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The di-copper(II) analogue, [CuII2(bis-LEt)](BF4)2 (2), of the previously reported mono-copper(II) complex [CuIILEt]BF4 (1) which resulted in long lived electrocatalytic hydrogen evolution reaction (HER), has been prepared, characterised and tested for HER. The new bis-macrocycle, bis-HLEt, was formed from two HLEt Schiff base macrocycles (prepared by 1 + 1 condensation of 2,2'-iminobisbenzaldehyde and diethylenetriamine) being connected by selective alkylation of the less sterically hindered secondary alkyl amine group (NH) of each, using α,α'-dibromo-para-xylene to form a linker between them. The desired dicopper(II) complex, [Cu2II(bis-LEt)](BF4)2·4H2O (2·4H2O), was readily prepared, as a yellowish brown solid in 82% yield. SCXRD on yellow-brown crystals of [CuII2(bis-LEt)](BF4)2·2MeCN (2·2MeCN) revealed both copper(II) centres are square planar with a very similar copper(II) coordination environment to that of square planar 1. Although dicopper(II) complex 2 is easier to reduce than the analogous monocopper(II) complex 1 in MeCN (E1/2(ΔE) 2 -1.20(0.12) V, 1 -1.39(0.09) V, vs. 0.01 M AgNO3/Ag), electrocatalytic HER testing of dicopper complex 2·4H2O, in MeCN with 80 equivalents of acetic acid, revealed it was inactive, in stark contrast to the high and ongoing activity of 1 under the same conditions. So two is definitely not better than one metal ion in this case. Rather, it may be that the presence of an NH group in the macrocycle of 1, but absent in the bis-macrocycle of 2 (due to alkylating that NH to link the two macrocycles), may be key to the HER activity seen for 1.Proteases are excellent biomarkers for a variety of diseases, offer multiple opportunities for diagnostic applications and are valuable targets for therapy. From a chemistry-based perspective this review discusses and critiques the most recent advances in the field of substrate-based probes for the detection and analysis of proteolytic activity both in vitro and in vivo.Focusing on the synthesis of nickel-based materials (such as nickel sulfides, nickel hydroxides, and nickel oxides) is an urgent need in the fields of batteries, supercapacitors, and catalysis. However, their controlled synthesis still remains a great challenge because of the inadequate understanding of the control factor of their synthesis. A two-step solvo-/hydrothermal process with halide ion embedding/releasing was proposed to understand the effect of the halide ions on the synthesis and sulfidation of nickel hydroxy-halides. We find that the halide ions determine the formation, growth, and evolution of nickel hydroxy halides and promote them to form unique architectures and morphologies, leading to obvious differences in structural characteristics, including conductivity and electrochemical activity. Because of the presence of halide ions, a series of hybrids with multiple interfaces, which consist of hydroxides and sulfides and have various morphologies, such as flower-like balls, solid balls, porous balls, schistose, and thorny balls, with capacities ranging from 100.7 to 261.2 mA h g-1, can be easily obtained. It is fully demonstrated that the halide anion plays a core role in the synthesis process of nickel-based materials, and this finding will provide more chances for controllably synthesizing high-activity electrode materials.Tailoring novel thermoelectric materials (TEMs) with a high efficiency is challenging due to the difficulty in realizing both low thermal conductivity and high thermopower factor. In this work, we propose ternary chalcogenides CsAg5Q3 (Q = Te, Se) as promising TEMs based on first-principles calculations of their thermoelectric properties. Using lattice dynamics calculations within self-consistent phonon theory, we predict their ultralow lattice thermal conductivities below 0.27 W m-1 K-1, revealing the strong lattice anharmonicity and rattling vibrations of Ag atoms as the main origination. this website By using the mBJ exchange-correlation functional, we calculate the electronic structures with the direct band gaps in good agreement with experiments, and evaluate the charge carrier lifetime as a function of temperature within the deformation potential theory. Our calculations to solve Boltzmann transport equations demonstrate high thermopower factors of 2.5 mW m-1 K-2 upon p-type doping at 300 K, comparable to the conventional dichalcogenide thermoelectric GeTe. With these ultralow thermal conductivities and high thermopower factors, we determine a relatively high thermoelectric figure of merit ZT along the z-axis, finding the maximum value of ZTz to be 2.5 at 700 K for CsAg5Se3 by optimizing the hole concentration. Our computational results highlight the great potentiality of CsAg5Q3 (Q = Te, Se) for high-performance thermoelectric devices operating at room temperature.The ability to understand the function of a protein often relies on knowledge about its detailed structure. Sometimes, seemingly insignificant changes in the primary structure of a protein, like an amino acid substitution, can completely disrupt a protein's function. Long-lived proteins (LLPs), which can be found in critical areas of the human body, like the brain and eye, are especially susceptible to primary sequence alterations in the form of isomerization and epimerization. Because long-lived proteins do not have the corrective regeneration capabilities of most other proteins, points of isomerism and epimerization that accumulate within the proteins can severely hamper their functions and can lead to serious diseases like Alzheimer's disease, cancer and cataracts. Whereas tandem mass spectrometry (MS/MS) in the form of collision-induced dissociation (CID) generally excels at peptide characterization, MS/MS often struggles to pinpoint modifications within LLPs, especially