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1.
Anal Chem ; 96(16): 6329-6336, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38597405

RESUMO

The simultaneous discrimination of multiple homologous sequences faces challenges due to the high similarity of sequences and the complexity of the discrimination system in most reported works. Herein, a simple and ingenious analysis method was developed to identify eight miRNAs of the let-7 family by combining logic gates and entropy-driven catalytic (EDC)-based lanthanide labeling inductively coupled plasma mass spectrometry (ICP-MS) technology. Specifically, eight miRNAs were first divided into four types according to the difference of bases in the domains 2 and 3 on sequences. To identify the type of targets, a DNA logic gate was constructed with two strand displacement reactions on magnetic beads that could be initiated by different types of targets. Based on the difference of the output signals after two strand displacement reactions, the type of targets was distinguished preliminarily. Then, the discrimination of a specific target was achieved with EDC-based lanthanide labeling ICP-MS detection. By labeling the different magnetic probes with different elemental tags, a specific element signal released from magnetic beads after EDC could be detected by ICP-MS, and therefore, simultaneous detection of homologous sequences was completed. This work provided a novel and simple method for highly specific identification of homologous sequences with the assistance of a logic gate and can promote further development of elemental labeling ICP-MS in the field of multiple analysis.

2.
Front Psychiatry ; 15: 1309501, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38469031

RESUMO

Introduction: Emotional words are often used as stimulus material to explore the cognitive and emotional characteristics of individuals with depressive disorder, while normal individuals mostly rate the scores of affective words. Given that individuals with depressive disorder exhibit a negative cognitive bias, it is possible that their depressive state could influence the ratings of affective words. To enhance the validity of the stimulus material, we specifically recruited patients with depression to provide these ratings. Methods: This study provided subjective ratings for 501 Chinese affective norms, incorporating 167 negative words selected from depressive disorder patients' Sino Weibo blogs, and 167 neutral words and 167 positive words selected from the Chinese Affective Word System. The norms are based on the assessments made by 91 patients with depressive disorder and 92 normal individuals, by using the paper-and-pencil quiz on a 9-point scale. Results: Regardless of the group, the results show high reliability and validity. We identified group differences in three dimensions: valence, arousal, and self-relevance: the depression group rated negative words higher, but positive and neutral words lower than the normal control group. Conclusion: The emotional perception affected the individual's perception of words, to some extent, this database expanded the ratings and provided a reference for exploring norms for individuals with different emotional states.

3.
Nanoscale ; 16(8): 4047-4055, 2024 Feb 22.
Artigo em Inglês | MEDLINE | ID: mdl-38354061

RESUMO

The rising top-down synthetic methodologies for transition metal single-atom catalysts (SACs) require controlled movement of metal atoms through the substrates; however, their direct transportation towards the ideal carrier remains a huge challenge. Herein, we showed a "top down" strategy for Co nanoparticles (NPs) to Co SA transformation by employing electrospun carbon nanofibers (CNFs) as atom carriers. Under high-temperature conditions, the Co atoms migrate from the surfaces of Co NPs and are then anchored by the surrounding carbon to form a Co-C3O1 coordination structure. The synthesized Co SAs/CNF electrocatalyst exhibits excellent electrocatalytic nitrate reduction reaction (NO3RR) activity with an NH3 yield of 0.79 mmol h-1 cm-2 and Faraday efficiency (FE) of 91.3% at -0.7 V vs. RHE in 0.1 M KNO3 and 0.1 M K2SO4 electrolytes. The in situ electrochemical characterization suggests that the NOH pathway is preferred by Co SAs/CNFs, and *NO hydrogenation and deoxygenation easily occur on Co SAs due to the small adsorption energy between Co SAs and *NO, as calculated by theoretical calculations. It is revealed that a small energy barrier (0.45 eV) for the rate determining step (RDS) ranges from *NO to *NOH and a strong capability for inhibiting hydrogen evolution (HER) significantly promotes the NH3 selectivity and activity of Co SAs/CNFs.

