Amorphous lanthanide complexes for organic luminescent materials

DNA codons, consisting of triplet nucleotides (NTs), could play important roles for RNA transcription and protein translation in living systems. Therefore, their recognition could be seen important for diagnosis and therapy purposes. Based on triplet sequence formations of Adenine (A), Guanine (G), Cytosine (C) and Thymine (T) NTs, 64 codons were investigated in this work regarding their complexation with a molecular cubane (CUB) wire. To achieve this aim, each of singular 64 codons and CUB were optimized to be prepared for docking processes of complex formations. Hence, 64 complexes of codon-CUB were docked to see the recognition potency of CUB wire versus each of DNA codons. Interestingly, the obtained docking scores indicated that the CUB could work specifically versus the DNA codons, in which G-rich and A-rich triples were seen to be more favorable for complexation with CUB in comparison with other C-rich and T-rich triplet codons. Moreover, the results indicated that not pure G triplet but GAG codon was the most favorable one to be recognized by the CUB wire. However, pure T triplet was the worst one for such complex formations. The results of this work remarkably indicated that the CUB wire could work for recognition process of DNA codons from each other and such recognition could be very much specified for each of G-rich and A-rich codons, in which GAG codon was the best one among all the 64 investigated codons.

/pdf/dna-codon-recognition-by-a-cubane-wire-in-silico-approach-1s2stwl2rk.pdf

DNA Codon Recognition by a Cubane Wire: In Silico Approach

This work presents the hydrothermal synthesis and characterization of cerium phthalate coordination polymer, Ce-Phth CP, from the inorganic precursor cerium sulphate and the organic linker phthalic acid. Characterization of Ce-Phth CP by SEM/EDX, XRD, and FTIR analyses show that Ce-Phth CP particles are made of rectangular bundled straws of micrometre dimension and can be categorized as crystalline material with some amorphousness. FTIR analysis demonstrates successful coordination of Ce(IV) with phthalate via the Ce–O bond. Ce-Phth CP was applied successfully for advanced oxidation processes (AOP) to degrade the stable azo dye methyl orange (MO) via the Ce-Phth CP/H2O2 heterogeneous catalysis system where the effect of initial pH (2, 7, 10), MO initial concentration (10, 20, 30 ppm) and Ce-Phth CP dosage (50, 100, 200 mg) were studied. Results show that H2O2 best decomposes at pH 10 (about 89% decomposition), while MO best degrades at pH 7 (about 98% degradation). pHPZC of Ce-Phth CP was determined as pH 7.4 which has shown a significant effect on the whole process, decomposition and degradation. Adsorption natures of both H2O2 and MO onto the Ce-Phth CP surface are suggested to be the reason behind the difference in this pH profile of H2O2 decomposition and MO degradation·H2O2 decomposition is shown to follow a regular second-order rate equation, while MO degradation follows the usual pseudo-first-order rate equation. For a selected conditions, Ce-Phth CP/H2O2 system showed 5-cycles reuse for MO degradation decreasing from 89.7% to 73.5%. In some detail, proposed mechanisms for H2O2 decomposition and MO degradation and the inter-relation between them are introduced to account for the best degradation at initial pH 7. 

Cerium-phthalate coordination polymer as fenton-like durable catalyst for hydrogen peroxide activation and anionic organic dyes degradation in wastewater

Controlled bottom-up synthesis of amorphous coordination polymers with tailored metal coordination is a research field in its infancy. In this study, synthesis control was achieved to selectively prepare one-dimensional (1D) crystalline and amorphous zinc(II)-based coordination polymers and a dimeric molecular compound, all with similar coordination geometry as evidenced by X-ray diffraction and total scattering studies. The compounds were obtained by bottom up self-assembly of Zn(II) with terephthalate (tph2−) as linker and the enantiopure chelating ligand S-(1,2)-bis(1H-benzimidazol-2-yl)ethanol (L). The solvent and the coordination ability of the precursor zinc salt anion control the crystalline products formed by slow diffusion at room temperature: perchlorate allows isolation of the phase pure crystalline 1D polymer {[Zn(tph)(L)]·H2O·3DMF}n (1·H2O·3DMF, DMF = N,N-dimethylformamide). In contrast, zinc chloride leads to the formation of either a mixture of polymeric 1·H2O·3DMF and a dimeric molecular species [Zn2Cl2(tph)(L)2]·4DMF (2·4DMF), or to the phase pure dimer 2·4DMF, depending on the Zn(II) : tphH2 stoichiometry. A modified synthesis using zinc nitrate and fast precipitation by base addition results in an amorphous analogue of the 1D polymer (3). Chains of 1·H2O·3DMF pack into a non-porous crystalline material with a surface area of just 6 m2 g−1, while the outer surface area of amorphous polymer 3 is a factor of eight larger. Hence, the amorphous compound provides larger metal site accessibility for potential surface chemical reactions, while maintaining the coordination geometry of the metal sites. The temperature response of crystalline polymer 1·H2O·3DMF was studied using multi-temperature single crystal X-ray diffraction (100–300 K). The a = b axes display normal positive thermal expansion, while the c axis remains constant with increasing temperature due to partial relaxation of the terephthalate linkers and slightly changed geometry within the individual polymer chains.

