Herein, we report a both regioselective and stereoselective method for the formation of C(sp)-P bonds using alkenylsulfonium salts and >P(O)-H compounds. By employing a palladium catalyst or KCO, a variety of ()-alkenylphosphorus compounds and terminal alkenylphosphorus compounds were successfully synthesized with high selectivity. Notably, trisubstituted ()-alkenylphosphorus compounds were synthesized for the first time under metal-free conditions.
View Article and Find Full Text PDFThe centrosymmetric constraint of Friedel's law in standard x-ray diffraction limits its ability to reveal complex molecular symmetry. In contrast, twisted x-ray diffraction with vortex beams, which carry orbital angular momentum, breaks Friedel's law yielding diffraction patterns that reflect the intrinsic symmetry of molecules. Through analytical derivations and numerical simulations, we demonstrate the enhanced sensitivity of twisted x-ray diffraction to the symmetry of M-fold symmetric molecules.
View Article and Find Full Text PDFMaintaining the surface structure stability of LiCoO (LCO) during rapid charge-discharge processes (>5C) and under high-voltage conditions (>4.2 V) is challenging due to interfacial side reactions, cobalt dissolution, and oxygen redox activity at deeply delithiated states, all of which contribute to performance degradation. Herein, different from traditional surface coating methods, we report a water-mediated strategy that modifies the surface architecture of LCO, creating a passivating layer to inhibit surface degradation and enhance cycling stability under fast charging conditions.
View Article and Find Full Text PDFQuantum coherence governs the outcome and efficiency of photochemical reactions and ultrafast molecular dynamics. Recent ultrafast gas-phase X-ray scattering and electron diffraction have enabled the observation of femtosecond nuclear dynamics driven by vibrational coherence. However, probing attosecond electron dynamics and coupled electron-nuclear dynamics remains challenging.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2024
The development of cathode materials has always been one of the most crucial areas of research in the field of sodium-ion batteries. Sulfate-based polyanionic materials, known for their high working voltage characteristics, have received widespread attention. In this work, a fluoro-sulfate sodium-ion battery cathode material, NaFe(SO)F modified with carbon nanotubes, was developed using a low-temperature solid-state annealing method.
View Article and Find Full Text PDFIncreasing the levels of antiapoptotic Bcl-2 proteins is an important way that cancer cells utilize to get out of apoptosis, underscoring their significance as promising targets for anticancer therapies. Lately, a primary compound 1 bearing thiazolidine-2,4-dione was discovered to exhibit comparable Mcl-1 inhibitory activity in comparison to WL-276. Herein, thirty-nine thiazolidine-2,4-dione analogs were yielded through incorporating different biphenyl moieties (R), amino acid side chains (R) and sulfonamides (R) on 1.
View Article and Find Full Text PDFIn recent years, significant advancements have been made in the research of photoswitchable probes. These probes undergo reversible structural and electronic changes upon light exposure, thus exhibiting vast potential in molecular detection, biological imaging, material science, and information storage. Through precisely engineered molecular structures, the photoswitchable probes can toggle between "on" and "off" states at specific wavelengths, enabling highly sensitive and selective detection of targeted analytes.
View Article and Find Full Text PDFA novel strategy for the selective construction of a C(sp)-P(III) or -P(V) bond from >P(O)-H compounds and aldehydes is disclosed. By using the HPO/I system, various secondary phosphine oxides could react with both aromatic and aliphatic aldehydes to afford valuable phosphines (isolated as sulfides) and phosphine oxides in good yields. This method features a wide substrate scope and simple reaction conditions and avoids the use of toxic halides and metals.
View Article and Find Full Text PDFCiprofloxacin (CIP) is a widely used broad-spectrum antibiotic and has been associated with various side effects, making its accurate detection crucial for patient safety, drug quality compliance, and environmental and food safety. This study presents the development of a ternary nucleotide-lanthanide coordination nanoprobe, GMP-Tb-BDC (GMP: guanosine 5'-monophosphate, BDC: 2-amino-1,4-benzenedicarboxylic acid), for the sensitive and ratiometric detection of CIP. The GMP-Tb-BDC nanoprobe was constructed by incorporating the blue-emissive ligand BDC into the Tb/GMP coordination polymers.
