6 research outputs found

    Pyrite (FeS2)-supported ultrafiltration system for removal of mercury (II) from water

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    This study investigated the Hg(II) removal efficiencies of the reactive adsorbent membrane (RAM) hybrid filtration process, a removal process that produces stable final residuals. The reaction mechanism between Hg(II) and pyrite and the rejection of the solids over time were characterized with respect to flux decline, pH change, and Hg and Fe concentration in permeate water. Effects of the presence of anions (Cl−, SO42−, NO3−) or humic acid (HA) on the rejection of the Hg(II)-contacted pyrite were studied. The presence of both HA and Hg(II) increased the rate of flux decline due to the formation of irreversible gel-like compact cake layers as shown in the experimental data and modeling related to the flux decline and the SEM images. Stability experiments of the final residuals retained on the membrane using a thiosulfate solution (Na2S2O3) show that the Hg(II)-laden solids were very stable due to little or no detection of Hg(II) in the permeate water. Experiment on the possibility of continuously removing Hg(II) by reusing the Hg/pyrite-laden membrane shows that almost all Hg(II) was adsorbed onto the pyrite surface regardless of the presence of salts or HA, and the Hg(II)-contacted pyrite residuals were completely rejected by the DE/UF system. Therefore, a membrane filter containing pyrite-Hg(II) could provide another reactive cake layer capable of further removal of Hg(II) without post-chemical treatment for reuse.Other Information Published in: Emergent Materials License: https://creativecommons.org/licenses/by/4.0See article on publisher's website: http://dx.doi.org/10.1007/s42247-021-00282-7</p

    Shape-Dependent Charge Transfers in Crystalline ZnO Photocatalysts: Rods versus Plates

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    ZnO particles with rod and plate configurations were synthesized using a solvothermal method using zinc acetate and zinc chloride, respectively. The surface of the as-synthesized ZnO rods and plates were characterized using various analysis tools (XRD, XPS, photoluminescence, FE-SEM, HR-TEM, BET, and UV–vis) and their photocatalytic activities were examined for six different redox reactions. The surface areas and bandgaps of the two ZnO samples were nearly identical; however, XPS and photoluminescence (PL) studies showed that the rods and the plates have relatively pronounced oxygen vacancy and oxygen interstitial contributions, respectively. ZnO rods were found to be active for the decomposition of methylene blue and phenol, the production of OH radicals, and the generation of photocurrents, all of which are associated with single-electron transfer reactions. On the other hand, ZnO plates were more effective for the production of molecular hydrogen and hydrogen peroxide, both of which are initiated by two-electron transfer reactions. These single versus multiple charge transfers are discussed with regard to the roles of oxygen vacancies and oxygen interstitials, which are located near the conduction and the valence bands, respectively

    Redox-Responsive Viologen-Mediated Self-Assembly of CB[7]-Modified Patchy Particles

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    Sulfonated surface patches of poly­(styrene)-based colloidal particles (CPs) were functionalized with cucurbit[7]­uril (CB[7]). The macrocycles served as recognition units for diphenyl viologen (DPV<sup>2+</sup>), a rigid bridging ligand. The addition of DPV<sup>2+</sup> to aqueous suspensions of the particles triggered the self-assembly of short linear and branched chainlike structures. The self-assembly mechanism is based on hydrophobic/ion-charge interactions that are established between DPV<sup>2+</sup> and surface-adsorbed CB[7]. DPV<sup>2+</sup> guides the self-assembly of the CPs by forming a ternary DPV<sup>2+</sup>⊂(CB­[7])<sub>2</sub> complex in which the two CB[7] macrocycles are attached to two different particles. Viologen-driven particle assembly was found to be both directional and reversible. Whereas sodium chloride triggers irreversible particle disassembly, the one-electron reduction of DPV<sup>2+</sup> with sodium dithionite causes disassembly that can be reversed via air oxidation. Thus, this bottom-up synthetic supramolecular approach allowed for the reversible formation and directional alignment of a 2D colloidal material

    Redox-Responsive Viologen-Mediated Self-Assembly of CB[7]-Modified Patchy Particles

    No full text
    Sulfonated surface patches of poly­(styrene)-based colloidal particles (CPs) were functionalized with cucurbit[7]­uril (CB[7]). The macrocycles served as recognition units for diphenyl viologen (DPV<sup>2+</sup>), a rigid bridging ligand. The addition of DPV<sup>2+</sup> to aqueous suspensions of the particles triggered the self-assembly of short linear and branched chainlike structures. The self-assembly mechanism is based on hydrophobic/ion-charge interactions that are established between DPV<sup>2+</sup> and surface-adsorbed CB[7]. DPV<sup>2+</sup> guides the self-assembly of the CPs by forming a ternary DPV<sup>2+</sup>⊂(CB­[7])<sub>2</sub> complex in which the two CB[7] macrocycles are attached to two different particles. Viologen-driven particle assembly was found to be both directional and reversible. Whereas sodium chloride triggers irreversible particle disassembly, the one-electron reduction of DPV<sup>2+</sup> with sodium dithionite causes disassembly that can be reversed via air oxidation. Thus, this bottom-up synthetic supramolecular approach allowed for the reversible formation and directional alignment of a 2D colloidal material

    Viologen-Based Conjugated Covalent Organic Networks via Zincke Reaction

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    Morphology influences the functionality of covalent organic networks and determines potential applications. Here, we report for the first time the use of Zincke reaction to fabricate, under either solvothermal or microwave conditions, a viologen-linked covalent organic network in the form of hollow particles or nanosheets. The synthesized materials are stable in acidic, neutral, and basic aqueous solutions. Under basic conditions, the neutral network assumes radical cationic character without decomposing or changing structure. Solvent polarity and heating method determine product morphology. Depending upon solvent polarity, the resulting polymeric network forms either uniform self-templated hollow spheres (<b>HS</b>) or hollow tubes (<b>HT</b>). The spheres develop via an inside-out Ostwald ripening mechanism. Interestingly, microwave conditions and certain solvent polarities result in the formation of a robust covalent organic gel framework (<b>COGF</b>) that is organized in nanosheets stacked several layers thick. In the gel phase, the nanosheets are crystalline and form honeycomb lattices. The use of the Zincke reaction has previously been limited to the synthesis of small viologen molecules and conjugated viologen oligomers. Its application here expands the repertoire of tools for the fabrication of covalent organic networks (which are usually prepared by dynamic covalent chemistry) and for the synthesis of viologen-based materials. All three materials<b>HT</b>, <b>HS</b>, and <b>COGF</b>serve as efficient adsorbents of iodine due to the presence of the cationic viologen linker and, in the cases of <b>HT</b> and <b>HS</b>, permanent porosity
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