Latest ArticlesSelective functionalization of C–F bonds in trifluoromethyl groups has recently received a growing interest, as it offers atom- and step-economic pathways to access highly valuable mono- and difluoroalkyl-substituted organic molecules using simple and inexpensive trifluoromethyl sources as the starting materials. In this regard, impressive progress has been made on the defluorinative functionalization reactions that proceed via radical intermediates. Nevertheless, it is still a great challenge to precisely control the defluorination process, due to the continuous decrease of the C–F bond strength after the replacement of one or two fluorine atoms with various functionalities. This review article is aimed to provide a brief overview of recently reported methods used to functionalize C–F bonds of CF3 groups via radical intermediates. An emphasis is placed on the discussion of mechanistic aspects and synthetic applications
Quantum dots-hydrogel composites are promising new materials that have attracted extensive attention due to their incomparable biocompatibility and acceptable biodegradability, leading to enormous potential applications for various fields. This review summarizes the recent advances in quantum dots-hydrogel composites with a focus on synthesis methods, including hydrogel gelation in quantum dots (QDs) solution, embedding prepared QDs into hydrogels after gelation, forming QDs in situ within the preformed gel and cross-linking via QDs to form hydrogels. In particularly, biomedical applications as bioimaging, biosensing and drug delivery are also reviewed, followed by a discussion on the inherent challenges of design optimization, biocompatibility and bimodal applications and the prospect of the future development. These results will guide the development of quantum dots-hydrogel composites and provide critical insights to inspire researchers in future.
Commercial lithium-ion batteries (LIBs) have been widely used in various energy storage systems. However, many unfavorable factors of LIBs have prompted researchers to turn their attention to the development of emerging secondary batteries. Aqueous zinc ion batteries (AZIBs) present some prominent advantages with environmental friendliness, low cost and convenient operation feature. MnO2 electrode is the first to be discovered as promising cathode material. So far, manganese-based oxides have made significant progresses in improving the inherent capacity and energy density. Herein, we summarize comprehensively recent advances of Mn-based compounds as electrode materials for ZIBs. Especially, this review focuses on the design strategies of electrode structures, optimization of the electrochemical performance and the clarification of energy storage mechanisms. Finally, their future research directions and perspective are also proposed.
In recent years, the strategy of inhibiting the interactions of p53 with murine double minute 2 (MDM2) and murine double minute X (MDMX) has been proved to be a promising approach for tumor therapy. However, the poor proteolytical stability and low intracellular delivery efficiency of peptide inhibitors limit their clinical application. Here, we designed and synthesized the bicyclic stapled peptides based on p53 by combining all-hydrocarbon stapling and lactam stapling strategies. We demonstrated that bicyclic stapled peptide p53-16 significantly improved α-helicity and proteolytic stability. Especially, p53-16 showed nanomolar binding affinity for MDM2 and MDMX. In addition, p53-16 could penetrate the cell membrane, and selectively inhibited the activity of tumor cells via activating p53 pathway in vitro. Our data suggest that p53-16 is a potential dual inhibitor of MDM2 and MDMX interactions. The bicyclic stapling strategy is a promising drug design strategy for protein–protein interactions inhibitors.
Development of new self-calibrating fluorescent sensing methods has been a popular research field with the aim of protecting the human health and environment sustainability. In this work, a novel Eu-based metal organic framework (MOF) Eu(2,6-NDC)(COO) (BUC-88) was developed by employing 2,6-NDC (2,6-naphthalenedicarboxylic acid) as bridging ligands. BUC-88 performed different sensing process toward quinolone antibiotics and tetracyclines antibiotics in terms of fluorescence intensity and color. BUC-88 exhibited excellent selectivity and sensitivity detection property toward enrofloxacin (ENR), norfloxacin (NOR) and ciprofloxacin (CIP) over other Pharmaceutical and Personal Care Products (PPCPs), accomplishing the detection limit of 0.12 μmol/L, 0.52 μmol/L, 0.75 μmol/L, respectively. Notably, BUC-88 acted as an excellent fluorescence sensor for tetracyclines antibiotics with fast response time (less than 1 s), high selectivity and sensitivity (LODs = 0.08 μmol/L). The fluorescent detection method was successfully used for visual and ultrasensitive detection of ENR, NOR, CIP and tetracycline hydrochloride (TC) in lake water with satisfied recovery from 99.75% to 102.30%. Finally, the photoinduced electron transfer and the competitive absorption of ultraviolet light are the main mechanisms for sensitive detection toward quinolone antibiotics and tetracyclines antibiotics.
