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  • Buhl Kaae posted an update 1 year, 6 months ago

    It is highly desirable to maintain both permanent accessible pores and selective molecular recognition capability of macrocyclic cavitands in the solid state. Integration of well-defined discrete macrocyclic hosts into ordered porous polymeric frameworks (e.g., covalent organic frameworks, COFs) represents a promising strategy to transform many supramolecular chemistry concepts and principles well established in the solution phase into the solid state, which can enable a broad range of practical applications, such as high-efficiency molecular separation, heterogeneous catalysis, and pollution remediation. However, it is still a challenging task to construct macrocycle-embedded COFs. 2-deoxyglucose In this work, a novel pillar[5]arene-derived (P5) hetero-porous COF, denoted as P5-COF, was rationally designed and synthesized. Featuring the unique backbone structure, P5-COF exhibited selective adsorption of C2H2 over C2H4 and C2H6, as well as significantly enhanced host-guest binding interaction with paraquat, in comparison with the pillar[5]arene-free COF analog, Model-COF. The present work established a new strategy for developing COFs with customizable molecular recognition/separation properties through the bottom-up “pre-porous macrocycle to porous framework” design.Although porous organic cages (POCs), particularly imine-linked (C[double bond, length as m-dash]N) ones, have advanced significantly over the last few decades, the reversible nature of imine linkages makes them prone to hydrolysis and structural collapse, severely limiting their applications under moist or water conditions. Herein, seven water-stable hydrazone-linked (C[double bond, length as m-dash]N-N) POCs are prepared through a simple coupling of the same supramolecular tetraformylresorcin[4]arene cavitand with different dihydrazide linkers. Their structures are all determined by single-crystal X-ray crystallography, demonstrating rich structural diversity from the [2 + 4] lantern, [3 + 6] triangular prism, and unprecedented [4 + 8] square prism to the extra-large [6 + 12] octahedron. In addition, they respectively exhibit tunable window diameters and cavity volumes ranging from about 5.4 to 11.1 nm and 580 to 6800 Å3. Moreover, their application in the water environment for pollutant removal was explored, indicating that they can effectively eliminate various types of contaminants from water, including radionuclide waste, toxic heavy metal ions, and organic micropollutants. This work demonstrates a convenient method for rationally constructing versatile robust POCs and presents their great application potentialities in water medium.Helicene is a functional material with chirality caused by its characteristic helical geometry. The inversion of its helicity by external stimuli is a challenging task in the advanced control of the molecular chirality. This study fabricated a novel helical molecule, specifically a pentahelicene-analogue twisted aromatic hydrocarbon fused with a graphene nanoribbon, via on-surface synthesis using multiple precursors. Noncontact atomic force microscopy imaging with high spatial resolution confirmed the helicity of the reaction products. The helicity was geometrically converted by pushing a CO-terminated tip into the twisted framework, which is the first demonstration of helicity switching at the single-molecule scale.The development of inhibitors of intracellular protein-protein interactions (PPIs) is of great significance for drug discovery, but the generation of a cell-permeable molecule with high affinity to protein is challenging. Oligo(N-substituted glycines) (oligo-NSGs), referred to as peptoids, are attractive as potential intracellular PPI inhibitors owing to their high membrane permeability. However, their intrinsically flexible backbones make the rational design of inhibitors difficult. Here, we propose a peptoid-based rational approach to develop cell-permeable PPI inhibitors using oligo(N-substituted alanines) (oligo-NSAs). The rigid structures of oligo-NSAs enable independent optimization of each N-substituent to improve binding affinity and membrane permeability, while preserving the backbone shape. A molecule with optimized N-substituents inhibited a target PPI in cells, which demonstrated the utility of oligo-NSA as a reprogrammable template to develop intracellular PPI inhibitors.Due to overcoming the limitation of aggregation caused quenching (ACQ) of solid-state emitters, aggregation-induced emission (AIE) organic luminogens have become a promising candidate in aqueous electrochemiluminescence (ECL). However, restricted by the physical nature of fluorescence, current organic AIE luminogen-based ECL (AIECL) faces the bottleneck of low ECL efficiency. Here, we propose to construct de novo aqueous ECL based on aggregation-induced delayed fluorescence (AIDF) luminogens, called AIDF-ECL. Compared with the previous organic AIE luminogens, purely organic AIDF luminogens integrate the superiorities of both AIE and the utilization of dark triplets via thermal-activated spin up-conversion properties, thereby possessing the capability of close-to-unity exciton utilization for ECL. The results show that the ECL characteristics using AIDF luminogens are directly related to their AIDF properties. Compared with an AIECL control sample based on a tetraphenylethylene AIE moiety, the ECL efficiency of our AIDF-ECL model system is improved by 5.4 times, confirming the excellent effectiveness of this innovative strategy.While cancer now impacts the health and well-being of more of the human population than ever before, the exponential rise in antimicrobial resistant (AMR) bacterial infections means AMR is predicted to become one of the greatest future threats to human health. It is therefore vital that novel therapeutic strategies are developed that can be used in the treatment of both cancer and AMR infections. Whether the target of a therapeutic agent be inside the cell or in the cell membrane, it must either interact with or cross this phospholipid barrier to elicit the desired cellular effect. Here we summarise findings from published research into the phospholipid membrane composition of bacterial and cancer cell lines and biological samples from cancer patients. These data not only highlight key differences in the membrane composition of these biological samples, but also the methods used to elucidate and report the results of this analogous research between the microbial and cancer fields.As lithium-ion batteries have been the state-of-the-art electrochemical energy storage technology, the overwhelming demand for energy storage on a larger scale has triggered the development of next-generation battery technologies possessing high energy density, longer cycle lives, and enhanced safety. However, commercial liquid electrolytes have been plagued by safety issues due to their flammability and instability in contact with electrodes. Efforts have focused on developing such electrolytes by covalently immobilizing anionic groups onto a polymer backbone, which only allows Li+ cations to be mobile through the polymer matrix. Such ion-selective polymers provide many advantages over binary ionic conductors in battery operation, such as minimization of cell polarization and dendrite growth. In this review, the design, synthesis, fabrication, and class are reviewed to give insight into the physicochemical properties of single-ion conducting polymer electrolytes. The standard characterization method and remarkable electrochemical properties are further highlighted, and perspectives on current challenges and future directions are also discussed.

