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Synthesis of Chiral Saturated Heterocycles Bearing Quaternary Centers via Enantioselective β-C(sp)-H Activation of Lactams.
J Am Chem Soc
January 2025
Department of Chemistry, The Scripps Research Institute, 10550 N. Torrey Pines Road, La Jolla, California 92037, United States.
The development of catalytic methods for the synthesis of enantiopure saturated heterocycles has been a long-standing challenge in asymmetric catalysis. We describe the first highly enantioselective palladium-catalyzed βC(sp)-H arylation and olefination of lactams for the preparation of various chiral N-heterocycles bearing quaternary carbon centers. The presence of strongly electron-withdrawing groups on the chiral bifunctional MPAThio ligand is crucial to the reactivity of weakly coordinating lactams.
View Article and Find Full Text PDFWhat Is the Mechanism by which the Introduction of Amorphous SeO Effectively Promotes Urea-Assisted Water Electrolysis Performance of Ni(OH)?
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January 2025
College of Materials Science and Engineering, Sichuan University, Chengdu, 610065, P. R. China.
Nickel hydroxide (Ni(OH)) is considered to be one of the most promising electrocatalysts for urea oxidation reaction (UOR) under alkaline conditions due to its flexible structure, wide composition and abundant 3D electrons. However, its slow electrochemical reaction rate, high affinity for the reaction intermediate *COOH, easy exposure to low exponential crystal faces and limited metal active sites that seriously hinder the further improvement of UOR activities. Herein it is reported electrocatalyst composed of rich oxygen-vacancy (O) defects with amorphous SeO-covered Ni(OH) (O-SeO/Ni(OH)).
View Article and Find Full Text PDFUnveiling the Dual Active Sites of Ni/Co(OH)-Ru Heterointerface for Robust Electrocatalytic Alkaline Seawater Splitting.
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January 2025
Department of Chemistry, School of Forensic Medicine, China Medical University, Shenyang, 110122, P. R. China.
Constructing bifunctional electrocatalysts through the synergistic effect of diverse metal sites is crucial for achieving high-efficiency and steady overall water splitting. Herein, a "dual-HER/OER-sites-in-one" strategy is proposed to regulate dominant active sites, wherein Ni/Co(OH)-Ru heterogeneous catalysts formed on nickel foam (NF) demonstrate remarkable catalytic activity for oxygen evolution reaction (OER) as well as hydrogen evolution reaction (HER). Meanwhile, the potentials@10 mA cm of Ni/Co(OH)-Ru@NF for overall alkaline water and seawater splitting are only 1.
View Article and Find Full Text PDFRedefining Ketamine Pharmacology for Antidepressant Action: Synergistic NMDA and Opioid Receptor Interactions?
Am J Psychiatry
January 2025
Biobehavioral Imaging and Molecular Neuropsychopharmacology Section, NIDA, Baltimore (Levinstein, Budinich, Michaelides); Department of Pathology and Experimental Therapeutics, Institute of Neurosciences, University of Barcelona, L'Hospitalet de Llobregat, Barcelona (Bonaventura); Neuropharmacology and Pain Group, Neuroscience Program, IDIBELL-Bellvitge Biomedical Research Institute, L'Hospitalet de Llobregat, Barcelona (Bonaventura); Department of Psychiatry and Behavioral Sciences, Stanford University School of Medicine, Stanford (Schatzberg); Experimental Therapeutics and Pathophysiology Branch, NIMH, Bethesda (Zarate); Department of Psychiatry and Behavioral Sciences, Johns Hopkins University School of Medicine, Baltimore (Michaelides).
Ketamine is a racemic compound and medication comprised of ()-ketamine and ()-ketamine enantiomers and its metabolites. It has been used for decades as a dissociative anesthetic, analgesic, and recreational drug. More recently, ketamine, its enantiomers, and its metabolites have been used or are being investigated for the treatment of refractory depression, as well as for comorbid disorders such as anxiety, obsessive-compulsive, and opioid use disorders.
View Article and Find Full Text PDFDual Activation Modes Enable Bifunctional Catalysis of Aldol Reactions by Flexible Dihydrazides.
J Am Chem Soc
January 2025
Department of Chemistry, University of Wisconsin─Madison, 1101 University Avenue, Madison, Wisconsin 53706, United States.
Hydrazides are known to catalyze reactions of α,β-unsaturated aldehydes via transient iminium formation. The iminium intermediate displays enhanced electrophilicity, which facilitates conjugate additions and cycloadditions. We observed that a hydrazide embedded in a seven-membered ring catalyzes homoaldol condensation of a simple aldehyde in a process that displays an approximate second-order dependence on the hydrazide.
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