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1.
Chem Commun (Camb) ; 57(60): 7382-7385, 2021 Jul 27.
Artigo em Inglês | MEDLINE | ID: mdl-34231575

RESUMO

The effect of platinum-supported nano-shaped ceria catalysts on methanol partial oxidation and methyl formate product selectivity has been investigated. A Pt-supported CeO2 nanocube catalyst had a higher turnover frequency than nanosphere catalysts; however, nanosphere catalysts showed higher selectivity towards methyl formate. The observed ceria shape effect in catalysis was associated with the shape-dependent Pt dispersion and its oxidation states. Furthermore, in situ studies revealed that the reduced platinum and mono-dentate methoxy group were responsible for the higher turnover frequency.

2.
ACS Appl Mater Interfaces ; 13(10): 11869-11878, 2021 Mar 17.
Artigo em Inglês | MEDLINE | ID: mdl-33660500

RESUMO

Solar thermal distillation is a promising way to harvest clean water due to its sustainability. However, the energy density of solar irradiation inevitably demands scalability of the systems. To realize practical applications, it is highly desirable to fabricate meter-scale solar evaporator panels with high capillary performance as well as optical absorptance using scalable and high-throughput fabrication methods. Here, we demonstrate a truly scalable fabrication process for a bi-facial solar evaporator with copper oxide dendrites via the hydrogen bubble templated electrochemical deposition technique. Furthermore, we construct a theoretical model combining capillarity and evaporative mass transfer, which leads to optimal operation conditions and wick characteristics, including superhydrophilicity, extreme capillary performance, and omni-angular high optical absorptance. The fabricated porous surfaces with excellent capillary performance and productivity provide a pathway toward a highly efficient bi-facial solar evaporator panel with meter-level scalability.

3.
PLoS One ; 15(4): e0230837, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-32271789

RESUMO

Interrogation elicits anxiety in individuals under scrutiny regardless of their innocence, and thus, anxious responses to interrogation should be differentiated from deceptive behavior in practical lie detection settings. Despite its importance, not many empirical studies have yet been done to separate the effects of interrogation from the acts of lying or guilt state. The present fMRI study attempted to identify neural substrates of anxious responses under interrogation in either innocent or guilt contexts by developing a modified "Doubt" game. Participants in the guilt condition showed higher brain activations in the right central-executive network and bilateral basal ganglia. Regardless of the person's innocence, we observed higher activation of the salience, theory of mind and sensory-motor networks-areas associated with anxiety-related responses in the interrogative condition, compared to the waived conditions. We further explored two different types of anxious responses under interrogation-true detection anxiety in the guilty (true positive) and false detection anxiety in the innocent (false positive). Differential neural responses across these two conditions were captured at the caudate, thalamus, ventral anterior cingulate and ventromedial prefrontal cortex. We conclude that anxiety is a common neural response to interrogation, regardless of an individual's innocence, and that there are detectable differences in neural responses for true positive and false positive anxious responses under interrogation. The results of our study highlight a need to isolate complex cognitive processes involved in the deceptive acts from the emotional and regulatory responses to interrogation in lie detection schemes.


Assuntos
Ansiedade , Encéfalo/diagnóstico por imagem , Culpa , Detecção de Mentiras/psicologia , Adulto , Análise de Variância , Ansiedade/psicologia , Encéfalo/fisiologia , Feminino , Giro do Cíngulo/diagnóstico por imagem , Giro do Cíngulo/fisiologia , Humanos , Aplicação da Lei , Imageamento por Ressonância Magnética , Masculino , Córtex Pré-Frontal/diagnóstico por imagem , Córtex Pré-Frontal/fisiologia
4.
J Chem Phys ; 151(23): 234716, 2019 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-31864251

RESUMO

Platinum-based heterogeneous catalysts are mostly used in various commercial chemical processes because of their high catalytic activity, influenced by the metal/oxide interaction. To design rational catalysts with high performance, it is crucial to understand the relationship between the metal-oxide interface and the reaction pathway. Here, we investigate the role of oxygen defect sites in the reaction mechanism for CO oxidation using Pt nanoparticles supported on mesoporous TiO2 catalysts with oxygen defects. We show an intrinsic correlation between the catalytic reactivity and the local properties of titania with oxygen defects (i.e., Ti3+ sites). In situ infrared spectroscopy observations of the Pt/mesoporous TiO2-x catalyst indicate that an oxygen molecule bond can be activated at the perimeter between the Pt and an oxygen vacancy in TiO2 by neighboring CO molecules on the Pt surface before CO oxidation begins. The proposed reaction pathways for O2 activation at the Pt/TiO2-x interface based on density functional theory confirm our experimental findings. We suggest that this provides valuable insight into the intrinsic origin of the metal/support interaction influenced by the presence of oxygen vacancies, which clarifies the pivotal role played by the support.

5.
Chem Commun (Camb) ; 55(64): 9503-9506, 2019 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-31328745

RESUMO

The strong metal-oxide interaction of platinum nanoparticles (PtNPs) deposited on two types of cobalt oxides, CoO and Co3O4, was investigated using CO oxidation. Two different sizes of PtNPs as well as arc-plasma-deposited (APD) PtNPs without a capping layer were used to reveal the effect of metal-oxide interfaces on catalytic activity. An enhanced catalytic activity was observed on the PtNPs on the Co3O4 substrate, which was ascribed to the reducible support and to the interfacial sites.

6.
Neuroimage ; 169: 485-495, 2018 04 01.
Artigo em Inglês | MEDLINE | ID: mdl-29284140

RESUMO

Although the relationship between resting-state functional connectivity and task-related activity has been addressed, the relationship between task and resting-state directed or effective connectivity - and its behavioral concomitants - remains elusive. We evaluated effective connectivity under an N-back working memory task in 24 participants using stochastic dynamic causal modelling (DCM) of 7 T fMRI data. We repeated the analysis using resting-state data, from the same subjects, to model connectivity among the same brain regions engaged by the N-back task. This allowed us to: (i) examine the relationship between intrinsic (task-independent) effective connectivity during resting (Arest) and task states (Atask), (ii) cluster phenotypes of task-related changes in effective connectivity (Btask) across participants, (iii) identify edges (Btask) showing high inter-individual effective connectivity differences and (iv) associate reaction times with the similarity between Btask and Arest in these edges. We found a strong correlation between Arest and Atask over subjects but a marked difference between Btask and Arest. We further observed a strong clustering of individuals in terms of Btask, which was not apparent in Arest. The task-related effective connectivity Btask varied highly in the edges from the parietal to the frontal lobes across individuals, so the three groups were clustered mainly by the effective connectivity within these networks. The similarity between Btask and Arest at the edges from the parietal to the frontal lobes was positively correlated with 2-back reaction times. This result implies that a greater change in context-sensitive coupling - from resting-state connectivity - is associated with faster reaction times. In summary, task-dependent connectivity endows resting-state connectivity with a context sensitivity, which predicts the speed of information processing during the N-back task.


Assuntos
Córtex Cerebral/fisiologia , Conectoma/métodos , Função Executiva/fisiologia , Processamento de Imagem Assistida por Computador/métodos , Memória de Curto Prazo/fisiologia , Modelos Teóricos , Rede Nervosa/fisiologia , Adulto , Córtex Cerebral/diagnóstico por imagem , Feminino , Humanos , Imageamento por Ressonância Magnética , Masculino , Rede Nervosa/diagnóstico por imagem , Adulto Jovem
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