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1.
Molecules ; 28(15)2023 Jul 31.
Artículo en Inglés | MEDLINE | ID: mdl-37570745

RESUMEN

Aiming at the generation of new functionalised thiosalicylate-based ionic liquids, a polymeric hydrogel consisting of 1-hexylimidazole propionitrile thiosalicylate [HIMP][TS], with a solid biomaterial support based on polyvinyl alcohol (PVA)-alginate beads, was produced. This study aimed to develop a treatment method for removing manganese (Mn) heavy metal from industrial wastewater, which is known to be toxic and harmful towards the environment and human health. The method utilised an adsorption-based approach with an alginate adsorbent that incorporated a functionalised thiosalicylate-based ionic liquid. The synthesised smooth round beads of PVA-alginate-[HIMP][TS] adsorbent were structurally characterised using Fourier transform infrared spectroscopy (FTIR) and field emission scanning electron microscopy (FESEM). The Mn concentration and removal efficiency were evaluated using atomic absorption spectroscopy (AAS). Three important parameters were evaluated: pH, adsorbent dosage, and contact time. During optimisation using the interactive factor design of experiments through the Box-Behnken model, the results showed that the system achieved a maximum Mn removal efficiency of 98.91% at an initial pH of 7.15, with a contact time of 60 min, using a bead dosage of 38.26 g/L. The beads were also tested in an available water filtration prototype system to illustrate their industrial application, and the performance showed a removal efficiency of 99.14% with 0 NTU total suspended solid (TSS) and 0.13 mg/L turbidity analysis. The recyclability of PVA-alginate-[HIMP][TS] beads using 0.5 M HCl resulted in four cycles with constant 99% Mn removal. The adsorption capacity of Mn was also determined in optimum conditions with 56 mg/g. Therefore, the alginate-thiosalicylate-based ionic liquid system is considered an effective and environmentally friendly method for removing Mn heavy metal due to the high removal efficiency achieved.

2.
J Colloid Interface Sci ; 572: 207-215, 2020 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-32244081

RESUMEN

Incorporation of isolated metal centers into well-organized nanostructures is a promising route in the development of the next generation of chemical, magnetic and electronic devices. In this work, a layer-by-layer protocol to grow highly ordered thin films of metal-decorated organic-inorganic cage-like polyhedral oligomeric silsesquioxane (POSS) is introduced. The key strategy is to use metal ions (Cu2+ or Fe3+) as linker for the amino-functionalized cage-like POSS, which are self-assembled between arachidic acid layers during Langmuir-Schaefer deposition. The Langmuir-Schaefer films are examined by X-ray photoelectron spectroscopy, X-ray diffraction, grazing incidence wide-angle X-ray scattering and extended X-ray absorption fine structure in order to understand how the coordination of metal ions influences the structure in the course of the layer-by-layer formation of the films.

3.
Materials (Basel) ; 13(1)2020 Jan 04.
Artículo en Inglés | MEDLINE | ID: mdl-31947932

RESUMEN

Tuning the architecture of multilayer nanostructures by exploiting the properties of their constituents is a versatile way to develop multifunctional films. Herein, we report a bottom-up approach for the fabrication of highly ordered hybrid films consisting of dimethyldioctadecylammonium (DODA), iron decorated polyhedral oligomeric silsesquioxanes (POSS), and montmorillonite clay platelets. Clay platelets provided the template where Fe/POSS moieties were grafted by the use of the surfactant. Driven by the iron ions present, DODA adopted a staggered arrangement, which is essential to realize the controllable layer-by-layer growth of the film. The elemental composition of the film was studied by X-ray photoelectron spectroscopy and X-ray reflectivity confirmed the existence of smooth interfaces between the different layers.

4.
Angew Chem Int Ed Engl ; 58(37): 13107-13112, 2019 Sep 09.
Artículo en Inglés | MEDLINE | ID: mdl-31342613

RESUMEN

Conductivity, carrier mobility, and a suitable Gibbs free energy are important criteria that determine the performance of catalysts for a hydrogen evolution reaction (HER). However, it is a challenge to combine these factors into a single compound. Herein, we discover a superior electrocatalyst for a HER in the recently identified Dirac nodal arc semimetal PtSn4 . The determined turnover frequency (TOF) for each active site of PtSn4 is 1.54 H2 s-1 at 100 mV. This sets a benchmark for HER catalysis on Pt-based noble metals and earth-abundant metal catalysts. We make use of the robust surface states of PtSn4 as their electrons can be transferred to the adsorbed hydrogen atoms in the catalytic process more efficiently. In addition, PtSn4 displays excellent chemical and electrochemical stabilities after long-term exposure in air and long-time HER stability tests.

5.
J Phys Chem Lett ; 10(11): 3171-3175, 2019 Jun 06.
Artículo en Inglés | MEDLINE | ID: mdl-31119942

RESUMEN

Two-dimensional (2D) perovskites incorporating hydrophobic organic spacer cations show improved film stability and morphology compared to their three-dimensional (3D) counterparts. However, 2D perovskites usually exhibit low photoluminescence quantum efficiency (PLQE) owing to strong exciton-phonon interaction at room temperature, which limits their efficiency in light-emitting diodes (LEDs). Here, we demonstrate that the device performance of 2D perovskite LEDs can be significantly enhanced by doping Mn2+ in (benzimidazolium)2PbI4 2D perovskite films to suppress the exciton-phonon interaction. The distorted [PbI6]4- octahedra by Mn-doping and the rigid benzimidazolium (BIZ) ring without branched chains in the 2D perovskite structure lead to improved crystallinity and rigidity of the perovskites, resulting in suppressed phonon-exciton interaction and enhanced PLQE. On the basis of this strategy, for the first time, we report yellow electroluminescence from free excitons in 2D ( n = 1) perovskites with a maximum brightness of 225 cd m-2 and a peak EQE of 0.045%.

6.
Inorg Chem ; 55(24): 12912-12922, 2016 Dec 19.
Artículo en Inglés | MEDLINE | ID: mdl-27989152

RESUMEN

Fe7Se8 exists as a hexagonal NiAs-like crystal structure with a large number of ordered intrinsic vacancies. It is an ideal candidate for studying the effect of defects on properties such as magnetism and electrical transport. In this work, highly crystalline Fe7Se8 with the 3c crystal structure was synthesized by a solid-state reaction. Sharp changes in the magnetization at 100 K confirm a rotation of the spins from the ab plane to the c axis with decreasing temperature. We observe an interesting metal-insulator transition at the same temperature as the spin-direction changes. We propose that locked spins in the grain boundaries induce electron localization and result in the metal-insulator transition. Electron localization is confirmed by X-ray photoelectron spectroscopy of the Fe 2p peaks, which exhibit two characteristic satellite peaks. This mechanism is also verified by comparing it with the properties of the 4c-Fe7Se8 crystal structure.

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