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The potential drug target choline acetyltransferase (ChAT) catalyzes the production of the neurotransmitter acetylcholine in cholinergic neurons, T‐cells, and B‐cells. Herein, we show that arylvinylpyridiniums (AVPs), the most widely studied class of ChAT inhibitors, act as substrate in an unusual coenzyme A‐dependent hydrothiolation reaction. This in‐situ synthesis yields an adduct that is the actual enzyme inhibitor. The adduct is deeply buried in the active site tunnel of ChAT and interactions with a hydrophobic pocket near the choline binding site have major implications for the molecular recognition of inhibitors. Our findings clarify the inhibition mechanism of AVPs, establish a drug modality that exploits a target‐catalysed reaction
Persistent luminescent nanoparticles (PLNPs) with intrinsic stimuli‐responsive properties are highly desirable for diverse applications because of no autofluorescence background and natural responsive luminescence. However, to our knowledge, the stimuli‐responsive features of pure PLNPs have been unexplored yet. Here we show a facile one‐pot hydrothermal synthesis of green‐emitting Zn2GeO4:Mn2+,Pr3+ nanoparticles (ZGMP) with regular shape, uniform size, good afterglow luminescent performance. We also report the pH stimuli‐responsive luminescent behavior of ZGMP and its possible mechanism. Taking the intriguing feature of pH responsive persistent luminescence, we explore ZGMP as autofluorescence‐free probes to achieve stimuli‐activated signa.
The design of synthetic routes via retrosynthetic logic is decisively influenced by the transformations available. In this context, transition metal‐catalyzed C–H activation has emerged as a powerful strategy for C–C bond formation, with myriad methods developed for diverse substrates and coupling partners . Despite its interest and proven efficacy however, its uptake in the total synthesis has been tepid, partially owing to their apparent synthetic intractability and inapplicability, as well as a lack of comprehensive guidelines for their implementation. These issues are addressed in this review, where we guide the identification of retrosynthetic opportunities to incorporate C–H activation processes for the generation of C–C bonds. By com.
A triplet radical‐radical complex consisting of a hydroxyl radical and phosphorus monoxide (.OH⋅⋅⋅OP.), which serves as an important intermediate in the combustion of phosphines, has been captured in solid Ar‐matrices at 2.8 K. Its interconversion with metaphosphorous acid (cis‐HOPO) has also been observed. Abstract. Phosphorus monoxide (.PO) is a key intermediate in phosphorus chemistry, and its association with the hydroxyl radical (.OH) to yield metaphosphorous acid (cis‐HOPO) contributes to the chemiluminescence in the combustion of phosphines. When photolyzing cis‐HOPO in an Ar‐matrix at 2.8 K, the simplest dioxophosphorane HPO2 and an elusive hydroxyl radical complex (HRC) of .PO form. This prototypical radical‐radical complex reforms
The formal (4+3) cycloaddition of 1,3‐dienes with Rh(II) and Au(I) non‐acceptor vinyl carbenes, generated from vinylcycloheptatrienes or alkoxyenynes, respectively, leads to 1,4‐cycloheptadienes featuring complex and diverse substitution patterns, including natural dyctiopterene C’ and a hydroxylated derivative of carota‐1,4‐diene.
Biomimetic breathing micelles which can simultaneously inhale nitric oxide and exhale carbon monoxide are developed by T. You, J. Hu et al. in their Communication (DOI: 10.1002/anie.202010009). The breathing micelles show a combinatorial anti‐inflammatory performance in the treatment of autoimmune inflammatory diseases such as rheumatoid arthritis, outperforming any single ingredient of the breathing micelles and commercially available NSAIDs such as dexamethasone.
Engineering multifunctional nanoplatform with high therapeutic benefits has become a promising strategy for intractable cancer treatment. Here, a novel polyphenol‐based nanocomplex is thus designed to evoke highly efficacious cancer immunosurveillance while localizing therapy on primary tumor and to minimize systemic side effects. This nanocomplex is prepared via a metal‐polyphenol coordination process by encapsulating a natural polyphenol gossypol and a newly synthesized polyethylene glycol‐Chlorin e6 (Ce6) polyphenol derivative. The combination of gossypol from cotton plant and photosensitizer Ce6 can induce chemotherapeutic/photodynamic immunogenic cancer cell death upon laser irradiation, which is supported by rich maturation of dendrit.
Heterogeneous Bi‐BTC successfully catalyzed a promising yield (92%) of para‐xylene from bio‐based 2,5‐dimethylfuran and acrylic acid conversion, under relatively mild conditions ( < 160 ºC, 10 bar) with low reaction energy barrier (47.3 kJ/mol). The proposed reaction strategy also demonstrated remarkable versatility for furan derivatives such as furan and 2‐methylfuran.
