The Royal Society of Chemistry最新文献

The development of high-energy-density Li metal batteries is limited by the uncontrollable growth of Li dendrites and an unstable Li/electrolyte interface during long-term Li plating/stripping. In this work, using high-concentration fluoroethylene carbonate (FEC) electrolyte, an LiF-rich interface layer was generated on the Li metal surface. This LiF-rich interface layer could effectively inactivate the high reactivity of the Li metal surface and suppress lithium dendrite growth, forming a uniform and dense structure at the Li/electrolyte interface to stabilize Li metal batteries. Owing to the enhanced interface stability offered by the high-concentration FEC electrolyte with LiFSI additive, the Li‖LiFePO₄ cell presented high capacity retention (89.1%) after 200 cycles at 1C (165 mA g⁻¹) and retained over 133.7 mA h g⁻¹ at 10C rate, whereas only 115.0 mA h g⁻¹ was achieved in the traditional carbonate ester electrolyte. The results show an obvious improvement in the cycle performance and rate capability of Li metal batteries containing a high-concentration FEC electrolyte with LiFSI as an additive.

A series of enone-hydrazones were synthesized through the reaction of enaminones with hydrazones under solvent-free, additive-free, and metal-catalyst-free conditions. The target products were obtained in high yields, with outstanding group tolerance, stereoselectivity, and chemical selectivity. In this work, a series of novel enaminone skeleton compounds were synthesized, and deuteration experiments showed that enone-hydrazones have different properties from traditional electron-deficient enketones.

Sulfinfinitenes, analogues of infinitene constructed from thiophene rings and assembled by applying a "cut-twist-restitch" sequence to two sulflowers, are explored through DFT calculations. The sulfinfinitene with 16 thiophene rings is only slightly more strained than the [8]sulflower, which has been synthesized, and can be considered as a promising synthetic target.

The properties of tissue interfaces - between separate populations of cells, or between a group of cells and its environment - has attracted intense theoretical, computational, and experimental study. Recent work on shape-based models inspired by dense epithelia have suggested a possible "topological sharpening" effect, by which four-fold vertices spatially coordinated along a cellular interface lead to a cusp-like restoring force acting on cells at the interface, which in turn greatly suppresses interfacial fluctuations. We revisit these interfacial fluctuations, focusing on the distinction between short length scale reduction of interfacial fluctuations and long length scale renormalized surface tension. To do this, we implement a spectrally resolved analysis of fluctuations over extremely long simulation times. This leads to more quantitative information on the topological sharpening effect, in which the degree of sharpening depends on the length scale over which it is measured. We compare our findings with a Brownian bridge model of the interface, and close by analyzing existing experimental data in support of the role of short-length-scale topological sharpening effects in real biological systems.

A new and highly efficient ring-closing metathesis-based strategy was developed for the synthesis of the cyclic urea 1,3-diazepinone, presenting significant improvement upon previous methods. Using a direct glycosylation approach, analogues of the potent cytidine deaminase (CDA) inhibitor diazepinone riboside were then synthesized including 2′-deoxyribo-, 2′-deoxy-2′-fluoroarabino-, and 2′-deoxy-2′,2′-difluoro-diazepinone nucleosides, all with moderate to good yield and excellent anomeric selectivity. Crucially, in contrast to the previous multistep linear synthesis of 2′-deoxyribo- and 2′-deoxy-2′-fluoroarabino-diazepinone nucleosides, this is the first report of direct glycosylation to access these nucleosides. Overall, we report efficient convergent routes to multiple 2′-modified-diazepinone nucleosides for further evaluation as CDA and potential APOBEC3 inhibitors.

Drug developers are currently focusing on investigating alternative strategies, such as “drug repositioning”, to address issues associated with productivity, regulatory obstacles, and the steadily rising cost of pharmaceuticals. Repositioning is the best strategy to stop searching for new drugs because it takes less time and money to investigate new indications for already approved or unsuccessful drugs. Although there are several potent Topo II inhibitors available on the market as important drugs used in the therapy of many types of cancer, more may be required in the future. The current inhibitors have drawbacks including acquired resistance and unfavorable side effects such as cardiotoxicity and subsequent malignancy. A substantial body of research documented the cytotoxic potential of experimental fluoroquinolones (FQs) on tumor cell lines and their remarkable efficacy against eukaryotic Topo II in addition to optimized physical and metabolic characteristics. The FQ scaffold has a unique ability to potentially resolve every major issue associated with traditional Topo II inhibitors while maintaining a highly desirable profile in crucial drug-likeness parameters; therefore, there is a significant chance that FQs will be repositioned as anticancer candidates. This review offers a summary of the most recent research on the anticancer potential of FQs that was published in 2023. Along with discussing structural activity relationship studies and the mechanism underlying their antiproliferative activity, this review aims to provide up-to-date information that will spur the development of more potent FQs as viable cancer treatment candidates.

