Drejersmedegaard2600

First total synthesis of the conjugation-ready pentasaccharide repeating unit of Plesiomonas shigelloides strain 302-73 (serotype O1) is reported. The complex target pentasaccharide is composed of all-rare amino sugars such as orthogonally functionalized d-bacillosamine, l-fucosamine, and l-pneumosamine linked through four consecutive α-linkages. The poor nucleophilicity of axial 4-OH of l-fucosamine and stereoselective glycosylations are the key challenges in the total synthesis, which was completed via a longest linear sequence of 27 steps in 3% overall yield.Structural studies of mass-selected biomolecules in the gas phase can reveal their intrinsic properties and provide useful benchmarks for biomolecular modeling. Here, we report the first evidence of transition metal ion FRET (tmFRET) in the gas phase and its application to measure short (10-40 Å) biomolecular backbone distances. The measured FRET efficiencies in rhodamine dye (donor) labeled helical peptides complexed with Cu2+ ions (acceptor) decreased with increasing donor - acceptor distances, confirming the occurrence of tmFRET. The distances estimated for similar peptide sequences from the FRET efficiencies were consistently longer in the gas phase compared to those reported in solution, indicating an expanded structure and a possible loss of helicity.Investigating the behavior of analytes at the electrode surface is crucial in understanding the electrochemical and electrocatalytic reactions. Although Surface Enhanced Raman Scattering (SERS) is sensitive to minor chemical changes in the analyte, it is not widely used to study the reaction mechanisms on nonplasmonic surfaces because of the interference from plasmonic SERS substrates. In this study, we have investigated the redox reaction of Nile Blue A on a glassy carbon surface using pinhole-free silica-coated silver nanoparticles for Raman signal enhancement. The silver nanostructures were synthesized by a chemical reduction method, and the quality of the silica layer was confirmed using microscopic and electrochemical method. The in situ spectroelectrochemical data reveals the catalytic interference from silver which considerably alters the native reaction mechanism. The pinhole-free silica layer prevents the hot electron transfer and yields an interference-free enhancement to the Raman signals.The generation and functionalization, under continuous flow conditions, of two different lithiated four-membered aza-heterocycles is reported. N-Boc-3-iodoazetidine acts as a common synthetic platform for the genesis of C3-lithiated azetidine and C2-lithiated azetine depending on the lithiation agent. Flow technology enables easy handling of such lithiated intermediates at much higher temperatures compared to batch processing. Flow technology combined with cyclopentylmethyl ether as an environmentally responsible solvent allows us to address sustainability concerns.Near-infrared persistent luminescent (or afterglow) nanoparticles with the biologically appropriate size are promising materials for background-free imaging applications, while the conventional batch synthesis hardly allows for reproducibility in controlling particle size because of the random variations of reaction parameters. Here, highly efficient chemistry was matched with an automated continuous flow approach for directly synthesizing differently sized ZnGa2O4Cr3+ (ZGC) nanoparticles exhibiting long persistent luminescence. The key flow factors responsible for regulating the particle formation process, especially the high pressure-temperature and varied residence time, were investigated to be able to tune the particle size from 2 to 6 nm and to improve the persistent luminescence. Upon silica shell encapsulation of the nanoparticles accompanied by an annealing process, the persistent luminescence of the resulting particles was remarkably enhanced. High-fidelity automated flow chemistry demonstrated here offers an alternative for producing ZGC nanoparticles and will be helpful for other compositionally complex metal oxide nanoparticles.Biaryl and indole units are important structural motifs in several bioactive molecules and functional materials. We have accomplished straightforward access to C2-biarylated indole derivatives through palladium-catalyzed C-H activation strategy with a broad range of substrate scope in yields of 24 to 92%. Besides, the UV/visible absorption and fluorescence properties of the ensuing products were explored. The calculated higher dihedral angle and rotational barrier values for the selected C2-biarylated indoles show that these compounds may display atropisomerism at room temperature.The coronavirus SARS-CoV-2 can survive in wastewater for several days with a potential risk of waterborne human transmission, hence posing challenges in containing the virus and reducing its spread. Herein, we report on an active biohybrid microrobot system that offers highly efficient capture and removal of target virus from various aquatic media. The algae-based microrobot is fabricated by using click chemistry to functionalize microalgae with angiotensin-converting enzyme 2 (ACE2) receptor against the SARS-CoV-2 spike protein. click here The resulting ACE2-algae-robot displays fast (>100 μm/s) and long-lasting (>24 h) self-propulsion in diverse aquatic media including drinking water and river water, obviating the need for external fuels. Such movement of the ACE2-algae-robot offers effective "on-the-fly" removal of SARS-CoV-2 spike proteins and SARS-CoV-2 pseudovirus. Specifically, the active biohybrid microrobot results in 95% removal of viral spike protein and 89% removal of pseudovirus, significantly exceeding the control groups such as static ACE2-algae and bare algae. These results suggest considerable promise of biologically functionalized algae toward the removal of viruses and other environmental threats from wastewater.Lithium-sulfur (Li-S) batteries suffer from sluggish sulfur redox reactions under high-sulfur-loading and lean-electrolyte conditions. Herein, a typical Co@NC heterostructure composed of Co nanoparticles and a semiconductive N-doped carbon matrix is designed as a model Mott-Schottky catalyst to exert the electrocatalytic effect on sulfur electrochemistry. Theoretical and experimental results reveal the redistribution of charge and a built-in electric field at the Co@NC heterointerface, which are critical to lowering the energy barrier of polysulfide reduction and Li2S oxidation in the discharge and charge process, respectively. With Co@NC Mott-Schottky catalysts, the Li-S batteries display an ultrahigh capacity retention of 92.1% and a system-level gravimetric energy density of 307.8 Wh kg-1 under high S loading (10.73 mg cm-2) and lean electrolyte (E/S = 5.9 μL mgsulfur-1) conditions. The proposed Mott-Schottky heterostructure not only deepens the understanding of the electrocatalytic effect in Li-S chemistry but also inspires a rational catalyst design for advanced high-energy-density batteries.