Double Perovskite LaFe(1-x)Ni(x)O(3) Coated with Sea Urchin-like Gold Nanoparticles Using Electrophoresis as the Photoelectrochemical Electrode to Enhance H(2) Production via Surface Plasmon Resonance Effect

利用电泳法将海胆状金纳米粒子包覆在双钙钛矿LaFe(1-x)Ni(x)O(3)上,作为光电化学电极,通过表面等离子体共振效应增强H(2)的生成。

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Abstract

The surface plasmon resonance (SPR) effect and the hetero-junction structure play crucial roles in enhancing the photocatalytic performances of catalysts for the water-splitting reaction. In this study, a series of double perovskites LaFe(1-x)N(ix)O(3) was synthesized. LaFe(1-x)N(ix)O(3) particles were then decorated with sea urchin-like Au nanoparticles (NPs) with the average size of approximately 109.83 ± 8.48 nm via electrophoresis. The d-spacing became narrow and the absorption spectra occurred the redshift phenomenon more when doping increasing Ni mole concentrations for the raw LaFe(1-x)N(ix)O(3) samples. From XPS analysis, the Ni atoms were inserted into the lattice of the matrix, resulting in the defect of the oxygen vacancy, and NiO and Fe(2)O(3) were formed. This hybrid structure was the ideal electrode for photoelectrochemical hydrogen production. The photonic extinction of the Au-coated LaFe(1-x)Ni(x)O(3) was less than 2.1 eV (narrow band gap), and the particles absorbed more light in the visible region. According to the Mott-Schottky plots, all the LaFe(1-x)N(ix)O(3) samples were the n-type semiconductors. Moreover, all the band gaps of the Au-coated LaFe(1-x)N(ix)O(3) samples were higher than 1.23 eV (H(+)/H(2)). Then, the hot electrons from the Au NPs were injected via the SPR effect, the coupling effect between LaFe(1-x)N(ix)O(3) and Au NPs, and the more active sites from Au NPs into the conduction band of the semiconductor, improving the hydrogen efficiency. The H(2) efficiency of the Au-coated LaFe(1-x)Ni(x)O(3) measured in ethanol was approximately ten times larger than the that of Au-coated LaFe(1-x)Ni(x)O(3) measured in 1-butanol at any testing temperature because ohmic and kinetic losses occurred in the latter solvent. Thus, the activation energies of ethanol at any testing temperature were smaller. The maximum real H(2) production was up to 43,800 μmol g(-1) h(-1) in ethanol. The redox reactions among metal ions, OH*, and oxides were consecutively proceeded under visible light illumination.

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