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Membrane-Supported Layered Coordination Polymer as an Advanced Sustainable Catalyst for Desulfurization.

ABSTRACT: The application of a catalytic membrane in the oxidative desulfurization of a multicomponent model diesel formed by most refractory sulfur compounds present in fuel is reported here for the first time. The catalytic membrane was prepared by the impregnation of the active lamellar [Gd(H₄nmp)(H₂O)₂]Cl·2H₂O (UAV-59) coordination polymer (CP) into a polymethyl methacrylate (PMMA, acrylic glass) supporting membrane. The use of the catalytic membrane in the liquid-liquid system instead of a powder catalyst arises as an enormous advantage associated with the facility of catalyst handling while avoiding catalyst mass loss. The optimization of various parameters allowed to achieve a near complete desulfurization after 3 h under sustainable conditions, i.e., using an aqueous H₂O₂ as oxidant and an ionic liquid as extraction solvent ([BMIM]PF₆, 1:0.5 ratio diesel:[BMIM]PF₆). The performance of the catalytic membrane and of the powdered UAV-59 catalyst was comparable, with the advantage that the former could be recycled successfully for a higher number of desulfurization cycles without the need of washing and drying procedures between reaction cycles, turning the catalytic membrane process more cost-efficient and suitable for future industrial application.

SUBMITTER: Mirante F

PROVIDER: S-EPMC8122353 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Enhanced proton conductivity in a layered coordination polymer.

Project description:[Gd(H4nmp)(H2O)2]Cl·2H2O (1) converts into [Gd2(H3nmp)2]·xH2O (2) (x = 1 to 4) with a notable increase in proton conductivity. 1 is a charged layered material counter balanced by chloride ions, with proton conductivity values of 1.23 × 10-5 S cm-1 at 98% relative humidity (RH) and 40 °C. At 98% RH and 94 °C the observed conductivity is 0.51 S cm-1, being to date one of the highest values ever reported for a proton-conducting coordination polymer. This increase is observed during a structural transformation into 2 that occurs at high temperature and RH. While this remarkable conductivity is observed only after transformation and by maintaining high humidity conditions, as-synthesized 2 also shows a conductivity value of 3.79 × 10-2 S cm-1 at 94 °C and 98% RH, still ranked as one of the highest reported values. Moreover, it is shown that the key factor for high proton conduction is the unusual dynamic structural transformation with water insertion and release of chloride ions.

| S-EPMC7448532 | biostudies-literature

A Cobalt Tandem Catalyst Supported on a Compressible Microporous Polymer Monolith.

Project description:A compressible microporous polymer monolith (MPM) was prepared by performing the Sonogashira-Hagihara reaction between 1,4-diiodobenzene and 1,3,5-triethynylbenzene in a gel state without stirring. MPM was functionalized via the click reaction with 1,3,5-tris(azidomethyl)-2,4,6-trimethylbenzene and 2,6-diethynylpyridine. MPM showed superhydrophobicity but became hydrophilic after the click reaction. The functionalized MPM (F-MPM) had polar triazole groups generated by the click reaction, which were used as coordination sites for Co(II) ions. Cobalt nanoparticles were loaded to F-MPM through in situ reduction of coordinated Co(II) ions to produce a monolithic Co heterogeneous catalyst (Co-MPM). The microscopic study showed that MPM, F-MPM, and Co-MPM consisted of fiber bundles, together with spherical particles on the micrometer scale. Co-MPM was used for tandem catalysis. Co-MPM promoted the reaction of dehydrogenation of ammonia borane and hydrogenation of nitro compounds in one pot to give amine products. The reactions with the compression and release process were much faster compared with the reactions performed under the stirring conditions, suggesting that the repeated compression and release facilitated interfacial contact between the reactants and active sites in Co-MPM.

| S-EPMC6644832 | biostudies-literature

A bio-inspired coordination polymer as outstanding water oxidation catalyst via second coordination sphere engineering.

