Strategy For Synthesis Research Articles

Iron-catalysed stereoselective NH transfer enables dynamic kinetic resolution of sulfoxides

Transition metal-catalysed asymmetric nitrene transfer provides a powerful means to access various bioactive N-containing compounds as single enantiomers. However, enantioselective NH transfer that allows concise assembly of unprotected enantioenriched amines remains an enduring challenge. We report here an iron-catalysed stereoselective NH imidation of sulfoxide, which is integrated with photocatalytic racemisation of sulfoxide, enabling a dynamic kinetic resolution (DKR) strategy for direct and asymmetric synthesis of NH-sulfoximines. This approach is distinct from the existing methods by avoiding protecting group manipulations and/or the use of chiral substrates. Computational studies on the NH imidation reaction suggest the involvement of an iron-aminyl radical intermediate, and its reaction with sulfoxide proceeds through a synchronous nucleophilic addition of sulfoxide to nitrogen center and ligand-to-metal single electron transfer process to form the N–S bond. In addition, the stereoselectivity is primarily dictated by the difference in dispersion interactions of the transition states.

Electrochemical Cyclopropanation of Unactivated Alkenes with Methylene Compounds

AbstractCyclopropanes are prevalent in natural products, pharmaceuticals, and bioactive compounds, functioning as a significant structural motif. Although a series of methods have been developed for the construction of the cyclopropane skeleton, the development of a direct and efficient strategy for the rapid synthesis of cyclopropanes from bench‐stable starting materials with a broad substrate scope and functional group tolerance remains challenging and highly desirable. Herein, we present an electrochemical method for the direct cyclopropanation of unactivated alkenes using active methylene compounds. The strategy shows a broad substrate scope with a high level of functional group compatibility, as well as potential application as demonstrated by late‐stage cyclopropanation of complex molecules and drug derivatives. Further mechanistic investigations suggest that Cp2Fe (Fc) plays an essential role as an oxidative mediator in generating radicals from active methylene compounds.

Electrochemical Cyclopropanation of Unactivated Alkenes with Methylene Compounds.

Cyclopropanes are prevalent in natural products, pharmaceuticals, and bioactive compounds, functioning as a significant structural motif. Although a series of methods have been developed for the construction of the cyclopropane skeleton, the development of a direct and efficient strategy for the rapid synthesis of cyclopropanes from bench-stable starting materials with a broad substrate scope and functional group tolerance remains challenging and highly desirable. Herein, we present an electrochemical method for the direct cyclopropanation of unactivated alkenes using active methylene compounds. The strategy shows a broad substrate scope with a high level of functional group compatibility, as well as potential application as demonstrated by late-stage cyclopropanation of complex molecules and drug derivatives. Further mechanistic investigations suggest that Cp2Fe (Fc) plays an essential role as an oxidative mediator in generating radicals from active methylene compounds.

Size-Tunable Covalent Organic Framework Nanoparticles for Assembling One-Dimensional Photonic Crystals With Visual Sensing.

One-dimensional photonic crystals (1D PCs) emerged as superb sensing platforms due to their high sensitivity to environmental changes. However, effectively translating the microscopic interactions between covalent organic frameworks (COFs) and analytes into macroscopic optical responses via 1D PCs for intuitive detection presents a significant challenge. Here, we propose a stepwise-induced synthesis strategy that for the first time achieves a size-controlled synthesis of uniform nanoscale COFs (60-80nm), leading to a high-quality COF layer. This advancement enables COF-based 1D PCs to exhibit diverse color variations and controllable saturation. Notably, the excellent compatibility of the COF layer with inorganic oxides, organic polymers, and metal-organic frameworks (MOFs) results in these 1D PCs exhibiting bright colors. Crucially, introducing the mesoporous materials enables 1D PCs to achieve deep integration of adsorption and recognition functions for volatile organic compounds (VOCs). The fabricated COF/MOF 1D PC allows differentiation of 12 VOCs and visually detects VOCs at different concentrations (0-80gm- 3) through color changes, with a response time under 1 s. In particular, COF-based 1D PCs can be transferred to flexible substrates while retaining VOC visual sensing. These attributes highlight the potential of COF-based 1D PCs for real-time VOC monitoring in industrial environments.