4.
IEEE Trans Image Process ; 33: 1670-1682, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38306266

RESUMO

When we recognize images with the help of Artificial Neural Networks (ANNs), we often wonder how they make decisions. A widely accepted solution is to point out local features as decisive evidence. A question then arises: Can local features in the latent space of an ANN explain the model output to some extent? In this work, we propose a modularized framework named MemeNet that can construct a reliable surrogate from a Convolutional Neural Network (CNN) without changing its perception. Inspired by the idea of time series classification, this framework recognizes images in two steps. First, local representations named memes are extracted from the activation map of a CNN model. Then an image is transformed into a series of understandable features. Experimental results show that MemeNet can achieve accuracy comparable to most models' through a set of reliable features and a simple classifier. Thus, it is a promising interface to use the internal dynamics of CNN, which represents a novel approach to constructing reliable models.

5.
Appl Opt ; 63(1): 77-84, 2024 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-38175011

RESUMO

In this paper, an ANLVENet speckle suppression method in holographic phase fringe patterns with different level noises is proposed based on FFDNet, combined with asymmetric pyramid non-local block with a verge extraction module. The experimental results are compared to three network models and several representative algorithms. It is shown that the ANLVENet method not only has better superiority in the speckle suppression with different noise levels, but also preserves more details of the image edge. In addition, another speckle noise model is applied in the phase fringe patterns to prove the stronger generalization of the ANLVENet algorithm. The proposed method is suitable for suppressing the speckle with different levels in a large noise range under complex environmental conditions.

6.
Nat Commun ; 15(1): 351, 2024 Jan 08.
Artigo em Inglês | MEDLINE | ID: mdl-38191779

RESUMO

Coupling high-capacity cathode and Li-anode with solid-state electrolyte has been demonstrated as an effective strategy for increasing the energy densities and safety of rechargeable batteries. However, the limited ion conductivity, the large interfacial resistance, and unconstrained Li-dendrite growth hinder the application of solid-state Li-metal batteries. Here, a poly(ether-urethane)-based solid-state polymer electrolyte with self-healing capability is designed to reduce the interfacial resistance and provides a high-performance solid-state Li-metal battery. With its dynamic covalent disulfide bonds and hydrogen bonds, the proposed solid-state polymer electrolyte exhibits excellent interfacial self-healing ability and maintains good interfacial contact. Full cells are assembled with the two integrated electrodes/electrolytes. As a result, the Li||Li symmetric cells exhibit stable long-term cycling for more than 6000 h, and the solid-state Li-S battery shows a prolonged cycling life of 700 cycles at 0.3 C. The use of ultrasound imaging technology shows that the interfacial contact of the integrated structure is much better than those of traditional laminated structure. This work provides an interesting interfacial dual-integrated strategy for designing high-performance solid-state Li-metal batteries.

7.
Adv Mater ; 36(18): e2308799, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38270498

RESUMO

The heterogeneity, species diversity, and poor mechanical stability of solid electrolyte interphases (SEIs) in conventional carbonate electrolytes result in the irreversible exhaustion of lithium (Li) and electrolytes during cycling, hindering the practical applications of Li metal batteries (LMBs). Herein, this work proposes a solvent-phobic dynamic liquid electrolyte interphase (DLEI) on a Li metal (Li-PFbTHF (perfluoro-butyltetrahydrofuran)) surface that selectively transports salt and induces salt-derived SEI formation. The solvent-phobic DLEI with C-F-rich groups dramatically reduces the side reactions between Li, carbonate solvents, and humid air, forming a LiF/Li3PO4-rich SEI. In situ electrochemical impedance spectroscopy and Ab-initio molecular dynamics demonstrate that DLEI effectively stabilizes the interface between Li metal and the carbonate electrolyte. Specifically, the LiFePO4||Li-PFbTHF cells deliver 80.4% capacity retention after 1000 cycles at 1.0 C, excellent rate capacity (108.2 mAh g-1 at 5.0 C), and 90.2% capacity retention after 550 cycles at 1.0 C in full-cells (negative/positive (N/P) ratio of 8) with high LiFePO4 loadings (15.6 mg cm-2) in carbonate electrolyte. In addition, the 0.55 Ah pouch cell of 252.0 Wh kg-1 delivers stable cycling. Hence, this study provides an effective strategy for controlling salt-derived SEI to improve the cycling performances of carbonate-based LMBs.

