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The use of Metal-Organic Frameworks as crystalline matrices for the synthesis of multiple component or multivariate solids by the combination of different linkers into a single material has emerged as a versatile route to tailor the properties of single-component phases or even access new functions. This approach is particularly relevant for Zr-MOFs due to the synthetic flexibility of this inorganic node. However, the majority of materials are isolated as polycrystalline solids, which are not ideal to decipher the spatial arrangement of parent and exchanged linkers for the formation of homogeneous structures or heterogeneous domains across the solid. Here we use high-throughput methodologies to optimize the synthesis of single crystals of UiO-68 and UiO-68-TZDC, a photoactive analogue based on a tetrazine dicarboxylic derivative. The analysis of the single linker phases reveals the necessity of combining both linkers to produce multivariate frameworks that combine efficient light sensitization, chemical stability, and porosity, all relevant to photocatalysis. We use solvent-assisted linker exchange reactions to produce a family of UiO-68-TZDC binary frameworks, which respect the integrity and morphology of the original crystals. Our results suggest that the concentration of TZDC in solution and the reaction time control the distribution of this linker in the sibling crystals for a uniform mixture or the formation of core-shell domains. We also demonstrate how the possibility of generating an asymmetric distribution of both linkers has a negligible effect on the electronic structure and optical band gap of the solids but controls their performance for drastic changes in the photocatalytic activity toward proton or methyl viologen reduction.
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http://dx.doi.org/10.1021/jacs.0c09015 | DOI Listing |
Heliyon
December 2024
Mechanical Engineering Department, Faculty of Engineering, Brawijaya University, MT Haryono167, Malang, 65145, Indonesia.
Industrial organic dyes represent a significant portion of pollutants discharged into the environment, particularly by the textile industry. These compounds pose serious threats to living organisms due to their high toxicity. Various techniques have been explored for the degradation of organic dyes, among which heterogeneous photocatalysis utilising titanium dioxide (TiO) stands out as a promising technology.
View Article and Find Full Text PDFHeliyon
December 2024
Department of Applied Chemistry, School of Applied Natural Science, Adama Science and Technology University, P.O. Box 1888, Adama, Ethiopia.
The pristine phases SS1(ZnO), SS2(MnO), and SS3 (CuO) photocatalysts and mixed phases of ZnO-based nanocomposites were synthesized by the sol-gel method. Whereas SS4 (g-CN) was prepared through polymerization of urea. The synthesized photocatalysts were characterized using TGA-DTA, XRD, DRS, PL, DLS, FTIR, SEM, TEM, and HRTEM.
View Article and Find Full Text PDFInorg Chem
December 2024
School of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, P. R. China.
In semiconductor catalysts, rational doping of nonmetallic elements holds significant scientific and technological importance for enhancing photocatalytic performance. Here, using a one-step hydrothermal technique, we synthesized iodine-doped BiOCl composite and evaluated the impact of iodine doping on its photocatalytic capability for organic dye degradation under visible light irradiation. In this study, we demonstrate that the introduction of iodide ions not only provides an ideal built-in electric field (BIEF) for BiOCl but also induces the generation of additional oxygen vacancies (OVs).
View Article and Find Full Text PDFJ Colloid Interface Sci
December 2024
School of Chemical Engineering, The University of Adelaide, North Terrace, Adelaide, SA 5005, Australia. Electronic address:
Photocatalytic oxygen evolution reaction (OER) is pivotal for sustainable energy systems yet lacks high-performance catalysts capable of strong visible light absorption, robust charge dynamics, fast reaction kinetics, and high oxidation capability. Herein, we report the multiscale optimization of carbon nitride through the construction of porous curled carbon nitride nanosheets (CNA-B30) incorporating boron center/cyano group Lewis acid-base pairs (LABPs). The unique chemical and structural features of CNA-B30 extended the photoabsorption edges of π → π* and n → π* electronic transitions to 470 nm and 715 nm, respectively.
View Article and Find Full Text PDFJ Colloid Interface Sci
December 2024
Key Laboratory of Green Chemical Process of Ministry of Education, School of Chemistry and Environmental Engineering, Wuhan Institute of Technology, Wuhan 430205, PR China. Electronic address:
Employing metallic nanoclusters as cocatalysts for semiconductor-based photocatalysts and understanding their roles in enhancing photocatalytic performance is crucial. Herein, a nickel thiolate with cyclohexanethiol as the ligands (i.e.
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