Latest ArticlesGlioblastoma multiforme (GBM) is the most common malignant primary brain tumor in adults. The precise identification and distinction of GBM heterogeneity from surrounding brain parenchyma at the cellular level and even at the tissue level are important for GBM therapy. In this study, GBM cells are distinguished from normal astrocytes and non-central nervous system (CNS) tumor cells by surface-enhanced Raman scattering (SERS) based on gold nanoshell (SiO2@Au) particles and support vector machine (SVM) algorithm. In addition, the gold nanoisland (AuNI) SERS substrates are further developed and explored for accurate detection of GBM at the tissue level. The distinction between glioma and trauma tissues, identification of different tumor grades, and IDH mutation are realized with the assistance of orthogonal partial least squares discriminant analysis (OPLS-DA) in a rapid, non-invasive, and convenient method. The results show that the developed SERS-based analytical method has the potential for practical application for the detection of GBM at the single-cell and tissue levels and even for real-time intraoperative diagnosis.
Protein recognition using host-guest recognition approach is of great interest but has been limited mainly to the protein N-terminal residues. Here, we site-specific incorporated two novel non-canonical amino acids containing supramolecular guest motifs into protein via an expanded genetic code. Through Staudinger reduction reactions, the encoded unnatural residues on protein becoming activated and can be specifically recognized by cucurbit[7]uril (CB[7]) and cucurbit[8]uril (CB[8]). We demonstrated that enzyme containing guest amino acid incorporated near the active site can be reversibly regulated by CB[7] recognition, and CB[8] recognition induces protein dimerization. These amino acids will make useful addition to the supramolecular toolbox for protein targeting using molecular recognition approaches.
A water-soluble macrocycle that bears four carboxylate anions has been designed and prepared, which forms a rectangular cavity that can efficiently encapsulate discrete electron-deficient aromatic compounds, including berberine and palmatine. This macrocycle is revealed to be highly biocompatible and able to inhibit the bitter taste of the two drugs.
Supported Pd based catalysts are considered as the efficient candidates for low-carbon alkane oxidation for their outstanding capability to break C-H bond. Whereas, the irreversible deactivation of Pd based catalysts was still frequently observed. Herein, we reinforced the extruded Pd nanoparticles with quantitive Pt to assemble the evenly distributed PdPt nanoalloy onto ferrite perovskite (PdPt-LCF) matrix with strengthened robustness of metal/oxide support interface. We further co-achieved the enhanced performance, anti-overoxidation as well as resistance of vapor-poisoning in durability measurement. The operando X-ray photoelectron spectroscopy (O-XPS) combined with various morphology characterizations confirms that the accumulation of surface deep-oxidation species of Pd4+ is the culprit for fast activity loss in exsolved Pd system, especially at high temperature of 400 ℃. Conversely, it could be completely suppressed by in-situ alloying Pd with equal amount of Pt, which helps maintain the metastable Pd2+/Pd shell and metallic solid-solution core structure. The density function theory (DFT) calculations further buttress that the dissociation of CH was facilitated on alloy/perovskite interface which is, on the contrary, resistant toward O–H bond cleavage, as compared to Pd/perovskite. Our work suggests that the modification of exsolved metal/oxide catalytic interface could further enrich the toolkit of heterogeneous catalyst design.
Lidocaine hydrochloride (LIDH) as an anesthetic is widely used in local anesthesia. Dissolving microneedles (MNs) have great application value in the field of skin anesthesia. However, the limited drug-loading of dissolving MNs is an existing challenge that affects clinical use. In this study, we have screened isomaltulose (ISO) as the proper matrix material for the MNs by using molecular dynamics (MD) simulation. Our findings indicate that ISO has good compatibility with LIDH, and the LIDH-loaded ISO MNs (LI-MNs) have high drug-loading capacity. The drug-loading capacity of LI-MNs could reach 80%, and it could effectively puncture the skin. In addition, the preparation method of customized LI-MNs was established based on three-dimensional (3D) printing technology. It was shown that the administration time of LI-MNs could be controlled within 3 min. Also, the LI-MNs were able to provide the local anesthetic efficacy within 2 min and sustained for more than 2 h. Significantly, LI-MNs had more efficient drug efficacy compared to the topical creams and the majority of existing LIDH-loaded dissolving MNs. They even provided a longer duration of action than the injections. Overall, the LI-MNs with high drug-loading have a promising application prospect.
Inverse vulcanized polymers (IVPs) that generated from elemental sulfur and smaller amounts of alkenes have found broad promising applications such as cathode materials for Li-S batteries, dynamic and repairable materials, optics applications, and metal sorption. However, their exploration in organic synthesis is still unprecedented. Here we first report the application of inverse vulcanized polymers in catalysis for organic transformations. A biomass-derived inverse vulcanized polymer (IVP-EAE) is found to be capable of catalyzing cross-coupling reactions in a transition-metal-free fashion under visible light. This method allows the direct CH functionalization of pyrroles and N-arylacrylamides with (hetero)aryl halides, respectively, leading to the formation of two sets of structurally important scaffolds including pyrrole-containing biaryls and 3,3′-disubstituted oxindoles with high selectivity. We anticipate this study will not only unveil the new potential of IVPs, but also offer a distinct type of catalysts for organic transformations.
Tin-based chalcogenides have attracted tremendous attention as an anode material for sodium storage owing to their unique structure and high theoretical capacity. Unfortunately, the large volume change and poor conductivity lead to sluggish reaction kinetics and poor cycling performance. Herein, SnS0.5Se0.5 nanoparticles coupled with N/S/Se triple-doped carbon nanofibers (SnS0.5Se0.5@NSSe-C) are designed and synthesized through electrospinning and annealing process. Benefiting from the synergistic effects of SnS0.5Se0.5 and NSSe-C, the SnS0.5Se0.5@NSSe-C nanofibers exhibit a high reversible capacity and ultralong cycle life at higher current density for sodium-ion batteries. Furthermore, the sodium storage mechanism and electrochemical reaction kinetics of the SnS0.5Se0.5@NSSe-C composite are characterized by the in-situ measurements. The theoretical calculations further reveal the structural advantages of SnS0.5Se0.5@NSSe-C composite, which exhibits a high adsorption energy of Na+. This work can provide a novel idea for the synthesis of ternary tin-based chalcogenides and is beneficial for the investigation of their reaction kinetics.
Coordination complex of a copper cyanurate (Cu(Ⅱ)-CA) was transformed into coordination polymers upon the stimulus of extra Cu(Ⅱ) through "directed Ostwald ripening". By increasing the molar ratio of Cu(Ⅱ) to CA, we obtained two coordination polymers with selective coordination sites: Cu(Ⅱ)-κN(HCA)κN-Cu(Ⅱ) and Cu(Ⅱ)-κN(HCA)κO-Cu(Ⅱ), which display disparate magnetic interactions.
One of the largest subfamilies within the famous Daphniphyllum alkaloid family is made up of the yuzurimine-type (or macrodaphniphyllamine-type) alkaloids. Their complex aza-polycyclic caged structures, several contiguous stereogenic centers, and vicinal all-carbon quaternary centers make these alkaloids formidable challenge for synthetic chemists. Recently, synthesis of these alkaloids has received extensive attention from our community. Herein, we wish to report the total synthesis of C14–epi-deoxycalyciphylline H, a putative member of yuzurimine-type alkaloid subfamily. Key transformations employed in our approach include an intramolecular Prins reaction and a Pd-catalyzed enyne cycloisomerization. In addition, synthesis of a daphnezomine L-type alkaloid, paxdaphnidine A, was also studied.
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