Journal of the American Chemical Society
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Toward a single-layer two-dimensional honeycomb supramolecular organic framework in water.
We have designed and synthesized a rigid stacking-forbidden 1,3,5-triphenylbenzene compound that bears three 4,4'-bipyridin-1-ium (BP) units on the peripheral benzene rings. Three hydrophilic bis(2-hydroxyethyl)carbamoyl groups are introduced to the central benzene ring to suppress 1D stacking of th...
Geometric and Electronic Structure of the Mn(IV)Fe(III) Cofactor in Class Ic Ribonucleotide Reductase: Correlation to the Class Ia Binuclear...
We have studied the Mn(IV)Fe(III) cofactor using nuclear resonance vibrational spectroscopy (NRVS) and absorption (Abs)/circular dichroism (CD)/magnetic CD (MCD)/variable temperature, variable field (VTVH) MCD spectroscopies to obtain detailed insight into its geometric/electronic structure and to c...
Electroanalytical evaluation of antioxidant activity of cerium oxide nanoparticles by nanoparticle collisions at microelectrodes.
We describe a simple, cost-effective and rapid electrochemical screening approach to evaluate antioxidant activity of cerium oxide nanoparticles (CeO2 NPs) by single nanoparticle collision at microelectrodes. The method is based on direct monitoring of the interaction between a Pt microelectrode and...
Interdomain dynamics explored by paramagnetic NMR.
We found the three crystal conformations in solution, but four additional MD-derived conformations had to be included into the ensemble to fulfill all the paramagnetic data and cross-validate optimally against unused paramagnetic data. Alternative approaches led to similar ensembles. Our "ensemble"...
Fluorogenic α-Tocopherol Analogue for Monitoring the Antioxidant Status within the Inner Mitochondrial Membrane of Live Cells.
We report here the preparation of a lipophilic fluorogenic antioxidant (Mito-Bodipy-TOH) that targets the inner mitochondrial lipid membrane (IMM) and is sensitive to the presence of lipid peroxyl radicals, effective chain carriers in the lipid chain autoxidation. Mito-Bodipy-TOH enables monitoring...
β-Ketoenamine-Linked Covalent Organic Frameworks Capable of Pseudocapacitive Energy Storage.
We describe a β-ketoenamine-linked 2D COF that exhibits reversible electrochemical processes of its anthraquinone subunits, excellent chemical stability to a strongly acidic electrolyte, and one of the highest surface areas of the imine- or enamine-linked 2D COFs. Electrodes modified with the redox-...
New insights on photocatalytic h2 liberation from water using transition-metal oxides: lessons from cluster models of molybdenum and tungste...
We investigate the chemical reactions of W3O5(-) and Mo3O5(-) clusters with water that shed light on a variety of key factors central to H2 generation. Our computational results explain why experimentally Mo3O5(-) forms a unique kinetic trap in its reaction while W3O5(-) undergoes a facile oxidation...
The direct oxidative addition of o2 to a mononuclear cr(i) complex is spin forbidden.
Mononuclear chromium(I) alkyne complex (i-Pr2Ph)2nacnacCr(η(2)-C2(SiMe3)2) (1) reacts rapidly with dioxygen to yield chromium(V) dioxo species (i-Pr2Ph)2nacnacCr(O)2 (2). The mechanism of this oxygen cleavage has been studied experimentally and computationally. Isotope labeling studies rule out a di...
Ruthenium catalyzed hydrohydroxyalkylation of isoprene with heteroaromatic secondary alcohols: isolation and reversible formation of the put...
Heteroaromatic secondary alcohols react with isoprene to form products of hydrohydroxyalkylation in the presence of ruthenium(0) catalysts generated from Ru3(CO)12 and tricyclohexylphosphine, enabling direct conversion of secondary to tertiary alcohols in the absence of premetalated reagents or stoi...
Nickel/Bis(oxazoline)-Catalyzed Asymmetric Negishi Arylations of Racemic Secondary Benzylic Electrophiles to Generate Enantioenriched 1,1-Di...
We have developed an efficient method for the synthesis of enantioenriched 1,1-diarylalkanes from readily available racemic benzylic alcohols. Formation of a benzylic mesylate (which is not isolated), followed by treatment with an arylzinc reagent, LiI, and a chiral nickel/bis(oxazoline) catalyst, f...