CaTiO 3 -supported Pt is sometimes referred to as an "Intelligent" catalyst because Pt can reversibly leave or enter the perovskite lattice following high-temperature reduction or oxidation; however, slow egress−ingress kinetics associated with large perovskite crystallites make these systems impractical. In the present work, thin films (∼1 nm) of CaTiO 3 were deposited onto MgAl 2 O 4 and then examined as catalyst supports for Pt and Pd. While Pd/ CaTiO 3 /MgAl 2 O 4 showed adsorption and CO-oxidation properties that were essentially the same as Pd/MgAl 2 O 4 , the Pt/CaTiO 3 /MgAl 2 O 4 catalyst exhibited evidence for strong support interactions. Pt/CaTiO 3 /MgAl 2 O 4 showed high activity for CO oxidation following reduction at 1073 K, even though CO adsorption was suppressed, but the catalysts were dramatically less active after oxidation at 1073 K and reduction at 773 K. Both Pt/CaTiO 3 /MgAl 2 O 4 and a catalyst formed by ex-solution of CaTi 0.95 Pt 0.05 O 3 exhibited very low rates for toluene hydrogenation in comparison to Pt/MgAl 2 O 4 . Scanning transmission electron microscopy (STEM) and energy-dispersive spectroscopy (EDS) showed that the CaTiO 3 films uniformly covered the MgAl 2 O 4 surface after both reduction and oxidation at 1073 K. Pt particles on reduced Pt/CaTiO 3 /MgAl 2 O 4 exhibited an unusual rhombohedral shape and may be flat, a further indication of strong interactions between the metal and the support. Low-energy ion scattering (LEIS) indicated that high-temperature reduction caused a restructuring of the CaTiO 3 . The implications of these results for understanding catalysts formed by ex-solution of metals from a perovskite lattice are discussed.
Unlike Co clusters, isolated Co atoms have been shown to be selective for catalytic dehydrogenation of ethane to ethylene; however, preparation of isolated Co sites requires special preparation procedures. Here, we demonstrate that Atomic Layer Deposition (ALD) of tris(2,2,6,6-tetramethyl-3,5-heptanedionato)cobalt(III) (Co(TMHD)3) on silica and other supports is effective in producing these isolated species. Silica-supported catalysts prepared with one ALD cycle showed ethylene selectivities greater than 96% at 923 K and were stable when CO2 was co-fed with the ethane. Co catalysts prepared by impregnation formed clusters that were significantly less active, selective, and stable. Rates and selectivities also decreased for catalysts with multiple ALD cycles. Isolated Co catalysts prepared on Al2O3 and MgAl2O4 showed reasonable selectivity for ethane dehydrogenation but were not as effective as their silica counterpart.
Thin, ~1-nm films of CaTiO3, SrTiO3, and BaTiO3 were deposited onto MgAl2O4 by Atomic Layer Deposition (ALD) and studied as catalyst supports for Rh. Scanning Transmission Electron Microcopy (STEM) and...
The dehydra-decyclization of tetrahydrofuran (THF) to butadiene was investigated over a series of metal oxide catalysts, where a common set of chemical pathways was identified. Alongside butadiene, propene is formed...
ObjectiveTo explore the structural brain abnormality and its relationship with neuropsychological disorders and electroclinical characteristics in juvenile myoclonic epilepsy (JME) patients.MethodsSixty-seven patients diagnosed with JME and 56 healthy controls were enrolled. All subjects underwent MRI using T1-weighted 3D brain structural images with 1 mm thickness. Voxel-based morphometry (VBM) and surface-based morphometry (SBM) analyses were performed. They also underwent a series of neuropsychological tests to assess cognitive function. The correlation analyses were conducted between structural changes, neuropsychological outcomes, and electroclinical features.ResultsThe gray matter concentration (GMC) was decreased in the bilateral pre-central and post-central gyrus, right anterior cingulate gyrus, left posterior orbital region, bilateral occipital regions, bilateral hippocampus and bilateral caudate nucleus in the JME groups (corrected P < 0.05). The evaluation of gray matter volume (GMV) showed significant decrease respectively in bilateral pre-central and post-central gyrus, left paracentral lobule, left orbital gyrus, left amygdala, left basal ganglia and left thalamus of JME patients (P < 0.05). The cortex thicknesses of the right inferior temporal gyrus, right insular gyrus, and right cingulate gyrus had negative correlations with the disease duration significantly. At the same time, the whole-brain white matter volume was positively associated with the course of the disease (P < 0.05). Patients with persistent abnormal EEG discharges had significantly less whole-brain gray matter volume than JME patients with normal EEG (P = 0.03). Correlation analyses and linear regression analyses showed that, in addition to the gray matter volumes of frontal and parietal lobe, the temporal lobe, as well as the basal ganglia and thalamus, were also significantly correlated with neuropsychological tests' results (P < 0.05).ConclusionThe JME patients showed subtle structural abnormalities in multiple brain regions that were not only limited to the frontal lobe but also included the thalamus, basal ganglia, parietal lobe, temporal lobe and some occipital cortex, with significant involvement of the primary somatosensory cortex and primary motor cortex. And we significantly demonstrated a correlation between structural abnormalities and cognitive impairment. In addition, the course of disease and abnormal discharges had a specific negative correlation with the structural changes.
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