Despite of the hazardous risk of Pb2+ leakage, lead dioxide has been attributed as a quasi-ideal anode material with high oxygen evolution potential, excellent conductivity, good stability and low cost in electrochemical oxidation wastewater treatment technique. In this study, a novel Ti/PbO2 anode was fabricated by embedding raw materials that are readily and cheaply available, i.e., hairs. The structure-activity relationship of the new electrode was firstly revealed by material and electrochemical characterizations. Then different levels of pollutants (azo dye, phenol and maleic acid) were used to investigate the electrochemical oxidation performance of the new electrode. Finally, the accelerated electrode lifetime and Pb2+ leakage tests were carried out. Results showed that the embedded hairs changed the preferential crystallographic orientation of PbO2 and decreased the grain size. Hairs introduced additional roughness and active sites, and decreased the electrode impedance, especially under 5 mg/cm2 of embedding amount. The removal efficiencies of different target pollutants were enhanced more or less by embedding appropriate amount of hairs, depending on the current density, but loading excessive hairs had a negative effect. The accumulation of intermediate products during phenol degradation was also changed by the hairs. The new electrode could undergo ~550 h of harsh electrolysis. It is also relieved that the Pb2+ leakage was found to be suppressed during this long-term electrolysis process.
Molecular self-assembly is the most important strategy for the development of chiral aggregates and chiral functional materials. In this study, we rationally designed and synthesized chiral fluorescent heteroclusters that were self-assembled into microscale cubosomes with a three-dimensional (3D) bicontinuous cubic phase nanostructure. The cubosomes exhibited chirality, indicating that chirality is transferred from the molecules to the 3D nanostructure. Therefore, we confirmed the formation of a chiral bicontinuous cubic phase nanostructure for the first time. We also showed that this chirality originates from the continuous change in the saddle-splay distortion of the molecules within the curved bilayer. At the same time, transparent films of chiral composites were prepared by mixing the chiral cubosomes with an epoxy resin and then curing the mixture. Therefore, we demonstrated an effective method for preparing chiral composites.
Biopolymers, including DNA and peptides have been used as excellent self-assembling building blocks for programmable single-component or hybrid materials, due to their controlled molecular interactions. However, combining two assembling principles of DNA-based programmability and peptide-based specific molecular interactions for hybrid structures to microscale has not yet been achieved. In this study, we describe a hybrid microsystem that emerges from the co-assembly of DNA origami structure and short elastin-like polypeptide conjugated oligonucleotides, and initiates liquid-liquid phase separation to generate microdroplets upon heating above the transition temperature. Moreover, the hybrid microdroplets are capable for guest molecule trapping and perform bi-/tri-enzymatic cascades with rate enhancements as open "microreactors". Our programmed assembled DNA-peptide microsystem represents a new combination of DNA nanotechnology and peptide science and opens potential application routes toward life-inspired biomaterials.
Homocysteine (Hcy), cysteine (Cys) and glutathione (GSH) play crucial roles in redox homeostasis during mitochondria functions. Simultaneous differentiation and visualization of mitochondrial biothiols dynamics are significant for understanding cell metabolism and their related diseases. Herein, a multisite-binding fluorescent probe (MCP) was developed for simultaneous sensing of mitochondrial Cys, GSH and Hcy from three fluorescence channels for the first time. This novel probe exhibited rapid fluorescence turn-on, good water-solubility, high selectivity and large spectral separation for discriminating Cys, GSH and Hcy with 131-, 96-, 748-fold fluorescence increasement at 471, 520, 567 nm through different excitation wavelengths, respectively. Importantly, this probe was successfully applied to simultaneous monitoring of mitochondrial Cys, GSH, and Hcy in live cells and zebrafish from three fluorescence channels, promoting the understanding of the functions of Hcy, Cys and GSH.
N6-methyl adenosine (m6A) is an eminent epigenetic mark in mRNAs that affects a broad range of biological functions in diverse species. However, the chemically inert methyl group prevents a direct labeling of this modification for subsequent detection and sequencing. Therefore, most current approaches for the labeling of m6A still have limitations of relying on the utilization of corresponding methyltransferases, which resulted in the lacking of efficiency. Here we present an approach which selectively alkylated the N6-formyl adenosine (f6A), the key intermediate during chemical oxidation of m6A, with an alkyne functionality that can be further labeled with click reactions. This covalent labeling approach will be able to facilitate in the affinity purification, detection and genome-wide profiling studies.
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