    The objective of this study was to compare the predictive accuracy of the acid exposure time (AET) with the DeMeester score (DMS) for gastroesophageal reflux-induced cough (GERC).

    A total of 277 patients who underwent multichannel intraluminal impedance pH monitoring (MII-pH) were enrolled, and their clinical information and laboratory results were retrospectively analyzed. The diagnostic value of AET for GERC was compared with that of the DMS, symptom association probability (SAP), and symptom index (SI).

    A total of 236 patients met the inclusion criteria, 150 patients (63.65%) were definitely diagnosed with GERC, including 111(74%) acid GERC and 39 (26%) nonacid GERC. The optimal cutoff value of AET for diagnosing GERC was AET > 4.8%, and its diagnostic value was equal to that of DMS > 14.7 (AUC = 0.827

    0.818,

     = 0.519) and was superior to that of SAP (AUC = 0.827

    0.689,

     = 0.000) and SI (AUC = 0.827

    0.688,

     = 0.000). When using both DMS > 14.7 and AET > 4.8% or either of the two for the diagnosis of GERC, the diagnosis rate was not improved over using DMS > 14.7 alone. The diagnostic value of AET and DMS for acid GERC were both high and equivalent (AUC = 0.925

    0.922,

     = 0.95). The optimal cutoff value of AET for diagnosing acid GERC was AET > 6.2%.

    AET and DMS are both equal in discriminating GERC. A GERC diagnosis should be considered when AET > 4.8%, whereas an acid GERC diagnosis should be considered when AET > 6.2%.

     6.2%.

    The aim of this study was to evaluate the association between nonalcoholic fatty liver disease (NAFLD) and NAFLD with different comorbidities and risk of chronic kidney disease (CKD) and abnormal albuminuria.

    A total of 3872 Chinese individuals excluding those with hepatitis B or C infection and absence of alcohol abuse were included in the study. NAFLD was diagnosed by abdominal ultrasonography. The liver fibrosis was assessed by NAFLD fibrosis score (NFS) and fibrosis-4 index (FIB-4). CKD was defined as an estimated glomerular filtration rate (eGFR) < 60 ml/min/1.73 m

    and/or abnormal albuminuria (urinary albumin-to-creatinine ratio ⩾ 3 mg/mmol). The logistic regression analysis was performed to examine the association between NAFLD and NAFLD with different comorbidities and risk of CKD.

    The prevalence of CKD and abnormal albuminuria was higher in individuals with NAFLD than in those without NAFLD (15.8% vs 11.9%,

     < 0.001; 14.8% vs 11.0%,

     < 0.001). Logistic regression analysis demonstrated that NAFLD was risk factor of CKD. Notably, after adjustment for sex, age, and DM, NAFLD was associated with 1.31-fold higher risk of prevalent CKD ⩾ 1 (

     < 0.05). NAFLD individuals with elder age, DM, obesity, hypertension, MetS, and advanced liver fibrosis had higher risks of both prevalent CKD and abnormal albuminuria than those without comorbidities.

    NAFLD and NAFLD with traditional comorbidities are strongly associated with risk of prevalence of CKD and abnormal albuminuria. Patients with NAFLD especially those with coexisting comorbidities were recommended to carefully access the development of CKD.

    NAFLD and NAFLD with traditional comorbidities are strongly associated with risk of prevalence of CKD and abnormal albuminuria. Patients with NAFLD especially those with coexisting comorbidities were recommended to carefully access the development of CKD.COVID-19 is an infectious disease-causing flu-like respiratory problem with various symptoms such as cough or fever, which in severe cases can cause pneumonia. The aim of this paper is to develop a rapid and accurate medical diagnosis support system to detect COVID-19 in chest X-ray images using a stacking approach combining transfer learning techniques and KNN algorithm for selection of the best model. In deep learning, we have multiple approaches for building a classification system for analyzing radiographic images. In this work, we used the transfer learning technique. This approach makes it possible to store and use the knowledge acquired from a pretrained convolutional neural network to solve a new problem. To ensure the robustness of the proposed system for diagnosing patients with COVID-19 using X-ray images, we used a machine learning method called the stacking approach to combine the performances of the many transfer learning-based models. The generated model was trained on a dataset containing four classes, namely, COVID-19, tuberculosis, viral pneumonia, and normal cases.