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A bifunctional 3d‐metal catalyst for the cascade synthesis of diverse pyrroles from nitroarenes is presented. The optimal catalytic system Co/NGr@SiO 2 ‐L is obtained by pyrolysis of a cobalt‐impregnated composite followed by subsequent selective leaching. In the presence of this material, (transfer) hydrogenation of easily available nitroarenes and subsequent Paal‐Knorr/Clauson‐Kass condensation provides >40 pyrroles in good to high yields using dihydrogen, formic acid, or a CO/H 2 O mixture (WGSR conditions) as reductant. In addition to the favorable step economy, this straightforward domino process does not require any solvents or external co‐catalysts. The general synthetic utility of this methodology was demonstrated on a variety of fu.
Hypoxia is a parameter related to many diseases. Ratiometric hypoxia probes often rely on a combination of an O 2 ‐insensitive fluorophore and an O 2 ‐sensitive phosphor in a polymer matrix, which are comprised by high cost and multi‐step synthesis of transition metal complexes. The two‐chromophore hypoxia probes encounter unfavorable energy transfer processes and different stabilities of the chromophores. Reported herein is a pure organic ratiometric hypoxia nanoprobe, assembled by a monochromophore, naphthalimide ureidopyrimidinone (BrNpA‐UPy) bridged by a bis‐UPy functionalized benzyl skeleton. The joint factors of quadruple hydrogen bonding, the rigid backbone of UPy, and bromine substitution of naphthalimide derivative facilitate brigh.
Physical separations can be superior to chemical separations when it comes to energetics and kinetics, especially when ideal sieving is feasible among hard‐to‐separate gas mixtures. Unfortunately, for industrial gases a very precise pore window size which must be ultramicroporous is needed for ideal sieving. In their Research Article (DOI: 10.1002/anie.202006414), Y. Huang, M. J. Zaworotko et al. describe a new variant of Ca‐trimesate that offers just the right pore size (0.31 nm) to enable ideal sieving of H2 from CO2, two of the primary components of syngas.
Magnetically induced alignment in NMR can be used as a convenient way to determine the configuration of small molecules. C. Griesinger et al. show in their Communication (DOI: 10.1002/anie.202004881) how the necessary anisotropic NMR data can be acquired exploiting the molecule's anisotropic magnetic susceptibility. This approach is demonstrated on the novel natural product gymnochrome G, which was isolated from a deep‐sea crinoid. Cover Illustration: A. Savastano.
Protein semi‐synthesis inside live cells from exogenous and endogenous parts offers unique possibilities for studying proteins in their native context. Split‐intein mediated protein trans ‐splicing is predestinated for such endeavors and has seen some successes, but a much larger variety of established split inteins and associated protocols is urgently needed. We characterized the association and splicing parameters of the Gp41‐1 split intein, which favorably revealed a nanomolar affinity between the intein fragments combined with the exceptionally fast splicing rate. Following bead‐loading of a chemically modified intein fragment precursor into live mammalian cells, we fluorescently labeled target proteins on their N and C termini with sho.
The potential of a dicationic strontium ansa ‐arene complex for Lewis‐acid catalysis has been explored. The key to its synthesis was a simple salt metathesis from SrI 2 and 2 Ag[Al(OR F ) 4 ] giving the base‐free strontium‐perfluoroalkoxyaluminate Sr[Al(OR F ) 4 ] 2 (OR F = OC(CF 3 ) 3 ). Addition of the ansa ‐arene yielded the highly Lewis‐acidic, dicationic strontium ansa ‐arene complex. In preliminary experiments, it was successfully applied as catalyst in a CO 2 ‐reduction to CH 4 and a surprisingly controlled isobutylene polymerization.