A Rapid and Surfactant-Free Synthesis Strategy for Variously Faceted Cuprous Oxide Polyhedra

We systematically investigated the morphology-controlled synthesis of Cu2O micro-nano crystals, especially under surfactant-free conditions, targeting a simple, rapid, and morphologically controllable preparation strategy for polyhedral Cu2O micro-nano crystals. By systematically investigating the effects of NaOH concentration, types of reducing agents, and copper salt precursors on crystal growth, precise control over the morphology of Cu2O crystals under surfactant-free conditions was achieved. This method can rapidly prepare variously faceted Cu2O crystals under mild conditions (70 °C, 7 min), including regular polyhedra with low-index facets exposure including cubes, octahedra and rhombic dodecahedra, as well as more complex polyhedra with high-index facets exposure such as 18-faceted, 26-faceted, 50-faceted and 74-faceted crystals. NaOH concentration is found to be the key factor in controlling Cu2O crystal morphology: as the concentration of NaOH increases, the morphology of Cu2O crystals gradually transforms from cubes that fully expose the {100} faces to regular polyhedra that expose the {110}, {111} faces, and even other high-index faces, ultimately presenting octahedra that fully expose the {111} faces. Additionally, Cu2O crystals with unique morphologies such as hollow cubes and 18-faceted with {110} face etched can be obtained by introducing surfactants or prolonging reaction durations. This work provides new insights into the morphology control of Cu2O crystals and establishes foundation in acquiring distinct Cu2O polyhedra in a facile manner for their application in catalysis, optoelectronics, sensing, and energy conversion fields.

Unified Strategy for the Concise Total Syntheses of All Six 3″-O-Acyl Quercitrins Based on Regioselective Acylation Catalyzed by Boronic Acid.

The naturally occurring 3″-O-acylquercitrin family exhibits a range of biological activities with significant potential health and medical benefits. Herein, we present a unified strategy for concise total syntheses of all six known 3″-O-acylquercitrin natural products─namely, 3″-O-galloylquercitrin, 3″-O-(E)-cinnamoylquercitrin, 3″-O-(E)-coumaroylquercitrin, 3″-O-(E)-feruloylquercitrin, 3″-O-acetylquercitrin, and 3″-O-tigloylquercitrin─based on regioselective acylation of carbohydrates catalyzed by N-methylimidazole-containing boronic acid. The core advancement in this approach is a late-stage catalytic regioselective functionalization of a common synthetic intermediate, enabling efficient access to the natural products.

Facile Synthesis of Palladium Nanorods: Self-Assembly into Thin 2D Layers for SERS Sensing

This study presents a simple, high-throughput synthesis approach for fabricating palladium (Pd) nanomaterials with anisotropic shapes, specifically Pd nanorods, via a self-assembly process. This method avoids the use of reducing agents, surface functionalization, and stabilizing agents. Palladium–poly(methyl methacrylate) (Pd-PMMA) nanocomposites were successfully synthesized using a vapor-induced phase separation (VIPS) method. The formation of Pd nanorods was controlled by tuning key parameters, such as the Pd precursor concentration, choice of solvents, and spin coating speed. Notably, the resulting nanorods exhibited high reproducibility and ultrasensitivity as a surface-enhanced Raman scattering (SERS) platform, achieving an enhancement factor of approximately 1.8 × 105, despite the relatively weak plasmonic properties of Pd. This work represents a novel, facile strategy for Pd nanorod synthesis, offering new potential for the design of Pd-based nanosensors for chemical sensing applications.

Room-Temperature Synthesis of Amorphous Fe-Doped Nickel Phosphate for High-Efficiency Alkaline Seawater Oxidation.

The construction of an efficient and durable oxygen evolution reaction (OER) electrocatalyst through a simple synthesis strategy is crucial for the hydrogen produced from seawater splitting. However, achieving this goal remains a great challenge. Herein, the synthesis of amorphous Fe-doped nickel phosphate (Fe-NixPO4) as a high-performance OER electrocatalysts for alkaline freshwater/seawater splitting is presented using a straightforward co-precipitation method at room-temperature. Experimental results reveal the structural reconstruction of Fe-NixPO4 into Fe-doped NiOOH decorated with PO4 3-. The collaborative interplay between Ni2+ and Fe3+, along with the decoration of PO4 3-, can effectively modulate the electronic environment of the electrocatalyst. Consequently, the optimized Fe-NixPO4 exhibits exceptional OER activity, requiring overpotentials of 359 and 422mV to generate 1000mA cm-2 in alkaline freshwater and alkaline seawater, respectively. Moreover, Fe-NixPO4 also displays outstanding stability for 100h at 100mA cm-2 in alkaline seawater. This research presents a viable approach for fabricating OER electrocatalysts with exceptional efficiency for seawater electrolysis.

Synthesis strategies and hydrogen storage performance of porous carbon materials derived from bio-oil

Synthesis strategies and hydrogen storage performance of porous carbon materials derived from bio-oil

Synthesis strategies and anti-parasitic evaluation of novel compounds for chagas disease: Advancing drug discovery through structure-activity relationships.

