Latest ArticlesThe design and preparation of luminescent M2L3 metal-organic cage via the coordination-driven selfassembly of carbazole-based ligand with a V-shaped geometry is described. The cage Zn-L1 with an open cavity which equipped aromatic rich ligands shows the highest emission quenching efficiency towards picric acid than other nitroaromatic explosives. The quenching ability depended on whether there formed the host-guest molecules are well explored by electrospray ionization mass spectrometry (ESIMS), and isothermal titration microcalorimetry (ITC).
Novel highly sensitive chiral organic field-effect transistors (COFET) were developed by directly assembling imidazolium3, 5-dimethylphenylcabamoylated-β-cyclodextrin(Im+-Ph-β-CD)and 3, 5-dimethylphenylcarbamoylated-β-CD (Ph-β-CD) respectively onto the semiconductor layer as sensing units. The Im+-Ph-β-CD/COFET afforded better enantioselectivity and a lowest detection concentration of 10 18 L/mol as well as the potentiality in quantitative analysis of commercial medicines.
A ruthenium based catalytic system ([Ru(p-cymene)Cl2]2/XantPhos with substoichiometric Cs2CO3) has been established to effectively achieve the first direct amination cyclization of 1, 2, 4-butanetriol with primary aromatic amines. The product of this sustainable hydrogen autotransfer process is valuable Naryl-3-pyrrolidinol.
TNFR1-associated death domain protein (TRADD) with arginine N-GlcNAcylation is a novel and structurally unique posttranslational modification (PTM) glycoprotein that blocks the formation of death-inducing signaling complex (DISC), orchestrating host nuclear factor kB (NF-kB) signaling in entero-pathogenic Escherichia coli (EPEC)-infected cells. This particular glycosylated modification plays an extremely vital role for the effective colonization and pathogenesis of pathogens in the gut. Herein we describe the total synthesis of TRADD death domain (residues 195-312) with arginine235 N-GlcNAcylation (Arg-GlcNAc TRADD (195-312)). Two longish peptidyl fragments of the wild-type primary sequence were obtained by robust, microwave-assisted, highly efficient, solid-phase peptide synthesis (SPPS), the N-GlcNAcylated sector was built by total synthesis and attached specifically to resinbound peptide with an unprotected ornithine residue via silver-promoted on-resin guanidinylation, Arg-GlcNAc TRADD (195-312) was constructed by hydrazide-based native chemical ligation (NCL). The facile synthetic strategy is expected to be generally applicable for the rapid synthesis of other proteins with Arg-GlcNAc modification and to pave the way for the related chemically biological study.
The construction of N-methyl amine moieties is an important reaction that has found numerous applications. Development of new methylation agents that are more environmentally benign than classical agents, such as iodomethane and methyl sulfate, is still highly desirable. Herein, we report a convenient protocol for direct reductive N-methylation of amines using formic acid as the methylation agent via simple inorganic base catalysis. The present protocol operates under transition-metal-free and air-tolerant conditions. Both the catalyst, K2HPO4, and the reductant, polymethylhydrosiloxane (PMHS), are cheap and easily separable from the crude reaction product mixture. Mechanistic investigations suggest that the reaction occur through the formation of an acetal intermediate followed by the C-N bond formation.
Polymeric carbon nitride (CN) semiconductor by thermal condensation of N-rich precursors has attracted much attention for its capability ranging from photocatalytic and photoelectrochemical energy conversion to biosensing. However, the influence of condensation process on the final structure of CN was rarely studied, making the condensation kinetic far from be fully optimized. Herein, we report the preparation of CN by a simple condensation kinetics modulation using a faster ramping rate during the polymerization process. The modified condensation recipe was even simpler than the conventional one, but led to an improved photocatalytic H2 evolution up to 3 times without any additional chemicals or other complements. Detailed mechanism studies revealed the increase of crystallinity and surface area due to the rapid condensation played the key roles. This work would offer a more facile and effective way to prepare bulk CN for large-scale industrial applications of bulk CN with higher photocatalytic actives for sustainable energy, environmental and biosensing.
Two A-B-C type conjugated amphiphilic triblock fullerene derivatives C60-2HMTPB and C60-2EHTPB were obtained in multi steps synthesis with three different blocks, and the amphiphilic diblock molecular C60-4TPB was also preferred as a reference. When as modifying layer on zinc oxide (ZnO), the three fullerene derivatives can all reduce the work function of ZnO via modulation of the interfacial dipoles and lead a better electrical coupling. As introducing treatment of toluene, the obvious self-assembly of fullerene derivatives were observed, which were supported by X-ray diffraction and contact angle of water measurement. Base on PTB7-Th:PC71BM system, the inverted organic solar cells devices with structure of ITO/ZnO/fullerene derivatives/PTB7-Th:PC71BM/MoO3/Al got power conversion efficiencies of 8.62%, 8.83% and 9.00% for C60-4TPB, C60-2HMTPB and C60-2EHTPB, respectively, compared 8.13% of devices with bare ZnO. The result of conjugated amphiphilic triblock fullerene derivatives provides a straightforward approaching by simultaneously modulating the morphology and interfacial work function of ZnO, which can also lead high performance in optoelectronic devices.
Alkaline phosphatase (ALP) is one of essential biomarkers in mammalian tissue. Here we report a ratiometric probe for ALP, which is rationally designed and synthesized by employing ESIPT fluorophore N-(3-(benzo[d]thiazol-2-yl)-4-hydroxyphenyl)benzamide (BTHPB). The enzymatic dephosphorylation converts the probe to BTHPB, which exhibits a large spectral red-shift (120 nm), allowing extremely high sensitivity of ALP sensing at 0.004 mU/mL. The probe also shows excellent biocompatibility and has been applied for monitoring the endogenic ALP in living cells.
A coumarinocoumarin-based fluorescent probe, JCCA, was developed for the detection of N2H4. JCCA exhibited a fast turn-on fluorescence enhancement in response to N2H4 with good selectivity, sensitivity and a detection limit of 7.4 nmol/L. Significantly, JCCA displayed a good capability for visualizing N2H4 in living cells and zebra fish.
Cysteine (Cys) plays a pivotal role in many physiological and pathological processes, including detoxification and protein synthesis. The abnormal levels of Cys are linked to many diseases. In this study, a novel red-emitting off-on fluorescent probe Cys-TCF was masterly constructed for discriminative detection of Cys. After a series of experimental assessment, Cys-TCF displayed higher selectivity and sensitivity for Cys over other biothilols with a low detection limit (0.04 μmol/L). More notably, the probe was also successfully applied to image Cys in live cells and live zebrafishes with low cytotoxicity.