Anion and solvent controlled growth of crystalline and amorphous zinc(ii) coordination polymers and a molecular complex.

Presently, an important step from basic research to practical applications is synthesizing nanostructured materials. Metal-organic structures, as well as coordination polymers, are a diverse group of materials with a wide range of potential and properties applications. It has been difficult to get these materials into commercial use because of many drawbacks. Polymers containing chelated units are described and assessed for their advancements and problems in preparation, properties, and structure. Here, a proposed approach based on designing coordination polymeric materials with chelated units using the metal-ligand approach (CPM-CU-MA) has been introduced for a columnar-layered plan, supramolecular components, and building levels. Nanocomposite materials can be formed through the thermal transformation of coordination polymers based on donor atoms. The polymeric metal chelates (PMCs) are categorized according to luminescent coordination polymer (LCoP) development. It is classified as macrocyclic intracomplex, polynuclear, and molecular according to its macrostructure. Supramolecular networks (SMNs) can be transformed into a coordination polymer by introducing cyclo-dehydrogenation of natural building blocks on a surface. The structure-property connections of LCPs can influence a framework of liquid crystal display (LCP) that has been given based on LC phase modulators with a large modulation depth and has useful applications in LC lens. In the spatial organization of PMCs, the main focus is on the commonalities and contrasts between higher- and lower-molecular-weight chelates based on molecularly imprinted sensors (MISs) and nanomaterial sensors for a wide range of uses. New functional nanoparticles based on the molecular components have exciting potential, as demonstrated by these findings based on parameters risk factors for human health, hazards reduction in the environment, lack of cost-effectiveness, environmental sustainability, and bioavailability of polymers with an overall performance of 95.3%.

https://downloads.hindawi.com/journals/jeph/2022/3937375.pdf

The Construct and Interpretation of Chelated Coordination Polymers and Their Use in Nanomaterials Research

A series of semicrystalline and amorphous one-dimensional (1D) polymeric chains consisting of cubane-like CoII4L4 units (L = S-1,2-bis(benzimidazol-2-yl)ethanol) and dicarboxylates were synthesized and characterized by single crystal diffraction and X-ray total scattering. The polycationic chains are composed of [Co4L4(dicarboxylate)]2+ monomeric units, while one molecular dicarboxylate counterion is balancing the charge of each monomer. The linear compound series has five members, and the crystal structures were solved for [Co4L4(tph)](tph) and [Co4L4(ndc)](ndc), where tph = terephthalate and ndc = 2,6-naphthalenedicarboxylate. Partly crystalline compounds were produced by slow assembly at elevated temperature (over days), while the amorphous compounds were formed by fast precipitation (within minutes). Pair distribution function (PDF) analysis based on X-ray total scattering data reveals the presence of the cubane-like entity in both the amorphous and semicrystalline samples. While the powders are non-porous, precipitation is a fast and versatile method to produce compounds with cubane-like centres with moderate surface areas of 17–49 m2 g−1 allowing for surface chemical reactions. The powders have a high concentration of Lewis base sites as verified by their selective adsorption of CO2 over N2. The use of an amorphous cubane-like polymer for the electrocatalytic oxygen evolution reaction was demonstrated.

Cubes on a string: a series of linear coordination polymers with cubane-like nodes and dicarboxylate linkers.

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Cubes on a string: a series of linear coordination polymers with cubane-like nodes and dicarboxylate linkers.

Anion and solvent controlled growth of crystalline and amorphous zinc(ii) coordination polymers and a molecular complex.