Notes

Nanowelding to further improve the particular Chemomechanical Stableness of the Ni-Rich Layered Cathode Supplies.
A mild organophotoredox synthetic protocol for forming a Csp3-S/Se bond by reacting widespread redox-active esters with thio/selenosulfonates has been developed. The power of the synthetic manifold is fueled by an unprecedented broad substrate scope and wide functional group tolerance.The highly diastereoselective sulfa-Michael addition of thiolates to enantiopure 2-sulfinyl dienes leads to anti or syn 2-ene-1,4-hydroxy sulfides in good yields and selectivities dependent on the reaction conditions in a diastereodivergent process. Synthetic applications of these enantiopure hydroxy sulfides by subsequent sigmatropic rearrangements have been outlined.Readily available aryldimethylsulfonium triflates react with zinc powder under nickel catalysis via the selective cleavage of the sp2-hybridized carbon-sulfur bond to produce salt-free arylzinc triflates under mild conditions. This zincation displays superb chemoselectivity and thus represents a protocol that is complementary or orthogonal to existing methods. The generated arylzinc reagents show both high reactivity and chemoselectivity in palladium-catalyzed and copper-mediated cross-coupling reactions.Achieving direct C-H hydroxylation in a highly diastereo- and enantioselective manner is still a challenging goal. selleckchem This reaction is mainly hindered by the potential for overoxidation of the generated alcohols as well as low stereoselectivity. Herein, we present an enantioselective benzylic C-H hydroxylation catalyzed by a manganese complex, H2O2, and a carboxylic acid in 2,2,2-trifluoroethanol. The benzylic alcohols were successfully furnished in excellent diastereoselectivities (up to >955) and enantioselectivities (up to 95% ee). As a highlight of this work, high diastereoselectivity of C-H hydroxylation could be achieved by tuning the amount of carboxylic acid additive.Unusual intermolecular trapping of esters by carbenes generated via a Huisgen cyclization/retroelectrocyclization/dediazotization cascade reaction is presented. β-Oxo-N-vinylimidates could be obtained in one step from propargyl carbonazidates. Mechanistic control experiments suggested reversible dipole formation by ester addition to the carbene, and nitrogen attack to the ester carbonyl was irreversibly followed by stereoselective decarboxylative elimination to give the Z-vinyl imidate. The cross-conjugated enone, imidate, and enamine functional groups in the β-oxo-N-vinylimidates offer novel syntheses of functionalized oxazoles.Carbon dioxide (CO2)-philic surfactants have broad application prospects in organic synthesis, fracture-enhanced oil recovery, polymerization, extraction, and other fields and can be used to enhance the viscosity of supercritical CO2 (scCO2). In this work, the relationship between the functional group of the surfactant tail and CO2-philicity is studied from a new perspective using density functional theory. Three common functional group types (fluorinated, oxidative, and methyl groups) were investigated. The analysis of binding energy demonstrates that all three types of functional groups can improve the CO2-philicity of the surfactant. Among these three kinds of functional groups, the strongest interaction with CO2 molecules is observed for oxidative functional groups followed by semifluorinated, fluorinated, and methyl groups. However, the CO2 molecules tend to be adsorbed onto the middle segment of the oxidative group, and the intrusion of the CO2 molecules results in the low solubility of oxidative surfactants. In contrast, fluorinated and methyl groups interact with CO2 at the end of the surfactant tail. As a result, the fluorinated surfactants show the best solubility in CO2. Therefore, the solubility of a surfactant in CO2 is not only related to the interaction strength between the surfactant and CO2, it also depends on the interaction structure. The results of this study provide a new strategy for evaluating surfactant CO2-philicity and provide guidance for the design of surfactants with high solubility in scCO2.Transition-metal-catalyzed dehydrogenative C-H allylation with 1,1-disubstituted alkenes via β-H elimination remains challenging, because of the low reactivity and difficulty of controlling selectivity. Herein, the development of a Pd(II)-catalyzed directed atroposelective C-H allylation with methacrylates is described. Exclusive allylic selectivity was achieved. A vast array of axially chiral biaryl-2-amines are efficiently synthesized with excellent enantioselectivities (up to >99% enantiomeric excess).We developed a nitroxyl-catalyzed bromoesterification of alkenes with bromo reagents, which includes a six-membered ring bromolactonization of alkenyl carboxylic acids catalyzed by AZADO as the nitroxyl radical catalyst, and an intermolecular bromoesterification of alkenes with carboxylic acids using NMO as the N-oxide catalyst. We also accomplished a remote diastereoselective bromohydroxylation via an AZADO-catalyzed six-membered ring bromolactonization and a subsequent ring cleavage reaction with alkylamines to furnish ε-bromo-δ-hydroxy amides with high diastereoselectivity.Nanoscale membrane curvature is a common feature in cell biology required for functions such as endocytosis, exocytosis and cell migration. These processes require the cytoskeleton to exert forces on the membrane to deform it. Cytosolic proteins contain specific motifs which bind to the membrane, connecting it to the internal cytoskeletal machinery. These motifs often bind charged phosphatidylinositol phosphate lipids present in the cell membrane which play significant roles in signaling. These lipids are important for membrane deforming processes, such as endocytosis, but much remains unknown about their role in the sensing of membrane nanocurvature by protein domains. Using coarse-grained molecular dynamics simulations, we investigated the interaction of a model curvature active protein domain, the epsin N-terminal homology domain (ENTH), with curved lipid membranes. The combination of anionic lipids (phosphatidylinositol 4,5-bisphosphate and phosphatidylserine) within the membrane, protein backbone flexibility, and structural changes within the domain were found to affect the domain's ability to sense, bind, and localize with nanoscale precision at curved membrane regions.
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