8.
Risk Anal ; 44(2): 459-476, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37330273

RESUMO

The Northern Sea Route (NSR) makes travel between Europe and Asia shorter and quicker than a southern transit via the Strait of Malacca and Suez Canal. It provides greater access to Arctic resources such as oil and gas. As global warming accelerates, melting Arctic ice caps are likely to increase traffic in the NSR and enhance its commercial viability. Due to the harsh Arctic environment imposing threats to the safety of ship navigation, it is necessary to assess Arctic navigation risk to maintain shipping safety. Currently, most studies are focused on the conventional assessment of the risk, which lacks the validation based on actual data. In this study, actual data about Arctic navigation environment and related expert judgments were used to generate a structured data set. Based on the structured data set, extreme gradient boosting (XGBoost) and alternative methods were used to establish models for the assessment of Arctic navigation risk, which were validated using cross-validation. The results show that compared with alternative models, XGBoost models have the best performance in terms of mean absolute errors and root mean squared errors. The XGBoost models can learn and reproduce expert judgments and knowledge for the assessment of Arctic navigation risk. Feature importance (FI) and shapley additive explanations (SHAP) are used to further interpret the relationship between input data and predictions. The application of XGBoost, FI, and SHAP is aimed to improve the safety of Arctic shipping using advanced artificial intelligence techniques. The validated assessment enhances the quality and robustness of assessment.

9.
Small ; 20(7): e2305494, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37797191

RESUMO

Lithium-sulfur (Li-S) batteries hold the superiority of eminent theoretical energy density (2600 Wh kg-1 ). However, the ponderous sulfur reduction reaction and the issue of polysulfide shuttling pose significant obstacles to achieving the practical wide-temperature operation of Li-S batteries. Herein, a covalent organic nanosheet-wrapped carbon nanotubes (denoted CON/CNT) composite is synthesized as an electrocatalyst for wide-temperature Li-S batteries. The design incorporates the CON skeleton, which contains imide and triazine functional units capable of chemically adsorbing polysulfides, and the underlaid CNTs facilitate the conversion of captured polysulfides enabled by enhanced conductivity. The electrocatalytic behavior and chemical interplay between polysulfides and the CON/CNT interlayer are elucidated by in situ X-ray diffraction detections and theoretical calculations. Resultantly, the CON/CNT-modified cells demonstrate upgraded performances, including wide-temperature operation ranging from 0 to 65 °C, high-rate performance (625 mAh g-1 at 5.0 C), exceptional high-rate cyclability (1000 cycles at 5.0 C), and stable operation under high sulfur loading (4.0 mg cm-2 ) and limited electrolyte (5 µL mgs -1 ). These findings might guide the development of advanced Li-S batteries.

10.
Artigo em Inglês | MEDLINE | ID: mdl-38038267

RESUMO

In this study, we demonstrate the fabrication of a novel 2D transition metal dichalcogenide, VTe2, into a saturable absorber (SA) by using the liquid phase exfoliation method. Furthermore, the first-principles calculations were conducted to elucidate the electronic band structures and absorption spectrum. The nonlinear optical absorption properties of VTe2 at 1.0, 2.0, and 3.0 µm were measured using open-aperture Z-scan and P-scan methods, which showed saturation intensities and modulation depths of 95.57 GW/cm2 and 9.24%, 3.11 GW/cm2 and 7.26%, and 15.8 MW/cm2 and 17.1%, respectively. Furthermore, in the realm of practical implementation, the achievement of stable passively Q-switched (PQS) lasers employing SA composed of few-layered VTe2 nanosheets has manifested itself with broadband operating wavelengths from 1.0 to ∼3.0 µm. Specifically, PQS laser operations from near-infrared to mid-infrared with pulse durations of 195 and 563 ns for 1.0 and 2.0 µm solid-state lasers, respectively, and 749 ns for an Er3+-doped fluoride fiber laser at 3.0 µm were obtained. Our experimental results demonstrate that VTe2 is a potential broadband SA device for achieving PQS lasers. To the best of our knowledge, this is the first demonstration of using VTe2 as an SA in PQS lasers in the near- and mid-infrared regions, which highlights the potential of VTe2 for future research and applications in optoelectronic devices.