View Article and Find Full Text PDFA Sb,N ligand () for Pd-catalyzed double N-arylation of primary amines was developed. This trivalent ligand , containing a 5,6,7,12-tetrahydrodibenzo[,][1,5]azastibocine skeleton and stable under air and moisture, could be synthesized facilely on a gram scale from chlorostibine () and cyclopentylmagnesium bromide. showed excellent catalytic performance in Pd(dba)-catalyzed double N-arylation of 2,2'-dibromo-1,1'-biphenyl () with primary amines (), affording functionalized carbazoles in good yields.
View Article and Find Full Text PDFLi insertion-induced structure transformation in crystalline electrodes vitally influence the energy density and cycle life of secondary lithium-ion battery. However, the influence mechanism of structure transformation-induced Li migration on the electrochemical performance of micro-crystal materials is still unclear and the strategy to profit from such structure transformation remains exploited. Here, an interesting self-optimization of structure evolution during electrochemical cycling in NbO micro-crystal with rich domain boundaries is demonstrated, which greatly improves the charge transfer property and mechanical strength.
View Article and Find Full Text PDFThe mechanism of Ru-catalyzed cyclization of aromatic amides with allylphosphine oxides is studied by density functional theory calculation (DFT). The results show that, first, a 5-membered Ru ring intermediate is formed by N-H and C-H diprotons via the concerted metalation-deprotonation mechanism (CMD) and then the allylphosphine oxide is inserted through the ring-extending reaction to form a 7-membered ring intermediate. Next, reduction elimination is followed via intramolecular hydrogen transfer isomerization.
View Article and Find Full Text PDFOrganic cycles play an important role in chemistry, pharmacology and material science for their unique properties. Construction of organic cycles from thioalkynes attracted increasing attention due to the facile access of thioalkynes. 2H-Azirines were synthesized successfully from thioalkynyl oxime ethers.
View Article and Find Full Text PDFCurrently, heterocycles have occupied an important position in the fields of drug design. Among them, azaindole moiety is regarded as one privileged scaffold to develop therapeutic agents. Since two nitrogen atoms of azaindole increase the possibility to form hydrogen bonds in the adenosine triphosphate (ATP)-binding site, azaindole derivatives are important sources of kinase inhibitors.
View Article and Find Full Text PDFSpectrochim Acta A Mol Biomol Spectrosc
August 2023
Hydrazine (NH) is a widely used raw material in the chemical industry, but at the same time hydrazine has extremely high toxicity. Therefore, the development of efficient detection methods is crucial for monitoring hydrazine in the environment and evaluating the biological toxicity of hydrazine. This study reports a near-infrared ratiometric fluorescent probe (DCPBCl-Hz) for the detection of hydrazine by coupling a chlorine-substituted D-π-A fluorophore (DCPBCl) to the recognition group acetyl.
View Article and Find Full Text PDF4-Sulfanyl-substituted 1,2,3-triazoles were provided regioselectively with good yields and broad scope via consecutive -BuOK-promoted dephosphinylation of 1-phosphinyl-2-sulfanylethynes and copper-catalyzed azide-alkyne cycloadditions (CuAAC) with alkyl azides. Unsymmetrically substituted ditriazoles were successfully obtained using a tandem dephosphinylative CuAAC protocol with diazides. Direct CuAAC of the 1-phosphinyl-2-sulfanylethynes with azides afforded regioisomeric mixtures of 4-phosphinyl-5-sulfanyl- and 5-phosphinyl-4-sulfanyl-1,2,3-triazoles that were easily separable from one another.
View Article and Find Full Text PDFRecent advances in perovskite ferroelectrics have fostered a host of exciting sensors and actuators. Defect engineering provides critical control of the performance of ferroelectric materials, especially lead-free ones. However, it remains a challenge to quantitatively study the concentration of defects due to the complexity of measurement techniques.
