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1.
J Am Chem Soc ; 146(23): 16039-16051, 2024 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-38832517

RESUMO

Efficient methane photooxidation to formic acid (HCOOH) has emerged as a sustainable approach to simultaneously generate value-added chemicals and harness renewable energy. However, the persistent challenge lies in achieving a high yield and selectivity for HCOOH formation, primarily due to the complexities associated with modulating intermediate conversion and desorption after methane activation. In this study, we employ first-principles calculations as a comprehensive guiding tool and discover that by precisely controlling the O2 activation process on noble metal cocatalysts and the adsorption strength of carbon-containing intermediates on metal oxide supports, one can finely tune the selectivity of methane photooxidation products. Specifically, a bifunctional catalyst comprising Pd nanoparticles and monoclinic WO3 (Pd/WO3) would possess optimal O2 activation kinetics and an intermediate oxidation/desorption barrier, thereby promoting HCOOH formation. As evidenced by experiments, the Pd/WO3 catalyst achieves an exceptional HCOOH yield of 4.67 mmol gcat-1 h-1 with a high selectivity of 62% under full-spectrum light irradiation at room temperature using molecular O2. Notably, these results significantly outperform the state-of-the-art photocatalytic systems operated under identical condition.

2.
Magn Reson Imaging ; 34(8): 1064-70, 2016 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-27114344

RESUMO

Musculoskeletal MR imaging under multi-angle situations plays an increasingly important role in assessing joint and muscle tissues system. However, there are still limitations due to the closed structures of most conventional RF coils. In this study, a time-harmonic target-field method was employed to design open multi-purpose coil (OMC) for multi-angle musculoskeletal MR imaging. The phantom imaging results suggested that the proposed OMC could achieve homogeneously distributed magnetic field and high signal-to-noise ratio (SNR) of 239.04±0.83 in the region of interest (ROI). The maximum temperature in the heating hazard test was 16°C lower than the standard regulation, which indicated the security of the designed OMC. Furthermore, to demonstrate the effectiveness of the proposed OMC for musculoskeletal MR imaging, especially for multi-angle imaging, a healthy volunteer was examined for MR imaging of elbow, ankle and knee using OMC. The in vivo imaging results showed that the proposed OMC is effective for MR imaging of musculoskeletal tissues at different body parts, with satisfied B1 field homogeneity and SNR. Moreover, the open structure of the OMC could provide a large joint movement region. The proposed open multi-purpose coil is feasible for musculoskeletal MR imaging, and potentially, it is more suitable for the evaluation of musculoskeletal tissues under multi-angle conditions.


Assuntos
Articulação do Tornozelo/anatomia & histologia , Articulação do Cotovelo/anatomia & histologia , Articulação do Joelho/anatomia & histologia , Imageamento por Ressonância Magnética/métodos , Humanos , Imagens de Fantasmas , Ondas de Rádio , Valores de Referência , Razão Sinal-Ruído
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