11.
Intractable Rare Dis Res ; 12(4): 251-256, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-38024584

RESUMO

On September 18, 2023, the National Health Commission of China officially announced the "Second List of Rare Diseases". This list of 86 rare diseases, drafted in accordance with the "Working Procedures for Drafting the List of Rare Diseases", marks the second release of a rare disease list since the initial list was issued in May 2018. Following the release of the first batch, the Chinese Government introduced various policies to enhance the diagnosis and treatment of rare diseases, to promote the research on, development of, production of, and availability of rare disease medications in China, and to improve medication access for patients with rare diseases. Consequently, this has elevated the level of rare disease diagnosis and treatment, ensuring greater accessibility to treatment for affected individuals. The expansion of the rare disease list through the release of the "Second List of Rare Diseases" will further enhance rare disease management, increase awareness, improve diagnosis and treatment, facilitate the development and availability of more rare disease medications, establish a comprehensive support system for patients with rare diseases, and ultimately benefit a larger number of individuals affected by rare diseases. The definition of rare diseases in China should be refined by explicitly establishing corresponding criteria based on incidence, prevalence, or the number of affected individuals. Additionally, the mechanism for removal of diseases from rare disease lists should be enhanced, and prompt adjustments should be made regarding diseases that do not align with the selection principles of the list, taking into consideration environmental changes.

12.
Front Neurosci ; 17: 1282322, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-38027520

RESUMO

Transcranial alternating current stimulation (tACS) is a non-invasive neuromodulation technique that is being tested clinically for treatment of a variety of neural disorders. Animal studies investigating the underlying mechanisms of tACS are scarce, and nearly absent in the cerebellum. In the present study, we applied 10-400 Hz alternating currents (AC) to the cerebellar cortex in ketamine/xylazine anesthetized rats. The spiking activity of cerebellar nuclear (CN) cells was transsynaptically entrained to the frequency of AC stimulation in an intensity and frequency-dependent manner. Interestingly, there was a tuning curve for modulation where the frequencies in the midrange (100 and 150 Hz) were more effective, although the stimulation frequency for maximum modulation differed for each CN cell with slight dependence on the stimulation amplitude. CN spikes were entrained with latencies of a few milliseconds with respect to the AC stimulation cycle. These short latencies and that the transsynaptic modulation of the CN cells can occur at such high frequencies strongly suggests that PC simple spike synchrony at millisecond time scales is the underlying mechanism for CN cell entrainment. These results show that subthreshold AC stimulation can induce such PC spike synchrony without resorting to supra-threshold pulse stimulation for precise timing. Transsynaptic entrainment of deep CN cells via cortical stimulation could help keep stimulation currents within safety limits in tACS applications, allowing development of tACS as an alternative treatment to deep cerebellar stimulation. Our results also provide a possible explanation for human trials of cerebellar stimulation where the functional impacts of tACS were frequency dependent.

13.
Anal Chim Acta ; 1280: 341875, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37858560

RESUMO

The non-specific adsorption behaviors of various interferents on the surface of a molecularly imprinted polymer (MIP) are adverse for the selectivity of an MIP-based sensor, which can be overcome via a differential strategy by using the differential signal between MIP- and non-imprinted polymer (NIP)-based sensors. However, the normal differential mode is not suitable for the MIP-based sensors with non-linear calibration curves. Herein, an improved differential strategy is reported for an MIP-based sensor with a semi-logarithmic calibration curve, demonstrated by an electrochemiluminescence (ECL) sensor for dopamine (DA). Glassy carbon electrode (GCE) was modified by the mixture of g-C3N4, TiO2 nanoparticles (NPs) and carbon nanotubes (CNTs). MIP membrane for DA was fabricated on the surface of g-C3N4/TiO2NPs/CNTs/GCE using chitosan for film-forming, obtained MIP@GCE. To enhance the anti-interference ability of the MIP-based DA sensor, the difference between exponential functions ECL intensities of MIP@GCE and NIP@GCE is used as the analytical signal in the improved differential strategy. The differential signal was increased linearly with increasing DA concentration ranging from 10 pM to 0.10 µM, with the detection limit of 5.6 pM. The interference level of Cu2+ on DA determination in the improved differential mode is only 9.7% of that in the normal MIP mode. The improved differential strategy can be used in other MIP-based sensors with semi-logarithmic calibration curves.