when the differences are only isomally significant as other fragmentation techniques, like radical directed dissociation (RDD). In summary, the extent of backbone and side-chain fragments produced by CTD enabled the differentiation of isomers and epimers of Asp in a variety of peptides.Leukemia is a hematological malignancy associated with the uncontrolled proliferation of mutant progenitors, suppressing the production of normal blood cells. Current treatments, including chemotherapy, radiotherapy, and immunotherapy, still lead to unsatisfactory results with a 5 year survival rate of only 30-50%. The poor prognosis is related to both disease relapse and treatment-associated toxicity. Delivery strategies can improve the in vivo pharmacokinetics of drugs, navigating the therapeutics to target cells or the tumor microenvironment and reversing drug resistance, which maximizes tumor elimination and alleviates systematic adverse effects. This review discusses available FDA-approved anti-leukemia drugs and therapies with a focus on the advances in the development of anti-leukemia drug delivery systems. Additionally, challenges in clinical translation of the delivery strategies and future research opportunities in leukemia treatment are also included.Chiral pillar[5]arene-functionalized silica microspheres were prepared and characterized for the first time, and can be used as a new kind of chiral stationary phase for effective enantioseparation under reversed-phase and normal phase modes with good reproducibility and stability.Tropo(thio)ne-embedded homoHPHACs and their dications were synthesised by an electrophilic annulation of secoHPHAC and successive oxidation. 13C NMR spectra of the dications represented global 22π homoaromaticity via homoconjugation, while alkylation of a thiocarbonyl-bridged homoHPHAC produced a 24π antiaromatic monocation.The kinetics of the reactions of tributylphosphine with allenic and olefinic Michael acceptors in dichloromethane at 20 °C was followed by photometric and NMR spectroscopic methods. Combination with DFT-calculated methyl anion affinities revealed the relevance of retroaddition barriers in phosphine-catalysed reactions when mixtures of allenic and olefinic substrates are used.Developing new methods for efficiently detecting tetracycline antibiotics in water has gained much importance. In this work, zeolitic imidazolate framework-8 (ZIF-8) was used as a host to encapsulate carbon dots (CDs) and safranine T (ST) during its self-assembly process to synthesize CDs/ST@ZIF-8, which was then applied as the dual-emissive probe for detecting tetracycline antibiotics. Benefiting from the confinement effects of ZIF-8 and its fluorescence enhancement effects toward tetracycline (TC), a unique tandem Förster resonance energy transfer (FRET) system from CDs to TC and then to ST could be established, with a low limit of detection of 46 nM and excellent selectivity. More importantly, as compared to the CDs/ST system without tandem FRET, the sensitivity of the CDs/ST@ZIF-8 toward TC increased ∼69-fold, and naked eye recognition could also be achieved. Furthermore, by analyzing the R, G, and B values of photos containing different concentrations of tetracycline with the help of a mobile phone and correlating them with the concentration of tetracycline, we can perform the on-site detection of tetracycline, which is convenient, fast, and accurate. This study shows that new insight can be gained for the rational design and application of ratiometric fluorescence sensors based on tandem Förster resonance energy transfer in metal-organic framework materials.Herein, the influence of compositional engineering via active site alternation on catalytic behaviour has been studied for the Ruddlesden-Popper-based system Sm2-xSrxNiO4-δ. A phase change from orthorhombic (x = 0.6) to tetragonal (x = 1.0) in bulk Sm2-xSrxNiO4-δ is confirmed by Rietveld (XRD) analysis, thermogravimetric analysis (TGA) and X-ray photoelectron spectroscopy (XPS). To alter the active sites, we fabricated thin films for x = 0.6 and x = 1.0 using a pulsed laser deposition technique. The electrocatalytic behaviour has been studied in an environmentally friendly medium, i.e., a neutral medium (pH = 7), for both bulk and thin films, and parameters such as transient response, electrochemical reversibility and oxygen evolution reactivity are measured. The cyclic voltammetry curves suggest that electrochemical reversibility for thin films is governed by adsorption as opposed to the diffusion observed for bulk samples. Our investigation further suggests that moderate electroactivity can be achieved with an increase in active sites on miniaturization with the phase change.The mechanism for the photocatalytic activation of Pt(IV) anticancer prodrugs by riboflavin in the presence of NADH has been investigated by DFT. In the first step of the reaction, the oxidation kinetics of NADH to afford the catalytically active riboflavin hydroquinone is dramatically favoured by generation of the flavin triplet excited state. In the triplet, formation of a π-π stacked adduct promotes the hydride transfer from NADH to riboflavin with an almost barrierless pathway (2.7 kcal mol-1). In the singlet channel, conversely, the process is endergonic and requires overcoming a higher activation energy (19.2 kcal mol-1). In the second half of the reaction, the reduction of the studied Pt(IV) complexes by riboflavin hydroquinone occurs via an inner sphere mechanism, displaying free energy barriers smaller than 10 kcal mol-1. Pt reduction by bioreductants such as NADH and ascorbate involve instead less stabilized transition states (22.2-38.3 kcal mol-1), suggesting that riboflavin hydroquinone is an efficient reducing agent for Pt(IV) derivatives in biological settings.
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