needed to address these defects so that MMMs can be deployed in real-world separation processes. From a fundamental perspective, strategies are needed to reliably form defect-free MMMs so that transport models can be applied to estimate pure MOF property sets, thereby enabling the development of robust structure-property relationships. To address these interfacial challenges, we have developed a method to surface-functionalize a UiO-66-NH2 MOF with a nanoscopic shell of covalently tethered 4,4'-(hexafluoroisopropylidene)diphthalic anhydride-Durene oligomers. When combined with a high-molecular-weight polymer of identical chemical structure to that of the imide-functional MOF surface, defect-free MMMs with uniform particle dispersions can be formed. With this technique, both permeabilities and selectivities of select gases in the MMMs were improved at loadings ranging from 5 to 40 wt %. At a 40 wt % loading, CO2 permeability and CO2/CH4 selectivity were enhanced by 48 and 15%, respectively. Additionally, pure MOF permeabilities for H2, N2, O2, CH4, and CO2 were predicted by the Maxwell model.

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Polyethyleneimine-Modified UiO-66-NH2(Zr) Metal-Organic Frameworks: Preparation and Enhanced CO2 Selective Adsorption.

Project description:UiO-66-NH2, a zirconium-based functional metal-organic framework (MOF), was postsynthetically modified via Schiff base reaction between aldehyde groups in glutaraldehyde and amino groups in UiO-66-NH2 and CO2-preabsorbed polyethyleneimine (PEI). The resulting PEI-modified MOFs, abbreviated as PEIC@UiO, were characterized with 1H NMR, Fourier transform infrared, powder X-ray diffraction, Brunauer-Emmett-Teller, scanning electron microscopy, and thermogravimetric analysis and evaluated as CO2 adsorbents. In comparison with pristine UiO-66-NH2, the PEIC@UiO adsorbents have reduced specific surface area (7-150 m2/g) but maintained the same crystal structure. Particularly, the PEIC96@UiO adsorbent exhibited significantly improved CO2/N2 adsorption selectivity (48 vs 25) and higher CO2 adsorption capacity (3.2 vs 2.7 mmol/g). The adsorbent also displayed moderate desorption energy (68 kJ/mol CO2), superior moisture endurance, and recyclability, which are very desirable for practical applications.

| S-EPMC6648867 | biostudies-literature

Towards metal-organic framework based field effect chemical sensors: UiO-66-NH2 for nerve agent detection.

Project description:We present a highly sensitive gas detection approach for the infamous 'nerve agent' group of alkyl phosphonate compounds. Signal transduction is achieved by monitoring the work function shift of metal-organic framework UiO-66-NH2 coated electrodes upon exposure to ppb-level concentrations of a target simulant. Using the Kelvin probe technique, we demonstrate the potential of electrically insulating MOFs for integration in field effect devices such as ChemFETs: a three orders of magnitude improvement over previous work function-based detection of nerve agent simulants. Moreover, the signal is fully reversible both in dry and humid conditions, down to low ppb concentrations. Comprehensive investigation of the interactions that lead towards this high sensitivity points towards a series of confined interactions between the analyte and the pore interior of UiO-66-NH2.

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Bio-Inspired Salinity-Gradient Power Generation With UiO-66-NH2 Metal-Organic Framework Based Composite Membrane.

Project description:Salinity-gradient directed osmotic energy between seawater and river water has been widely considered as a promising clean and renewable energy source, as there are numerous river estuaries on our planet. In the past few decades, reverse electrodialysis (RED) technique based on cation-selective membranes has been used as the key strategy to convert osmotic energy into electricity. From this aspect, developing high-efficiency anion-selective membranes will also have great potential for capturing osmotic energy, however, remains systematically unexplored. In nature, electric eels can produce electricity from ionic gradients by using their "sub-nanoscale" protein ion channels to transport ions selectively. Inspired by this, here we developed a UiO-66-NH2 metal-organic framework (MOF) based anion-selective composite membrane with sub-nanochannels, and achieved high-performance salinity-gradient power generation by mixing artificial seawater (0.5 M NaCl) and river water (0.01 M NaCl). The UiO-66-NH2 metal-organic framework based composite membranes can be easily and economically fabricated with dense structure and long-term working stability in saline, and its performance of power generation can also be adjusted by pH to enhance the surface charge density of the MOF sub-nanochannels. This study will inspire the exploitation of MOFs for investigating the sub-nanochannel directed high-performance salinity-gradient energy harvesting systems based on anion-selective ion transport.