14.
Anal Chim Acta ; 1279: 341780, 2023 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-37827678

RESUMO

MicroRNAs (miRNAs) are closely associated with human disease occurrence, including cancers, diabetes, inflammation, heart diseases, and viral infections, and their rapid and accurate detection is vital for the diagnosis and treatment of these diseases. Based on one-step reaction of strand displacement amplification (SDA) and primer exchange reaction (PER), a label-free and highly sensitive miRNA-21 detection strategy was developed. In this strategy, the target miRNA-21 binds directly to the hairpin template, triggering the SDA reaction and generating a large number of single strand DNAs as primers for PER amplification. With the help of polymerase, plenty of G-quadruplex fragments of different lengths were accumulated, and the organic dye thioflavin T selectively binds to these G-quadruplex fragments to produce a strong fluorescent signal. There is a wide detection range in this method, miRNA-21 can be detected in the range of 10 fM - 1 nM, the detection limit is low (1.25 fM). This method has good specificity and can effectively distinguish single-base mismatches of miRNA. In addition, the versatility of the method was validated by changing the target recognition site of SDA template.


Assuntos
Técnicas Biossensoriais , Quadruplex G , MicroRNAs , Neoplasias , Humanos , MicroRNAs/genética , Técnicas de Amplificação de Ácido Nucleico/métodos , Corantes , Limite de Detecção
15.
Artigo em Chinês | MEDLINE | ID: mdl-37549950

RESUMO

Objective:To investigate surgical treatment of carotid artery diseases in neck tumor surgery. Methods:A retrospective analysis of the clinical data on carotid artery treatment was conducted in the five cases of neck tumor surgeries treated at Department of Surgical Oncology, the First Peoples Hospital of Lanzhou from March 2010 to May 2020. Surgical methods, including carotid artery resection and ligation, tumor-involved artery resection and vascular reconstruction, and tumor peeling and carotid rupture repairing were used, respectively. Results:Five cases were successfully operated on. One case of carotid artery ligation was followed by intermittent dizziness and decreased contra-lateral limb strength after the surgery. The remaining patients exhibited no neurological complications. A patient with cervical low-grade myofibroblastoma developed into lung metastases 8 months after the surgery. Another patient with cervical lymph node metastases in papillary thyroid cancer developed into lung metastases 24 months after the surgery. Conclusion:Currently, surgical methods for clinical treatment of diseased carotid arteries include carotid artery resection and ligation, simple tumor peeling, tumor invasion artery resection and vascular reconstruction, and interventional therapy. Each surgical method has its own advantages and disadvantages. Therefore, the choice of treatment depends on the patient's specific conditions, physician's clinical experience, and the equipment available.


Assuntos
Neoplasias de Cabeça e Pescoço , Neoplasias Pulmonares , Neoplasias da Glândula Tireoide , Humanos , Estudos Retrospectivos , Artérias Carótidas/cirurgia , Artérias Carótidas/patologia , Neoplasias de Cabeça e Pescoço/cirurgia , Neoplasias de Cabeça e Pescoço/patologia , Neoplasias da Glândula Tireoide/cirurgia , Neoplasias Pulmonares/patologia
16.
Chem Rec ; 23(11): e202300146, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37283443

RESUMO

Preparing valuable olefins from cheap and abundant alkane resources has long been a challenging task in organic synthesis, which mainly suffers from harsh reaction conditions and narrow scopes. Homogeneous transition metals catalyzed dehydrogenation of alkanes has attracted much attention for its excellent catalytic activities under relatively milder conditions. Among them, base metal catalyzed oxidative alkane dehydrogenation has emerged as a viable strategy for olefin synthesis for its usage of cheap catalysts, compatibility with various functional groups, and low reaction temperature. In this review, we discuss recent development of base metal catalyzed alkane dehydrogenation under oxidative conditions and their application in constructing complex molecules.

17.
Adv Mater ; 35(38): e2303460, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37269455

RESUMO

Ultrathin and super-toughness gel polymer electrolytes (GPEs) are the key enabling technology for durable, safe, and high-energy density solid-state lithium metal batteries (SSLMBs) but extremely challenging. However, GPEs with limited uniformity and continuity exhibit an uneven Li+ flux distribution, leading to nonuniform deposition. Herein, a fiber patterning strategy for developing and engineering ultrathin (16 µm) fibrous GPEs with high ionic conductivity (≈0.4 mS cm-1 ) and superior mechanical toughness (≈613%) for durable and safe SSLMBs is proposed. The special patterned structure provides fast Li+ transport channels and tailoring solvation structure of traditional LiPF6 -based carbonate electrolyte, enabling rapid ionic transfer kinetics and uniform Li+ flux, and boosting stability against Li anodes, thus realizing ultralong Li plating/stripping in the symmetrical cell over 3000 h at 1.0 mA cm-2 , 1.0 mAh cm-2 . Moreover, the SSLMBs with high LiFePO4 loading of 10.58 mg cm-2 deliver ultralong stable cycling life over 1570 cycles at 1.0 C with 92.5% capacity retention and excellent rate capacity of 129.8 mAh g-1 at 5.0 C with a cut-off voltage of 4.2 V (100% depth-of-discharge). Patterned GPEs systems are powerful strategies for producing durable and safe SSLMBs.