Project description:First-row transition metal-based catalysts have been developed for the oxygen evolution reaction (OER) during the past years, however, such catalysts typically operate at overpotentials (η) significantly above thermodynamic requirements. Here, we report an iron/nickel terephthalate coordination polymer on nickel form (NiFeCP/NF) as catalyst for OER, in which both coordinated and uncoordinated carboxylates were maintained after electrolysis. NiFeCP/NF exhibits outstanding electro-catalytic OER activity with a low overpotential of 188 mV at 10 mA cm-2 in 1.0 KOH, with a small Tafel slope and excellent stability. The pH-independent OER activity of NiFeCP/NF on the reversible hydrogen electrode scale suggests that a concerted proton-coupled electron transfer (c-PET) process is the rate-determining step (RDS) during water oxidation. Deuterium kinetic isotope effects, proton inventory studies and atom-proton-transfer measurements indicate that the uncoordinated carboxylates are serving as the proton transfer relays, with a similar function as amino acid residues in photosystem II (PSII), accelerating the proton-transfer rate.

| S-EPMC6838099 | biostudies-literature

Ni-citric acid coordination polymer as a practical catalyst for multicomponent reactions.

Project description:Coordinative polymers (CP) are a subclass of Metal-organic frameworks (MOFs) with porous microstructures which have been widely synthesized in recent years and applied in various fields especially in catalysis science. In this work Coordinative polymers (CP) of nickel and citric acid (CA) was prepared as a new catalyst (Ni-CP) and applied in organic multicomponent reactions. The obtained catalyst was characterized by SEM, WDX, EDS, AAS, FT-IR, XRD and BET analysis. N2 adsorption-desorption isotherms indicate good BET surface area for Ni-CP; therefore can be employed as an efficient catalyst in multicomponent reactions for the synthesis of polyhydroquinoline and 2,3-dihydroquinazolin-4(1H)-one derivatives. Finally, this catalyst was recovered and reused several consecutive times.

| S-EPMC8714820 | biostudies-literature

Solar-Driven Hydrogen Peroxide Production Using Polymer-Supported Carbon Dots as Heterogeneous Catalyst.

Project description:Safe, sustainable, and green production of hydrogen peroxide is an exciting proposition due to the role of hydrogen peroxide as a green oxidant and energy carrier for fuel cells. The current work reports the development of carbon dot-impregnated waterborne hyperbranched polyurethane as a heterogeneous photo-catalyst for solar-driven production of hydrogen peroxide. The results reveal that the carbon dots possess a suitable band-gap of 2.98 eV, which facilitates effective splitting of both water and ethanol under solar irradiation. Inclusion of the carbon dots within the eco-friendly polymeric material ensures their catalytic activity and also provides a facile route for easy catalyst separation, especially from a solubilizing medium. The overall process was performed in accordance with the principles of green chemistry using bio-based precursors and aqueous medium. This work highlights the potential of carbon dots as an effective photo-catalyst.

| S-EPMC6199036 | biostudies-literature

Modulating plant growth-metabolism coordination for sustainable agriculture

Project description:Using ChIP-seq experiment, find the downstream genes and binding motif of NGR2.

2018-08-15 | GSE114287 | GEO

Heterometallic Coordination Polymer Gels Supported by 2,4,6-Tris(pyrazol-1-yl)-1,3,5-triazine.

