7,809 research outputs found
Plasmonic catalysis with designer nanoparticles
Catalysis is central to a more sustainable future and a circular economy. If the energy required to drive catalytic processes could be harvested directly from sunlight, the possibility of replacing contemporary processes based on terrestrial fuels by the conversion of light into chemical energy could become a step closer to reality. Plasmonic catalysis is currently at the forefront of photocatalysis, enabling one to overcome the limitations of "classical" wide bandgap semiconductors for solar-driven chemistry. Plasmonic catalysis enables the acceleration and control of a variety of molecular transformations due to the localized surface plasmon resonance (LSPR) excitation. Studies in this area have often focused on the fundamental understanding of plasmonic catalysis and the demonstration of plasmonic catalytic activities towards different reactions. In this feature article, we discuss recent contributions from our group in this field by employing plasmonic nanoparticles (NPs) with controllable features as model systems to gain insights into structure-performance relationships in plasmonic catalysis. We start by discussing the effect of size, shape, and composition in plasmonic NPs over their activities towards LSPR-mediated molecular transformations. Then, we focus on the effect of metal support interactions over activities, reaction selectivity, and reaction pathways. Next, we shift to the control over the structure in hollow NPs and nanorattles. Inspired by the findings from these model systems, we demonstrate a design-driven strategy for the development of plasmonic catalysts based on plasmonic-catalytic multicomponent NPs for two types of molecular transformations: the selective hydrogenation of phenylacetylene and the oxygen evolution reaction. Finally, future directions, challenges, and perspectives in the field of plasmonic catalysis with designer NPs are discussed. We believe that the examples and concepts presented herein may inspire work and progress in plasmonic catalysis encompassing the design of plasmonic multicomponent materials, new strategies to control reaction selectivity, and the unraveling of stability and reaction mechanisms.Peer reviewe
A mobile data acquisition system
A mobile data aquisition (MobiDAQ) was developed for the ATLAS central hadronic
calorimeter (TileCal). MobiDAQ has been designed in order to test the functionalities of the TileCal
front-end electronics and to acquire calibration data before the final back-end electronics were built
and tested. MobiDAQ was also used to record the first cosmic ray events acquired by an ATLAS
subdetector in the underground experimental area
Stochastic Modelling Approach to the Incubation Time of Prionic Diseases
Transmissible spongiform encephalopathies like the bovine spongiform
encephalopathy (BSE) and the Creutzfeldt-Jakob disease (CJD) in humans are
neurodegenerative diseases for which prions are the attributed pathogenic
agents. A widely accepted theory assumes that prion replication is due to a
direct interaction between the pathologic (PrPsc) form and the host encoded
(PrPc) conformation, in a kind of an autocatalytic process. Here we show that
the overall features of the incubation time of prion diseases are readily
obtained if the prion reaction is described by a simple mean-field model. An
analytical expression for the incubation time distribution then follows by
associating the rate constant to a stochastic variable log normally
distributed. The incubation time distribution is then also shown to be log
normal and fits the observed BSE data very well. The basic ideas of the
theoretical model are then incorporated in a cellular automata model. The
computer simulation results yield the correct BSE incubation time distribution
at low densities of the host encoded protein
The elastic constants of MgSiO3 perovskite at pressures and temperatures of the Earth's mantle
The temperature anomalies in the Earth's mantle associated with thermal
convection1 can be inferred from seismic tomography, provided that the elastic
properties of mantle minerals are known as a function of temperature at mantle
pressures. At present, however, such information is difficult to obtain
directly through laboratory experiments. We have therefore taken advantage of
recent advances in computer technology, and have performed finite-temperature
ab initio molecular dynamics simulations of the elastic properties of MgSiO3
perovskite, the major mineral of the lower mantle, at relevant thermodynamic
conditions. When combined with the results from tomographic images of the
