279 research outputs found

    ESR evidence for disordered magnetic phase from ultra-small carbon nanotubes embedded in zeolite nanochannels

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    A multi-frequency electron spin resonance (ESR) study provides evidence for the occurrence of low temperature ferromagnetic/spin-glass behavior in aligned arrays of sub-nanometer single walled carbon nanotubes confined in zeolite nano-channels, owing to sp2-type non-bonding carbon associated localized states with density of ~3 x 1019 /g. Features related to the much anticipated conduction ESR are not detected. In the paramagnetic phase, the ESR linewidth is found to be weakly dependent on microwave frequency.Comment: Accepted to be published in EuroPhysics Letter

    Lower Intrinsic ADP-Stimulated Mitochondrial Respiration Underlies In Vivo Mitochondrial Dysfunction in Muscle of Male Type 2 Diabetic Patients

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    OBJECTIVE—A lower in vivo mitochondrial function has been reported in both type 2 diabetic patients and first-degree relatives of type 2 diabetic patients. The nature of this reduction is unknown. Here, we tested the hypothesis that a lower intrinsic mitochondrial respiratory capacity may underlie lower in vivo mitochondrial function observed in diabetic patients

    Mechanism of selective benzene hydroxylation catalyzed by iron-containing zeolites

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    A direct, catalytic conversion of benzene to phenol would have wide-reaching economic impacts. Fe zeolites exhibit a remarkable combination of high activity and selectivity in this conversion, leading to their past implementation at the pilot plant level. There were, however, issues related to catalyst deactivation for this process. Mechanistic insight could resolve these issues, and also provide a blueprint for achieving high performance in selective oxidation catalysis. Recently, we demonstrated that the active site of selective hydrocarbon oxidation in Fe zeolites, named α-O, is an unusually reactive Fe(IV)=O species. Here, we apply advanced spectroscopic techniques to determine that the reaction of this Fe(IV)=O intermediate with benzene in fact regenerates the reduced Fe(II) active site, enabling catalytic turnover. At the same time, a small fraction of Fe(III)-phenolate poisoned active sites form, defining a mechanism for catalyst deactivation. Density-functional theory calculations provide further insight into the experimentally defined mechanism. The extreme reactivity of α-O significantly tunes down (eliminates) the rate-limiting barrier for aromatic hydroxylation, leading to a diffusion-limited reaction coordinate. This favors hydroxylation of the rapidly diffusing benzene substrate over the slowly diffusing (but more reactive) oxygenated product, thereby enhancing selectivity. This defines a mechanism to simultaneously attain high activity (conversion) and selectivity, enabling the efficient oxidative upgrading of inert hydrocarbon substrates

    β-delayed fission and α decay of At196

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    A nuclear-decay spectroscopy study of the neutron-deficient isotope At196 is reported where an isotopically pure beam was produced using the selective Resonance Ionization Laser Ion Source and On-Line Isotope Mass Separator (CERN). The fine-structure α decay of At196 allowed the low-energy excited states in the daughter nucleus Bi192 to be investigated. A β-delayed fission study of At196 was also performed. A mixture of symmetric and asymmetric fission-fragment mass distributions of the daughter isotope Po196 (populated by β decay of At196) was deduced based on the measured fission-fragment energies. A βDF probability PβDF(At196)=9(1)×10−5 was determined

    Laser-assisted decay spectroscopy and mass spectrometry of 178Au^178Au

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    A comprehensive study of the isotope 178Au has been made at the CERN-ISOLDE facility, using resonance laser ionization. Two long-lived states in 178Au were identified—a low-spin ground state and a high-spin isomer—each of which were produced as pure beams. Using the ISOLTRAP precision Penning trap, the excitation energy of the isomeric state in 178Au was determined to be E∗=189(14)keV. The α-decay fine structure patterns of the two states were studied using the Windmill decay station, providing information on the low-lying states in the daughter nucleus 174Ir. Nuclear spin assignments of I(178Aug)=(2,3) and I(178Aum)=(7,8) are made based on the observed β-decay feeding and hyperfine structure intensity patterns. These spin assignments are used for fitting the hyperfine structures of the two states from which values for the magnetic dipole moments are extracted. The extracted moments are compared with calculations using additivity relations to establish the most probable configurations for 178Aug,m
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