The global problem of ecological safety and public health necessitates, the development of new sustainable ideas for pollution remediation. In recent development, metal–organic frameworks (MOF) are the emerging technology with remarkable potential, which have been employed in environmental remediation. MOFs are networks that are created by the coordination of metals or polyanions with ligands and contain organic components that can be customized. The interesting features of MOFs are a large surface area, tuneable porosity, functional diversity, and high predictability of pollutant adsorption, catalysis, and degradation. It is a solid material that occupies a unique position in the war against environmental pollutants. One of the main benefits of MOFs is that they exhibit selective adsorption of a wide range of pollutants, including heavy metals, organics, greenhouse gases, water and soil. Only particles with the right combination of pore size and chemical composition will achieve this selectivity, derived from the high level of specificity. Besides, they possess high catalytic ability for the removal of pollutants by means of different methods such as photocatalysis, Fenton-like reactions, and oxidative degradation. By generating mobile active sites within the framework of MOFs, we can not only ensure high affinity for pollutants but also effective transformation of toxic chemicals into less harmful or even inert end products. However, the long-term stability of MOFs is becoming more important as eco-friendly parts are replaced with those that can be used repeatedly, and systems based on MOFs that can remove pollutants in more than one way are fabricated. MOFs can reduce waste production, energy consumption as compared to the other removal process. With its endless capacities, MOF technology brings a solution to the environmental cleansing problem, working as a flexible problem solver from one field to another. The investigation of MOF synthesis and principles will allow researchers to fully understand the potential of MOFs in environmental problem solving, making the world a better place for all of us.

The ambiguous nature of non-innocent ligand catalysts provides an excellent strategy for developing an efficient catalyst system featuring extended applicability in sustainable catalysis. In this study, we unveil the catalytic activity of an NNN-Ru catalyst for lactic acid synthesis from a mixture of glycerol, ethylene glycol, and methanol. The developed strategy was also implemented to synthesize lactate (up to 80% yield) with good selectivity via the dehydrogenative upgradation of a crude glycerol and ethylene glycol mixture. As an extended utility, the method was utilized for lactate synthesis from triglyceride directly with hydrogen gas generation.

Correction for 'Cu(II)-Mediated aerobic oxidative synthesis of sulfonated chromeno[4,3-c]pyrazol-4(2H)-ones' by Quan Zhou et al., Org. Biomol. Chem., 2022, 20, 5575-5581, https://doi.org/10.1039/D2OB00639A.

Given that the hydration water of polymer matrices may differ from that of outermost polymer surfaces, processes at biomaterial-biofluid interfaces and role of hydration water therein cannot be adequately examined using most conventional characterization methods. To bridge this gap, a gold substrate was herein modified with linear and cyclic poly(2-methoxyethyl acrylate) to prepare gl-PMEA and gc-PMEA surfaces, respectively, as models for the outermost surfaces of blood-contacting medical devices. Both surfaces suppressed the adhesion of human platelets but differed in the adhesion behaviors of normal and tumor cells despite having the same areal density of fixed-end units. The surfaces were analyzed using quartz crystal microbalance (QCM), frequency modulation atomic force microscopy (FM-AFM), and X-ray emission spectroscopy (XES) measurements under wet conditions to clarify the relationship between bioresponsivity and hydration water. QCM measurements provided evidence that both grafted-PMEA were hydrated. FM-AFM observations revealed that the swelling layer was thicker for gc-PMEA. To rationalize the differences in the surface hydration states, we performed XES measurements under conditions enabling control over the number of hydration water molecules. In the low-water-content region, hydrogen bonds or interactions between water molecules developed in the vicinity of gl-PMEA but not gc-PMEA. Thus, the initial hydration behavior of the gc-PMEA surface, which promoted intermediate water formation, was different from that of the gl-PMEA surface. The results suggested that the adjustment and optimization of the hydration state of outermost biomaterial surfaces enable the control of bioresponsivity, including the selective isolation of tumor cells.