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High Gas Permeability in Aged Superglassy Membranes with Nanosized UiO-66-NH2 /cPIM-1 Network Fillers.

Project description:Superglassy membranes synthesised by polymers of intrinsic microporosity (PIMs) suffer from physical aging and show poor gas permeance over time, especially thin membranes, due to the fast rearrangement of nonequilibrium polymer chains. Herein, we constructed a novel PIM-1 thin film nanocomposite membrane (TFN) using nanosized UiO-66-NH2 (≈10 nm)/carboxylated PIM-1 (cPIM-1) as the composite filler. Unlike conventional fillers, which interact with the polymer only via the surface, the UiO-66-NH2 /cPIM-1 forms a stable three-dimensional (3D) network intertwining with the polymer chains, being very effective to impede chain relaxation, and thus physical aging. Nanosizing of UiO-66-NH2 was achieved by regulating the nucleation kinetics using carbon quantum dots (CQD) during the synthesis. This led to increased surface area, and hence more functional groups to bond with cPIM-1 (via hydrogen bonding between -NH2 and -COOH groups), which also improved interfacial compatibility between the 3D network and polymer chains avoiding defect formation. As a result, the novel TFN showed significantly improved performance in gas separation along with reduced aging (i.e. ≈6 % loss in CO2 permeability over 63 days); the aged membranes had a CO2 permeance of 2504 GPU and ideal selectivity values of 37.2 and 23.8 for CO2 /N2 and CO2 /CH4 , respectively.

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Liquid-Phase Quasi-Epitaxial Growth of Highly Stable, Monolithic UiO-66-NH2 MOF thin Films on Solid Substrates.

Project description:High quality, monolithic UiO-66-NH2 thin films on diverse solid substrates have been prepared via a low temperature liquid phase epitaxy method. The achievement of continuous films with low defect densities and great stability against high temperatures and hot water is proven, clearly outperforming other reported types of MOF thin films.

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Improvement of anti-corrosion performance of an epoxy coating using hybrid UiO-66-NH2/carbon nanotubes nanocomposite.

Project description:In this study, a porous nanocontainer from UiO-66-NH2/CNTs nanocomposite with an excellent barrier characteristics was constructed through amine-functionalized Zr-based metal organic framework. The characterization of the prepared nano-materials were performed using different analyses such as FTIR, XRD, SEM, EDS, TEM, and BET and the results proved the successful synthesize of UiO-66-NH2/CNTs nanocomposite. The corrosion protection performance of the coated panels was investigated by electrochemical impedance spectroscopy (EIS), salt spray, and contact angle measurement. The EIS results revealed that unmodified and UiO-66-NH2 containing coating in 3.5 wt.% NaCl electrolyte were failed after 45 days but the corrosion was negligible in UiO-66-NH2/CNTs coating due to high pore resistance values even after 45 days. Salt spray and contact angle measurements confirmed that UiO-66-NH2/CNTs containing coating acts as an efficient barrier against wet saline environment even at long exposure times. This is attributed to uniform dispersion in the epoxy matrix and formation of a uniform nanocomposite coating.

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TpBD/UiO-66-NH2 micro-mesoporous hybrid material as a stationary phase for open tubular capillary electrochromatography.

Project description:The excellent stability of covalent organic frameworks (COFs) and the diversity of metal organic frameworks (MOFs) make MOF/COF hybrid materials promising candidates for chromatographic stationary phases. In this paper, a TpBD/UiO-66-NH2 hybrid material was synthesized through a Schiff-base reaction between TpBD COFs and UiO-66-NH2 MOFs; characterized using Fourier-transform infrared spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy; and bonded to a capillary to prepare a TpBD/UiO-66-NH2-bonded open tubular capillary electrochromatography (OT-CEC) column. Results suggested that the hybrid material had the crystal morphology of a single COF and MOF, a micro-mesoporous structure, and good thermal stability. The inner surface of the OT-CEC column was tightly and uniformly distributed with the stationary phase (∼1.5 μm). The baseline separation of 13 amino acids and three families (4 acidic antibiotics, 4 preservatives and 6 sulfonamides) of emerging pollutant mixtures was achieved due to the synergistic effect of TpBD and UiO-66-NH2 in the stationary phase. The OT-CEC column showed good reproducibility and stability with relative standard deviations of migration time and resolutions in the range of 1.17-3.93% and 1.79-4.31%, respectively.

| S-EPMC11369885 | biostudies-literature