View Article and Find Full Text PDFNanomaterials (Basel)
October 2022
Nitrogen dioxide (NO) is the major reason for acid rain and respiratory illness in humans. Therefore, rapid, portable, and effective detection of NO is essential. Herein, a novel and simple method to construct a ZnO-SnO heterojunction is fabricated by pyrolysis of bimetallic metal organic frameworks.
View Article and Find Full Text PDFZirconium is a silvery-white malleable and ductile metal at room temperature with a crustal abundance of 162 ppm. Its compounds, showing Lewis acidic behavior and high catalytic performance, have been recognized as a relatively cheap, low-toxicity, stable, green, and efficient catalysts for various important organic transformations. Commercially available inorganic zirconium chloride was widely applied as a catalyst to accelerate amination, Michael addition, and oxidation reactions.
View Article and Find Full Text PDFBackground: Benzoxazine is one of the most important privileged scaffolds in medicinal chemistry. Compounds bearing benzoxazine moiety usually have a variety of biological activities, such as anti-inflammatory, anti-microbial, anti-tuberculosis, anti- oxidant and anti-cancer activities. The fascinating bioactivity profile of benzoxazine scaffold in various fields has prompted medicinal chemists to design and discover novel benzoxazine derivatives as potential therapeutic candidates with the desired biological properties.
View Article and Find Full Text PDFDeveloping new oxide solid electrolytes with fast Li-ion transport and high stability is an important step to realize high-performance solid-state Li-ion batteries. Hydrate materials containing confined water widely exist in nature or can be easily synthesized. However, they have seldom been explored as Li-ion solid electrolytes due to the stereotype that the presence of water limits the electrochemical stability window of a solid electrolyte.
View Article and Find Full Text PDFPhosphanylnaphtho[2,1-]oxazoles were synthesized successfully through one-pot phosphonation of naphthoquinone with diaryl(alkyl)phosphine oxides and Cu-catalyzed oxidative condensation with imines, followed by methylation and reduction. Upon applying 4-phosphanylnaphtho[2,1-]oxazole as a P,N-chelating ligand, Pd-catalyzed C-N formation of amines or nitrobenzene as well as Ni-catalyzed C-C formation and the synthesis of quinoline proceeded successfully. The reaction was facilely scaled up to give -benzylaniline 15a in a gram scale synthesis.
View Article and Find Full Text PDFSmall-molecule photosensitizers have great application prospects in photoelectrochemical (PEC) sensing due to their defined composition, diversified structure, and adjustable photophysical properties. Herein, we propose a new strategy for PEC analysis based on the target-induced in situ formation of the organic photosensitizer. Taking thiophenol (PhSH) as a model analyte, we designed and synthesized a 2,4-dinitrophenyl (DNP)-caged coumarin precursor (Dye-PhSH), which was then covalently coupled onto the TiO nanoarray substrate to obtain the working photoanode.
View Article and Find Full Text PDFBackground: At present, the clinical conclusion that robotic-assisted thoracic surgery (RATS) and video-assisted thoracic surgery (VATS), which is better for patients with non-small cell lung cancer (NSCLC) is not clear. Therefore, this meta-analysis aimed to compare the perioperative outcomes between RATS and VATS for NSCLC.
Methods: The Population, Interventions, Comparators, Outcomes, and Study design (PICOS) framework was employed to develop the search strategy, and the findings was reported in accordance with the Preferred Reporting Items for Systematic Reviews and Meta-Analyses (PRISMA) statement.
The selective visualization of HS in mitochondria is still a challenge, but it correlates closely with mitochondrial damage and some related diseases. In this work, a cyclometalated iridium complex Ir-DNB, [Ir(ppy)(N^N)](PF) (ppy = 2-phenylpyridine, N^N = (4'-methyl-[2,2'-bipyridin]-4-yl)methyl 2-((2,4-dinitrophenyl) thio)benzoate) has been explored for the detection of mitochondrial HS. Adding HS to a solution of complex Ir-DNB results in a clearly luminescence enhancement, and displays high selectivity and sensitivity.
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