Project description:Complexes of type [M(tpt)2]X2 (M2+ = Fe2+, Co2+, Ni2+; tpt = 2,4,6-tri{pyrazol-1-yl}-1,3,5-triazine; X- = BF4 - or ClO4 -) crystallize in a cubic lattice, with the metal ion and ligand conformation showing unusual symmetry-imposed disorder. Addition of 1 equiv AgX to the corresponding preformed [M(tpt)2]X2 salt in concentrated MeNO2 solution affords thixotropic gels. Gelation was not observed in analogous reactions using [Mn(tpt)2][ClO4]2, or from reactions in other, more donating solvents. Scanning electron microscopy (SEM) images from dilute solutions of the reagents confirmed the fibrous microstructure of the gels and their homogeneous elemental composition. However, energy-dispersive X-ray data show a reduced Fe/Ag ratio compared to the Co/Ag and Ni/Ag gels, where a 1:1 ratio of metals is evident. More concentrated gels decomposed to silver nanoparticles during SEM sample preparation. Mass spectrometry and 1H NMR indicate that silver induces partial ligand displacement reactions in [Fe(tpt)2]2+ and [Co(tpt)2]2+, but not in [Ni(tpt)2]2+. Hence, the strength of the gels, which follows the order M = Mn (no gel) < Fe < Co < Ni, correlates with the stability of octahedral [M(tpt)2]2+ under gelation conditions. Iron(II) complexes of the related ligands 2,4,6-tri{pyrazol-1-yl}pyridine (tpp) and 2,4,6-tri{pyrazol-1-yl}pyrimidine (tpym) did not undergo gelation with silver salts under the above conditions. The unique properties of tpt as a gelator in this work may reflect the crystallographically observed ability of metal-coordinated tpt to chelate to exogenous silver ions, through its pendant pyrazolyl group and triazinyl N donors. In contrast, the pendant azolyl substituents in silver complexes of the nongelators tpp and tpym only bind exogenous silver in monodentate fashion.

| S-EPMC6644042 | biostudies-literature

Gallium-containing polymer brush film as efficient supported Lewis acid catalyst in a glass microreactor.

Project description:Polystyrene sulfonate polymer brushes, grown on the interior of the microchannels in a microreactor, have been used for the anchoring of gallium as a Lewis acid catalyst. Initially, gallium-containing polymer brushes were grown on a flat silicon oxide surface and were characterized by FTIR, ellipsometry, and X-ray photoelectron spectroscopy (XPS). XPS revealed the presence of one gallium per 2-3 styrene sulfonate groups of the polymer brushes. The catalytic activity of the Lewis acid-functionalized brushes in a microreactor was demonstrated for the dehydration of oximes, using cinnamaldehyde oxime as a model substrate, and for the formation of oxazoles by ring closure of ortho-hydroxy oximes. The catalytic activity of the microreactor could be maintained by periodic reactivation by treatment with GaCl3.

| S-EPMC3778416 | biostudies-literature

Palladium Supported on Porous Organic Polymer as Heterogeneous and Recyclable Catalyst for Cross Coupling Reaction.

Project description:Palladium immobilized on an amide and ether functionalized porous organic polymer (Pd@AEPOP) is reported to be an effective heterogeneous catalyst for the Heck cross-coupling reaction of aryl iodides with styrene for the synthesis of diphenylethene derivatives. Excellent yields can be obtained using a 0.8 mol% Pd catalyst loading under the optimized reaction condition. The heterogeneous Pd@AEPOP catalyst can also be applied on the Suzuki reaction and the reduction of nitroarene.

| S-EPMC9332046 | biostudies-literature

Dynamic Polymer Networks: A New Avenue towards Sustainable and Advanced Soft Machines.

Project description:While the fascinating field of soft machines has grown rapidly over the last two decades, the materials they are constructed from have remained largely unchanged during this time. Parallel activities have led to significant advances in the field of dynamic polymer networks, leading to the design of three-dimensionally cross-linked polymeric materials that are able to adapt and transform through stimuli-induced bond exchange. Recent work has begun to merge these two fields of research by incorporating the stimuli-responsive properties of dynamic polymer networks into soft machine components. These include dielectric elastomers, stretchable electrodes, nanogenerators, and energy storage devices. In this Minireview, we outline recent progress made in this emerging research area and discuss future directions for the field.

| S-EPMC8248167 | biostudies-literature

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