mantle, our results indicate that the lower mantle is either significantly
anelastic or compositionally heterogeneous on large scales. We found the
temperature contrast between the coldest and hottest regions of the mantle, at
a given depth, to be about 800K at 1000 km, 1500K at 2000 km, and possibly over
2000K at the core-mantle boundary.Comment: Published in: Nature 411, 934-937 (2001
Improving physical activity behaviors, physical fitness, cardiometabolic and mental health in adolescents - ActTeens program : a protocol for a randomized controlled trial
This trial aims to investigate the effects of the ActTeens physical activity program, on adolescents' physical activity level, health-related fitness, cardiometabolic and mental health. The trial will aim to recruit ∼140 adolescents (aged 13-14 years). Participants will be randomized into either intervention or control groups. The intervention will be guided by social cognitive theory and self-determination theory and implemented over one school term (24- weeks). The ActTeens Program will include: (1) structured physical activity sessions delivered within physical education, including movement-based games and dynamic stretching warm-ups; resistance training skill development; high-intensity training workouts; and cooldowns; (2) self-monitoring plus goal setting for physical activity by pedometer-smart wearable; and (3) healthy lifestyle guidance (social support) by WhatsApp® messages about healthy eating and regular physical activity for the intervention and parents groups. Study outcomes will be assessed at baseline, 24-weeks from baseline, and 12-months from baseline. Physical activity (accelerometer) is the primary outcome. Secondary outcomes include muscular and cardiorespiratory fitness, cardiometabolic profile, and mental health. A process evaluation will be conducted (i.e., recruitment, retention, attendance, and program satisfaction). This project will have the potential to address many questions and debates regarding the implementation of physical activity interventions in low-and- middle-income countries
Spontaneously Hypertensive Rats (SHR) Are Resistant to a Reserpine-Induced Progressive Model of Parkinson's Disease: Differences in Motor Behavior, Tyrosine Hydroxylase and alpha-Synuclein Expression
Reserpine is an irreversible inhibitor of vesicular monoamine transporter-2 (VMAT2) used to study Parkinson's disease (PD) and screening for antiparkinsonian treatments in rodents. Recently, the repeated treatment with a low-dose of reserpine was proposed as a progressive model of PD. Rats under this treatment show progressive catalepsy behavior, oral movements and spontaneous motor activity decrement. In parallel, compared to Wistar rats, spontaneously hypertensive rats (SHR) are resistant to acute reserpine-induced oral dyskinesia. We aimed to assess whether SHR would present differential susceptibility to repeated reserpine-induced deficits in the progressive model of PD. Male Wistar and SHR rats were administered 15 subcutaneously (s.c.) injections of reserpine (0.1 mgkg) or vehicle, every other day and motor activity was assessed by the catalepsy, oral movements and open field tests. Only reserpine-treated Wistar rats presented increased latency to step down in the catalepsy test and impaired spontaneous activity in the open field. On the other hand, there was an increase in oral movements in both reserpine-treated strains, although with reduced magnitude and latency to instauration in SHR. After a 15-day withdrawn period, both strains recovered from motor impairment, but SHR animals expressed reduced latencies to reach control levels. Finally, we performed immunohistochemistry for tyrosine hydroxylase (TH) and a-synuclein (alpha-syn) 48 h after the last injection or 15 days after withdrawn. Reserpinetreated animals presented a reduction in TH and an increase in alpha-syn immunoreactivity in the substantia nigra and dorsal striatum (dSTR), which were both recovered after 15 days of withdraw. Furthermore, SHR rats were resistant to reserpine-induced TH decrement in the substantia nigra, and presented reduced immunoreactivity to a-syn inthe dSTR relative to Wistar rats, irrespective of treatment. This effect was accompanied by increase of malondaldhyde (MDA) in the striatum of reserpine-treated Wistar rats, while SHR presented reduced MDA in both control and reserpine conditions relative to Wistar strain. In conclusion, the current results show that SHR are resilient to motor and neurochemical impairments induced by the repeated low-dose reserpine protocol. These