Latest ArticlesWater splitting by photoelectrochemical (PEC) processes to convert solar energy into hydrogen energy using semiconductors is regarded as one of the most ideal methods to solve the current energy crisis and has attracted widespread attention. Herein, Co-based metal-organic framework (Co(bpdc)(H2O)4 (Co-MOF) nanosheets as passivation layers were in-situ constructed on the surface of BiVO4 films through an uncomplicated hydrothermal method (Co-MOF/BiVO4). Under AM 1.5G illumination, synthesized Co-MOF/BiVO4 electrode exhibited a 4-fold higher photocurrent than bare BiVO4, measuring 6.0 mA/cm2 at 1.23 V vs. RHE in 1 mol/L potassium borate electrolyte (pH 9.5) solution. Moreover, the Co-MOF/BiVO4 film demonstrated a 96% charge separation efficiency, a result caused by an inhibited recombination rate of photogenerated electrons and holes by the addition of Co-MOF nanosheets. This work provides an idea for depositing inexpensive 2D Co-MOF nanosheets on the photoanode as an excellent passivation layer for solar fuel production.
Activity-based Ubiquitin probes (Ub-ABPs) carrying a reporter group have emerged as effective tools for the investigation of deubiquitinating enzymes (DUBs), such as studying the molecular mechanism of DUBs, profiling new DUBs. But so far, the synthesis of commonly used biotin-bearing Ub-ABPs is a technical challenge. Here, we report a one-pot semi-synthetic strategy for the acquiring of Ub-ABPs carrying a biotin tag through sequential enzymatic ligation, N-S acyl transfer and aminolysis reaction without any purification steps. These probes enable to capture the different family of DUBs for enrichment and immunoblotting using the attached biotin tag.
A new Rh(Ⅲ)-catalyzed aldehydic C-H activation/[4 + 3] annulation cascade of N-sulfonyl-2-aminobenzaldehydes with gem-difluorocyclopropenes is reported for the first time, and used to produce a range of hitherto unreported precedented β-monofluorinated benzo[b]azepin-5-ones with good yields and complete regioselectivity. This approach features a broad substrate scope, good functional group tolerance, and high regioselectivity, which may include Rh(Ⅲ)-catalyzed aldehydic C−H activation, tandem site-/regioselective insertion, defluorinated ring-scission, and 1, 2-elimination.
The Ni−Al bimetallic catalysis of intramolecular enantioselective and regioselective C−H cyclization of 4-oxoquinazolines with tethered alkenes has been successfully developed. Some new secondary phosphine oxides (SPOs) with large steric hindrance (SPO6-11) were designed and successfully synthesized from readily available chiral amines or amino acids. The developed chiral SPOs as ligands or preligands demonstrate much higher efficiency in the asymmetric catalytic reactions than the reported traditional ones. A new class of chiral tricyclic pyrroloquinazolinones were obtained in up to 95% yield and 99% ee.
Bicyclic peptides, a class of polypeptides with two loops within their structure, have emerged as powerful tools in the development of new peptide drugs. They have the potential to bind to challenged drug targets, with antibody-like affinity and selectivity. Meanwhile, bicyclic peptides possess small molecule-like access to chemical synthesis, which is conducive to large-scale synthesis and screening. In the last five years, bicyclic peptide technology has been increasingly developed, and researchers have carried out a variety of studies to elucidate the potential functions of bicyclic peptides. With the continuous development of synthetic methods and the advances of new technology to build bicyclic peptide libraries, bicyclic peptides are now becoming widely used in the development of new drugs for various diseases. This perspective provides an overview of the structure types, synthesis and applications of bicyclic peptides in current drug development, and our own views on future challenges of bicyclic peptides.
Chirality is one of the most important features of the nature. The recognition of enantiomers plays significant roles in the field of life science, pharmaceutical analysis and food chemistry. Among various recognition methods, fluorescence spectrometry has attracted much attention of researchers thanks to its high sensitivity and easy operation. Compared with traditional fluorescent probes, chiral molecules with aggregation-induced emission (AIE) have drawn increasing interests due to their huge potential in high-efficiency chemo/biosensors and solid emitters. Chiral AIE luminogens (AIEgens) can not only discriminate two enantiomers with excellent enantioselectivity, but also show general applicability for many chiral analytes, such as chiral acids, amino acids, amines, alcohols. In this review, we mainly summarized the recent development of chiral probes with AIE properties, including chiral tetraphenylethylene (TPE) derivatives, α-cyanostilbene derivatives, Schiff base derivatives and other AIEgens. Their synthetic routes, recognition capabilities and possible working mechanisms were well discussed. It is envisioned that the present review can give some significant guidance for design and synthesis of chiral AIEgens with good enantioselectivity and inspire more readers to join the research of chiral AIE.
A novel route of enzalutamide was developed in five steps. Starting from 4-amino-2-(trifluoromethyl)benzonitrile (7) and Boc-2-aminoisobutyric acid (16), condensation, deprotection, Ullmann coupling, cyclization and amination provided enzalutamide in 41.0% total yield. This route avoids the using of toxic chemical, unstable intermediate and high-risk reaction. It is a potential efficient and economical procedure for industrialization.
Microneedles are considered to be an effective, convenient, non-invasive, biosafety and compliant medical technology for vaccinations, biomarker testing, medical aesthetics and other related fields. Nonetheless, further clinical and commercial translation of regular microneedles is hampered by challenges in manufacturability, cost variability, insufficient comfort, contamination and so on. Recent innovations in functional biomaterials and chemical engineering technologies have been applied to develop extensible and swellable hydrogel-forming microneedles, achieving precise and controlled drug delivery and localized sampling from the target tissues. In this review, we systematically summarize the latest development of the extensible and swellable hydrogel-forming microneedles, including deep point-of-care testing, drug deployment, wound healing and mucoadhesion improvement. In addition, further analysis of the challenges and prospects for clinical application of current strategies is well presented. It is believed that the combined efforts of engineering, material, pharmaceutical and clinical research will contribute to the future success of this clinical and commercial translation.
Heterogeneous Fenton has been widely used in the disposal of organic pollutants, however, slow regeneration of Fe(Ⅱ) remains limitation for its practical application of long-term treatment. Herein, we come up with a novel Fe-based heterogeneous Fenton catalyst named as FeSxOy-X (X is the ratio of ethylene glycol to N, N-dimethylformamide). With the help of the abundant defect electrons in Sulfur vacancies, Fe(Ⅱ) regeneration on the surface of FeSxOy-1:1 was accelerated, resulting in a stable proportion of Fe(Ⅱ) on the surface, which maintained continuously stable generation of hydroxyl radical (•OH) and singlet oxygen (1O2). Thus, without any organic reagents or cocatalysts, FeSxOy-1:1 based Fenton system achieved effective long-term degradation of 560 mg/L quinoline within only 7 days, which was evidently better than reported FeS and SV-FeS2 (SV: Sulfur vacancy). The system had excellent adaptability to water quality and the COD removal rate of biochemical wastewater was as high as 79.8%.
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