Previously described Lewis superacids are moisture sensitive and predominantly hard in character – features that are severely limiting their widespread use in orbital controlled reactions and under non‐inert conditions. Herein, we describe adducts of bis(perchlorocatecholato)germane, the first hard and soft Lewis superacid based on germanium. Remarkably, the synthesis of this compound is performed in water, and the obtained H 2 O‐adduct constitutes a strong Brønsted acid. If applied as adduct with aprotic donors, it displays excellent activity in a diverse set of Lewis acid catalyzed transformations, covering hydrosilylation, hydrodefluorination, transfer hydrogenation, and carbonyl‐olefin metathesis. Given the very straightforward syntheti.
Chalcogen bonds are σ hole interactions and have been used in recent years as an alternative to hydrogen bonds. In general, the electrostatic potential at the chalcogen atom and orbital delocalization effects are made responsible for the orientation of the chalcogen bond. Here, we were able to show by means of SAPT calculations that neither the induction (orbital delocalization effects) nor the electrostatic term is causing the spatial orientation of strong chalcogen bonds in tellurium‐containing aromatics. Instead, steric interactions (Pauli repulsion) are responsible for the orientation. Against chemical intuition the dispersion energies of the examined tellurium‐containing aromatics are far less important for the net attractive forces co.
A new DNA architecture addresses the question, how far energy migrates in DNA and forms cyclobutane pyrimidine dimers (CPDs) as photodamages causing skin cancer. The 3‐methoxyxanthone nucleoside allows site‐selective photoenergy injection into DNA. The designated CPD site lacks the phosphodiester bond and can be placed in defined distances. The CPD formation links two oligonucleotides together and allows probing by gel electrophoresis. We obtained a sigmoidal distance dependence with R 0 of 25±3 Å. Below R 0 , short‐range energy migration occurs with high CPD yields and shallow distance dependence, characteristic for a coherent process. 5‐methyl‐C as epigenetic modification on the 3’‐side facilitates CPD formation. Above R 0 , long‐range in.
A wide range of tunability in physical parameters of a semiconductor used for X‐ray detection is desirable to achieve targeted performance optimization. However, in a dense‐phase semiconductor, fine‐tuning one parameter often leads to unwanted changes in other parameters. Herein, the intrinsic openness in an open‐framework semiconductor has been proven for the first time to be a key structural factor that weakens the mutual exclusivity of the adjustable physical parameters owing to a non‐linear control mechanism. The controllable doping of S into a zeolitic In‐Se host results in an optimal balance between resistivity, band gap, and carrier mobility, which finally results in an excellent X‐ray detector with a high figure‐of‐merit of the mobi.
DNAzymes are widely used as functional units for creating DNA‐based sensors and devices. Switching of DNAzyme activity by external stimuli is of increasing interest. Herein we report a Cu II ‐responsive DNAzyme rationally designed by incorporating one of the most stabilizing artificial metallo‐base pairs, a Cu II ‐mediated carboxyimidazole base pair ( Im C –Cu II – Im C ), into a known RNA‐cleaving DNAzyme. Cleavage of the substrate was suppressed without Cu II , but the reaction proceeded efficiently in the presence of Cu II ions. This is due to the induction of a catalytically active structure by Im C –Cu II – Im C pairing. The on–off ratio was as high as 12‐fold, which far exceeds that of the previous DNAzyme having a Cu II ‐mediated hyd.
Developing a facile controllable avenue to selective semihydrogenation of alkynes to alkenes with a defined configuration using a cheap and safe hydrogen donor is highly desirable, but remains a big challenge. Here, we reported a selective semihydrogenation (deuteration) of numerous terminal and internal alkynes using H 2 O (D 2 O) as the H (D) source over a Pd‐P alloy cathode at a lower potential. Density functional theory (DFT) calculation revealed that the doping of P caused the enhanced specific adsorption of alkynes and the promoted intrinsic activity for producing adsorbed atomic hydrogen (H* ads ) from water electrolysis. The semihydrogenation of alkynes could be accomplished at a lower potential with up to 99% selectivity and 78% Fa.