This study presents a comprehensive exploration of the synthesis of novel compounds targeting Chagas Disease (CD) caused by Trypanosoma cruzi. It is a global health threat with over 6-7 million infections worldwide. Addressing challenges in current treatments, the investigation explores diverse compound classes, including thiazoles, thiazolidinone, imidazole, pyrazole, 1,6-diphenyl-1H-pyrazolo[3,4-b] pyridine, pyrrole, naphthoquinone, neolignan, benzeneacyl hydrazones, and chalcones-based compounds. Highlighting compounds with superior trypanocidal activity compared to standard drugs. The study elucidates structure-activity relationships, emphasizing the impact of substituents, fluorine presence, and substitution patterns. Noteworthy findings include neolignan derivatives demonstrating efficacy against intracellular amastigotes and free-moving trypomastigotes, with unsaturated side chains. Benzeneacylhydrazones and chalcones, as novel classes, showed varied efficacy, with certain compounds surpassing benznidazole. A novel series of triketone compounds exhibited strong anti-parasitic activity, outperforming standard drugs. Docking study revealed that the halogen and methoxy substituted phenyl ring, thiazole, thiazolidine-4-one, quinoline, isoindoline-1,3-dione, pyrrole heterocyclic motifs can play the key role in the designing of effective inhibitors of T. cruzi. Mutually, these insights placed the foundation for the development of innovative and effective treatments for CD, addressing the urgent need for improved therapeutic options.

MIL materials: Synthesis strategies, morphology control, and biomedical application: A critical review

MIL materials: Synthesis strategies, morphology control, and biomedical application: A critical review

SDBS/SDSN-assisted alkaline dissolution-conversion of ε-Zn(OH)2 strategy for efficient synthesis of 1D ZnO with enhanced mechanical property

SDBS/SDSN-assisted alkaline dissolution-conversion of ε-Zn(OH)2 strategy for efficient synthesis of 1D ZnO with enhanced mechanical property

Structure-guided design of a Zbasic2-mediated dual-enzyme nanoreactor for chiral amine synthesis.

The synthesis of chiral amines is of critical importance but still challenging. Here, we present a self-sufficient and reusable dual-enzyme nanoreactor for chiral amine synthesis, featuring Zbasic2-mediated site-specific immobilization of amine dehydrogenase (AmDH) and glucose dehydrogenase (GDH) onto mesoporous silica nanoflowers (MSN). Molecular dynamics simulations revealed that the Zbasic2 tag was bound to MSN via electrostatic interactions, thus maintaining the fusion enzyme's active pocket accessibility and improving its catalytic performance. Using the Zbasic2 tags, AmDH and GDH were purified and immobilized on MSN in a one-pot process, thus creating the dual-enzyme nanoreactor. The dual-enzyme system exhibited remarkable activity and reusability, achieving high yields of 76-99% (ee>99%) for various chiral amines at a substrate concentration of 400mM and retaining a yield of 65% after 10cycles. This Zbasic2-based platform offers a robust and scalable strategy for sustainable chiral amine synthesis.

Synthesis and optimization strategy for enhancing SERS performance of Cu2O nanoparticles

Synthesis and optimization strategy for enhancing SERS performance of Cu2O nanoparticles

Enhancing polymethyl methacrylate (PMMA) surfaces: Taguchi optimization of PPy coating synthesis and surface modification strategies

Enhancing polymethyl methacrylate (PMMA) surfaces: Taguchi optimization of PPy coating synthesis and surface modification strategies

Advanced nanomicelles for targeted glioblastoma multiforme therapy.

Glioblastoma multiforme (GBM) is the most aggressive and malignant primary brain tumor, classified as grade IV by the WHO. Despite standard treatments like surgical resection, radiotherapy and chemotherapy (i.e. temozolomide), GBM's prognosis remains poor due to its heterogeneity, recurrence and the impermeability of the blood-brain barrier (BBB). The exact cause of GBM is unclear with potential factors including genetic predisposition and ionizing radiation. Innovative approaches such as nanomicelles-nanoscale, self-assembled structures made from lipids and amphiphilic polymers show promise for GBM therapy. These nanocarriers enhance drug solubility and stability, enabling targeted delivery of therapeutic agents across the BBB. This review explores the synthesis strategies, characterization and applications of nanomicelles in GBM treatment. Nanomicelles improve the delivery of both hydrophobic and hydrophilic drugs and provide non-invasive delivery options. By offering site-specific targeting, biocompatibility, and stability, nanomicelles can potentially overcome the limitations of current GBM therapies. This review highlights recent advancements in the use of nanomicelles for delivering therapeutic agents and nucleic acids addressing the critical need for advanced treatments to improve GBM patient outcomes.

Immunomagnetic metal-organic frameworks based coupling-free and extraction-free sensitive detection of aflatoxin B1 in peanut oils.

