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1.
J Am Chem Soc ; 142(45): 19209-19216, 2020 11 11.
Artigo em Inglês | MEDLINE | ID: mdl-33124818

RESUMO

Tuning the performance of nanoparticle (NP) catalysts by controlling the NP surface strain has evolved as an important strategy to optimize NP catalysis in many energy conversion reactions. Here, we present our new study on using an eigenforce model to predict and experiments to verify the strain-induced catalysis enhancement of the oxygen reduction reaction (ORR) in the presence of L10-CoMPt NPs (M = Mn, Fe, Ni, Cu, Ni). The eigenforce model allowed us to predict anisotropic (that is, two-dimensional) strain levels on distorted Pt(111) surfaces. Experimentally, by preparing a series of 5 nm L10-CoMPt NPs, we could push the ORR catalytic activity of these NPs toward the optimum region of the theoretical two-dimensional volcano plot predicted for L10-CoMPt. The best ORR catalyst in the alloy NP series we studied is L10-CoNiPt, which has a mass activity of 3.1 A/mgPt and a specific activity of 9.3 mA/cm2 at room temperature with only 15.9% loss of mass activity after 30 000 cycles at 60 °C in 0.1 M HClO4.


Assuntos
Nanopartículas Metálicas/química , Oxigênio/química , Ligas/química , Catálise , Teoria da Densidade Funcional , Oxirredução
2.
Nat Commun ; 13(1): 2166, 2022 04 20.
Artigo em Inglês | MEDLINE | ID: mdl-35443755

RESUMO

Photothermal sensing is crucial for the creation of smart wearable devices. However, the discovery of luminescent materials with suitable dual-wavelength emissions is a great challenge for the construction of stable wearable optical fibre temperature sensors. Benefiting from the Mn2+-Mn2+ superexchange interactions, a dual-wavelength (530/650 nm)-emitting material Li2ZnSiO4:Mn2+ is presented via simple increasing the Mn2+ concentration, wherein the two emission bands have different temperature-dependent emission behaviours, but exhibit quite similar excitation spectra. Density functional theory calculations, coupled with extended X-ray absorption fine structure and electron-diffraction analyses reveal the origins of the two emission bands in this material. A wearable optical temperature sensor is fabricated by incorporating Li2ZnSiO4:Mn2+ in stretchable elastomer-based optical fibres, which can provide thermal-sensitive emissions at dual- wavelengths for stable ratiometric temperature sensing with good precision and repeatability. More importantly, a wearable mask integrated with this stretchable fibre sensor is demonstrated for the detection of physiological thermal changes, showing great potential for use as a wearable health monitor. This study also provides a framework for creating transition-metal-activated luminescence materials.


Assuntos
Fibras Ópticas , Dispositivos Eletrônicos Vestíveis , Elastômeros , Monitorização Fisiológica , Temperatura
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