findings indicate that the neurochemical, molecular and genetic differences in the SHR strain are potential relevant targets to the study of susceptibility to PD.Conselho Nacional de Desenvolvimento Cientifico e Tecnologico (CNPq)Coordenacao de Aperfeicoamento de Pessoal de Nivel Superior (CAPES)Fundacao de Apoio a Pesquisa do Estado do Rio Grande do Norte (FAPERN)Pro-reitoria de Pesquisa da Universidade Federal do Rio Grande do Norte (PROPESQ/UFRN)Fundacao de Amparo a Pesquisa do Estado de Sao Paulo (FAPESP)Univ Fed Rio Grande do Norte, Dept Physiol, Memory Studies Lab, Natal, RN, BrazilUniv Fed Rio Grande do Norte, Brain Inst, Natal, RN, BrazilUniv Fed Sao Paulo, Dept Pharmacol, Behav Neurosci Lab, Sao Paulo, BrazilUniv Fed Sao Paulo, Dept Pharmacol, Sao Paulo, BrazilUniv Fed Rio Grande do Norte, Dept Physiol, Neurochem Studies Lab, Natal, RN, BrazilUniv Santa Catarina, Dept Cellular Biol Embryol & Genet, Lab Behav Genet, Florianopolis, SC, BrazilUniv Fed Sao Paulo, Dept Biosci, Santos, BrazilUniv Fed Sao Paulo, Dept Pharmacol, Behav Neurosci Lab, Sao Paulo, BrazilUniv Fed Sao Paulo, Dept Pharmacol, Sao Paulo, BrazilUniv Fed Sao Paulo, Dept Biosci, Santos, BrazilFAPESP: 2015/12308-5FAPESP: 2015/03354-3Web of Scienc
MnO2-Ir Nanowires: Combining Ultrasmall Nanoparticle Sizes, O-Vacancies, and Low Noble-Metal Loading with Improved Activities towards the Oxygen Reduction Reaction
"Although clean energy generation utilizing the Oxygen Reduction Reaction (ORR) can
be considered a promising strategy, this approach remains challenging by the dependence on high
loadings of noble metals, mainly Platinum (Pt). Therefore, efforts have been directed to develop
new and efficient electrocatalysts that could decrease the Pt content (e.g., by nanotechnology tools or
alloying) or replace them completely in these systems. The present investigation shows that high
catalytic activity can be reached towards the ORR by employing 1.8 ± 0.7 nm Ir nanoparticles (NPs)
deposited onto MnO2 nanowires surface under low Ir loadings (1.2 wt.%). Interestingly, we observed
that the MnO2
-Ir nanohybrid presented high catalytic activity for the ORR close to commercial
Pt/C (20.0 wt.% of Pt), indicating that it could obtain efficient performance using a simple synthetic
procedure. The MnO2
-Ir electrocatalyst also showed improved stability relative to commercial Pt/C,
in which only a slight activity loss was observed after 50 reaction cycles. Considering our findings,
the superior performance delivered by the MnO2
-Ir nanohybrid may be related to (i) the significant
concentration of reduced Mn3+ species, leading to increased concentration of oxygen vacancies at its
surface; (ii) the presence of strong metal-support interactions (SMSI), in which the electronic effect
between MnOx and Ir may enhance the ORR process; and (iii) the unique structure comprised by Ir
ultrasmall sizes at the nanowire surface that enable the exposure of high energy surface/facets, high
surface-to-volume ratios, and their uniform dispersion.
Kondo Effect of a Magnetic Ion Vibrating in a Harmonic Potential
To discuss Kondo effects of a magnetic ion vibrating in the sea of conduction
electrons, a generalized Anderson model is derived. The model includes a new
channel of hybridization associated with phonon emission or absorption. In the
simplest case of the localized electron orbital with the s-wave symmetry,
hybridization with p-waves becomes possible. Interesting interplay among the
conventional s-wave Kondo effect and the p-wave one and the Yu-Anderson type
Kondo effect is found and the ground state phase diagram is determined by using
the numerical renormalization group method. Two different types of stable fixed
points are identified and the two-channel Kondo fixed points are generically
realized on the boundary.Comment: 15 pages, 17 figures, J. Phys. Soc. Jpn. 80 (2011) No.6 to be
publishe
Charge-transfer metal-insulator transitions in the spin-one-half Falicov-Kimball model
The spin-one-half Falicov-Kimball model is solved exactly on an
infinite-coordination-number Bethe lattice in the thermodynamic limit. This
model is a paradigm for a charge-transfer metal-insulator transition where the
occupancy of localized and delocalized electronic orbitals rapidly changes at
the metal-insulator transition (rather than the character of the electronic
states changing from insulating to metallic as in a Mott-Hubbard transition).
The exact solution displays both continuous and discontinuous (first-order)
transitions.Comment: 22 pages including 4 figures(eps), RevTe
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