Intermolecular bond formations among Pt atoms in oligomers of PtII complexes are induced by photo‐irradiation. Femtosecond time‐resolved absorption measurements for aqueous solutions of K2[Pt(CN)4] recorded clear oscillations of transient absorption in the first few picoseconds with complex dynamics. The oscillations arise from the Pt−Pt stretch motions of the S1 trimer and S1 tetramer. The analysis of the oscillations provides clear assignments of the oligomers, as described by M. Iwamura, T. Tahara et al. their Research Article (DOI: 10.1002/anie.202011813).
The synthesis of an NHC‐containing porphyrinoid ligand is presented. The formally antiaromatic 20 πe− macrocyclic framework can be obtained via a 1,3‐dipolar cycloaddition (“click‐reaction”) to form two triazole moieties which were alkylated to the respective triazolium macrocycle. Deprotonation of the ligand precursor with lithium bases to the respective dilithio carbena­porphyrin complex and transmetallation to scandium lead to complexes that exhibit orange fluorescence. Optical property combined with TD‐DFT studies verify an aro­matic character for each heterocyclic moiety rather than an anti­aromatic macrocycle in the ligand precursor as well as in the com­plexes. While the geometric features of the carbenaporphyrin ligand strongly rese.
Aprotic Na‒O 2 batteries have attracted growing interest due to their low overpotentials and high energy density. Their cycling stability and Coulombic efficiency are limited, however, by Na dendrite formation and superoxide (O 2 ‐ ) degradation. Here, we present a bifunctional cation additive, tetrabutylammonium cations (TBA + ), to simultaneously protect the Na anode and stabilize the superoxide. The adsorption of TBA + on the Na anode suppresses the dendrite formation in the Na plating and ensures stable anode cycling at high current density in both Ar and oxygen atmospheres. In addition, the aprotic Na‒O 2 batteries with TBA + show increased Coulombic efficiency as well as good rate capability. These are rewarded by the fast desolvation.
Well‐defined assemblies of photosynthetic protein com­plexes are required for an optimal performance of semi‐artificial ener­gy conversion devices, capable of providing unidirectional electron flow when light‐harvesting proteins are interfaced with electrode sur­faces.
Hydrogen bonding is a key governing force in molecular recognition, notably in biological systems. While it has been studied and exploited by supramolecular chemists for many years, most of this work has been conducted in organic solvents. Investigations in water, the biological solvent, have proceeded more slowly, largely because the interaction is weakened by solvation and less easy to detect. Recently it has become appreciated that the problems should be addressed, and work towards the deployment of H‐bonding in water has accelerated. This minireview discusses a range of synthetic receptors designed to bind organic molecules in aqueous media by combining hydrogen bonding with hydrophobic interactions. Some of these systems are capable of.
C–H/N–H cross‐coupling represents an ideal strategy to synthesize various amines but remains challenging due to the requirement for sacrificial chemical oxidants and the difficulty in controlling the regio‐ and chemo‐selectivity. Herein we report a site‐selective electrochemical amination reaction that can convert benzylic C–H bonds to C–N linkages via H 2 evolution without need for external oxidants or metal catalysts. The synthetic strategy involves anodic cleavage of benzylic C–H to form a carbocation intermediate, which is then trapped with an amine nucleophile leading to C–N bond formation. Key to the success is to include HFIP as a cosolvent to modulate the oxidation potentials of the alkylbenzene substrate and the aminated product to.
Dinuclear cages are metallo‐supramolecular hosts assembled from a minimum of components. Numerous examples for the most trivial, lantern‐shaped topology (two metals bridged by three or four bowed ligands) have been reported, but other structural motifs are rare. In their Communication (DOI: 10.1002/anie.202010995), G. H. Clever et al. detail a new variety for a [Pd2Ligand4] assembly, consisting of two figure‐eight‐shaped chelate complexes, doubly connected by mechanical bonds. The chiral ligands are based on peptidic macrocycles, giving the nano‐sized object a natural product‐like character.
Prodrug and drug delivery systems are two effective strategies for improving the selectivity of chemotherapeutics. Molecularly imprinted polymers (MIPs) have emerged as promising carriers in targeted drug delivery for cancer treatment, but have not yet been integrated with the prodrug strategy. Herein we report an MIP‐based smart prodrug delivery system for specific targeting, prolonged retention and tumor microenvironment‐triggered release. 5’‐deoxy‐5‐fluorocytidine (DFCR) and sialic acid (SA) were used as a prodrug and a marker for tumor targeting, respectively. Their co‐imprinted nanoparticles were prepared as a smart carrier. Prodrug‐loaded MIP specifically and sustainably accumulated at the tumor site and then gradually released. Unlik.
Hydrogen‐bonded structures of water in a self‐organized subnanoporous water treatment membrane obtained using soft X‐ray emission spectroscopy indicate that structural consistency among associated hydrogen‐bonded water molecules contributes to ion selectivity.

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