By virtue of the unique feature of Shewanella oneidensis MR‐1 ( S. oneidensis MR‐1) that anaerobically catabolize lactate through transferring electrons to metal minerals for respiration, a lactate‐fueled biohybrid (Bac@MnO 2 ) here is constructed by modifying manganese dioxide (MnO 2 ) nanoflowers on the S. oneidensis MR‐1 surface.
Spontaneously blinking dyes eliminated the requirements of intense laser irradiations and additives to induce fluorophore blinking and greatly facilitated single‐molecule localization microscopy (SMLM) in live‐cell super‐resolution imaging. While the spontaneously blinking had been demonstrated via the thermally induced spirocyclization equilibrium of rhodamines, the stringent requirement on this equilibrium sets a formidable obstacle for the creation of multi‐colored spontaneously blinking rhodamines. Consequently, only a few such dyes were developed to date. Herein, we reported a simple, fast, and quantitative theoretical descriptor Δ G C‐O that allows accurate predictions of a wide range of spontaneously blinking rhodamines. Δ G C‐O deno.
Phenylfuropyridone natural products from fungi exhibit a range of antibacterial and cytotoxicity activities, and can potentiate azole antifungals. Herein, we report the concise biosynthetic pathway of compounds in the citridone family through heterologous reconstitution of the pfp pathway. We demonstrate multiple members of this family can be accessed from a reactive ortho‐ quinone methide (QM) intermediate through electrocyclization, cycloisomerization or conjugated addition. Formation of the quaternary carbon in citridone B is catalyzed by an epoxide‐forming P450, followed by carbon skeletal rearrangement. Our results showcase how nature harvests the reactivities of an enzymatically generated o‐ QM to biosynthesize complex natural product.
The fusion and fission behaviors of exosomes are essential for the cell‐to‐cell communication. Developing exosome‐mimetic vesicles with such behaviors is of vital importance, but still remains a big challenge. Herein, we present an artificial supramolecular vesicle that exhibits redox‐modulated reversible fusion‐fission functions. These vesicles tend to fuse together and form large‐sized vesicles upon oxidation, while undergo a fission process and return to small‐sized vesicles through reduction. Noteworthy, the aggregation‐induced emission (AIE) characteristics of the supramolecular building blocks enable the molecular configuration during vesicular transformation to be monitored by fluorescence technology. Moreover, the presented vesicles.
The amination of racemic alcohols to produce enantiopure amines is an important green chemistry reaction for pharmaceutical manufacturing, requiring simple and efficient solutions. Here we developed a novel concept and the simplest system for ADH‐TA‐catalyzed cascade reaction to aminate racemic alcohols, which utilizes an ambidextrous ADH to oxidize a racemic alcohol, an enantioselective transaminase to convert the ketone intermediate to chiral amine, and isopropylamine to recycle PMP and NAD + cofactors via the reversed cascade reactions. The concept was proven by using an ambidextrous CpSADH‐W286A engineered from ( S )‐enantioselective CpSADH as the first example of evolving ambidextrous ADHs, an enantioselective BmTA, and isopropylamine.
A general and direct synthesis of dicarboxylic acids including industrially important adipic acid by palladium‐catalyzed dicarbonylation of allylic alcohol is reported. Specifically, the combination of PdCl2 and a bisphosphine ligand (HeMaRaphos) promotes two different carbonylation reactions with high activity and excellent selectivity.
Monitoring multiple molecular probes simultaneously establishes their correlations and reveal the holistic mechanism. Current fluorescence imaging, however, is limited to about four colors because of typically ~100‐nm spectral width. Here we show that molecular supracence imparts superior spectral resolution, resolving eight colors in 300‐nm width, about 37.5‐nm per color. A recently discovered light‐molecule interacting phenomenon, supracence only measures molecular emission above its excitation energy due to entanglement between atomic quantum system and electronic quantum system. As such, supracence takes advantage of sharp spectral edge and excitation specificity to produce narrow bands, whereas fluorescence has to deal with the low‐ene.


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