Conventional AFB1 detection methods are hindered by cumbersome pretreatment procedures, primarily due to the lack of new sample pretreatment materials and technologies. This work developed a novel coupling-free synthesis strategy for the immunomagnetic metal-organic frameworks (IMMOFs), focusing on its effective and promising application in the extraction-free detection of AFB1. By coupling with UPLC-FLD, a sensitive quantification detection method for AFB1 was developed, exhibiting a linear range of 0.5 to 20μg/kg and a detection limit of 0.1μg/kg. The spiked recoveries at three concentrations ranged from 90.3% to 97.9%, with RSDs of less than 6%. Moreover, the established method was successfully employed for analyzing AFB1 in naturally contaminated peanut oil samples, with results further confirmed by the traditional immunoaffinity column (IAC) method. This study provides an effective extraction-free detection technique for AFB1 that addresses the limitations of the traditional methods.

A review on molecularly imprinted magnetic solid phase extraction emphasizing the analysis of antibiotics in complex matrices:Design, preparation, and application.

Magnetic solid phase extraction (MSPE) has been widely employed in the isolation and enrichment of antibiotics in complex matrices because it presents various unique advantages over traditional SPE including simple operation, fast extraction procedure, low cost and eco-friendliness. In recently years, magnetic molecularly imprinted nanoparticles (MMINs) containing highly specific recognition performance have been widely used to specific extraction of antibiotics under the format of MSPE. In this connection, recent advances of MMINs in the analysis of antibiotic residues are reviewed. Firstly, the common structure of MMINs including core-shell, core-satellite, cavity structure and nanotube/nanosheet-supported structurewere introduced. After that, a main section covers the synthesis strategies of MMINs including one-step preparation and multi-steps preparation (precipitation polymerization, emulsion polymerization, suspension polymerization and surface imprinting technique) were illustrated. Furthermore, the applications of MMINs in the selective extraction of various antibiotic residues (sulfonamides, quinolones, tetracyclines, β-lactams, aminoglycosides and so on) in environmental and food samples were summarized. Finally, the existing problems and future prospects of MMINs were outlined in the final section of the review.

Emerging Promise of Green Synthesized Metallic Nanoparticles for the Management of Neurological Disorders.

The management of neurological disorders is very challenging due to the presence of the bloodbrain barrier (BBB) that prevents the entry of drugs into the central nervous system (CNS). The advancement of metallic nanoparticles (NPs) provides a novel direction for the treatment of neurological disorders. However, there is a significant concern regarding the toxic effects of metal NPs on biological tissues like the brain. The green synthesis strategy offers a superior alternative to the traditional methods for the development of metallic NPs. Notable metal and metal oxide NPs can be produced using various bio-reductants derived from natural sources such as plant tissues, fungi, bacteria, yeast, and alga. These biological agents play double roles as they expedite the reduction process and act as capping and stabilizing agents. In this paper, we discuss the major neurological disorders and the physical barriers limiting the transport of therapeutics to the CNS. Moreover, a special focus is given to the unique features of green synthesized metallic NPs for therapeutic purposes in various neurological disorders. The insights provided will guide future research toward better outcomes and facilitate the development of innovative treatments for neurological disorders.

Construction of enzyme-MOFs composite with carbon dots: A strategy to enhance the activity and increase the growth rate of the enzyme-ZIF-8 composite.

Encapsulating enzymes in metal-organic frameworks (MOFs) enhances enzyme protection and improves the accuracy of inhibitor recognition and screening. Zeolitic imidazolate framework-8 (ZIF-8) has been widely used as a host matrix for enzyme immobilization. However, challenges such as the microporous structure and hydrophobicity of ZIF-8, along with the protonation of 2-methylimidazole, hinder the maintenance of activity and the rapid formation of composite. Herein, a new strategy to synthesize novel enzyme-MOFs composite by encapsulating carbon dots (CDs)-modified enzyme and Fe3O4 nanoparticles within ZIF-8 is presented for the first time. The contribution of CDs in enzyme-MOFs composite was investigated. Characterizations reveal that the CDs-modified enzymes compete with imidazole for Zn ions, inducing mesoporous structures that alleviate diffusion limitations. Modification of enzyme with CDs also modulates enzyme-MOFs interfacial interactions, accelerating the formation of composite. Activity evaluation shows that enzyme-MOFs composite (THR@CDs/Fe3O4@ZIF-8) retains 81.76% enzyme activity under harsh conditions and maintains 66.0% of the initial enzyme activity after 10 reuse cycles. This synthesis strategy for the novel enzyme-MOFs composite was proven to be universal. The Km value of THR@CDs/Fe3O4@ZIF-8 (19.32μM) is lower than that of THR/Fe3O4@ZIF-8, indicating that modification with CDs significantly increases the affinity of enzyme. Furthermore, THR@CDs/Fe3O4@ZIF-8 was effectively utilized for enzyme inhibitor recognition and screening. These results demonstrate that the proposed method is a universal approach for rapidly and controllably fabricating enzyme-ZIF-8 composite with elevated activity and exceptional stability, offering promising potential for advanced drug recognition and screening platforms.