18.
Behav Sci (Basel) ; 13(6)2023 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-37366752

RESUMO

(1) Background: To examine the relationship among just-world beliefs, self-control, and cyberaggression among college students. (2) Methods: A total of 1133 college students were surveyed using the just-world belief scale, self-control scale, and cyberaggression scale. (3) Results: The results showed that college students with low levels of belief in justice frequently showed cyberaggression; belief in a just world directly and negatively predicted cyberaggression, and indirectly predicted student cyberaggression through self-control; gender moderated the indirect effect of self-control on cyberaggression and the direct effect of belief in a just world on cyberaggression. (4) Conclusions: Belief in a just world significantly and negatively predicts cyberaggression; self-control has an indirect significant effect on cyberaggression; the direct effect of belief in a just world on cyberaggression and the mediating effect of self-control on this association are moderated by gender.

19.
Anal Chem ; 95(26): 10096-10104, 2023 07 04.
Artigo em Inglês | MEDLINE | ID: mdl-37351925

RESUMO

In this work, a potential-resolved electrochemiluminescence (ECL) multiplex immunoassay (MIA) was developed using zirconium-based metal-organic framework (MOF) nanoparticles with intense self-ECL as an anodic ECL tag and CdTe nanocrystals (NCs) as a cathodic ECL tag. ECL luminophore 5,5'-(anthracene-9,10-diyl)diisophthalic acid (H4ADIP) and coreactant hexamethylenetetramine (HMT) bound to zirconium nodes in the MOF, giving Zr-ADIP-HMT nanoparticles. Benefiting from the intrareticular charge transfer (ICT) between the oxidized ligands of H4ADIP and HMT via hydrogen bonds, the intense self-ECL from Zr-ADIP-HMT was applied to the potential-resolved ECL MIA without an exogenous anodic coreactant, which can eliminate detrimental effects of multiplex coreactants and anodic ECL emission from CdTe NCs. The ICT within Zr-ADIP-HMT nanoparticles could shorten the electron transport path and reduce the complexity of radical intermediate transport. The ECL intensity from Zr-ADIP-HMT was 18.6-fold that from the mixture of H4ADIP and HMT. In potential-resolved ECL MIA, two lung cancer biomarkers, carcinoembryonic antigen and neuron-specific enolase, were adopted as model analytes, with detection limits of 18 and 5.3 fg·mL-1, respectively. The dual-ligand Zr-ADIP-HMT nanoparticles provide a proof of concept using ICT-based self-ECL luminophores for potential-resolved ECL MIAs with isolated coreactants.


Assuntos
Técnicas Biossensoriais , Compostos de Cádmio , Nanopartículas Metálicas , Estruturas Metalorgânicas , Nanopartículas , Pontos Quânticos , Estruturas Metalorgânicas/química , Zircônio , Compostos de Cádmio/química , Técnicas Eletroquímicas , Medições Luminescentes , Telúrio/química , Nanopartículas/química , Imunoensaio , Nanopartículas Metálicas/química , Limite de Detecção
20.
Angew Chem Int Ed Engl ; 62(24): e202302908, 2023 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-37062703

RESUMO

Fluoroalkyl aryl ethers are valuable structural motifs in pharmaceuticals because compounds with these motifs are more metabolically stable and more lipophilic than their nonfluorinated analogues. However, hexafluoroisopropyl aryl ethers have not been extensively studied, presumably because of the lack of efficient synthetic methods. Herein, we describe a rhodium-catalyzed nucleophilic aromatic substitution of aryl chlorides or bromides, which act as the limiting reagents, with weakly nucleophilic hexafluoro-2-propanol under mild reaction conditions. This method provides diverse hexafluoroisopropyl aryl ethers. We demonstrated the generality of this method by carrying out reactions of a large array of unactivated aryl halides, and we found that the success of the reactions relied on arene activation by means of η6 -coordination.

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