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A self-supporting bimetallic Au@Pt core-shell nanoparticle electrocatalyst for the synergistic enhancement of methanol oxidation.

ABSTRACT: The morphology of Pt-Au bimetal nanostructures plays an important role in enhancing the catalytic capability, catalytic stability and utilization efficiency of the platinum. We designed and successfully prepared Au@Pt nanoparticles (NPs) through an economical, surfactant-free and efficient method of seed-mediated growth. The Au@Pt NPs displayed electrochemical performances superior to those of commercial Pt/C catalysts because their agglomeration was prevented and exhibited better long-term stability with respect to methanol oxidation in acidic media by efficiently removing intermediates. Among the obtained Au@Pt NPs, Au₉₀@Pt₁₀ NPs exhibited the most significantly enhanced catalytic performance for the methanol oxidation reaction (MOR). Their mass and electrochemically active surface area (ECSA)-normalized current densities are approximately 3.9 and 4.6 times higher than those of commercial Pt/C catalysts, respectively. The oxidation current densities of the Au₉₀@Pt₁₀ NPs are approximately 1.8 times higher than those of commercial Pt/C catalysts after 4000 s of continuous measurement because the small Pt NPs grown on the surface of the Au₉₀@Pt₁₀ NPs were effectively stabilized by the Au metal support. This approach may be a facile method for the synthesis of self-supported bimetallic nanostructures, which is of great significance for the development of high performance electrocatalysts and sensors.

SUBMITTER: Tan C

PROVIDER: S-EPMC5524951 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Integration of plasmonic nanoantennas with catalytically active reactors in deliberately designed hybrid supra-nanostructures creates a dual-functional materials platform, based upon which precise modulation of catalytic reaction kinetics becomes accomplishable through optical excitations of plasmon resonances. Here, we have developed a multistep synthetic approach that enables us to assemble colloidal Au@C/Pt core@shell/satellite supra-nanostructures, in which the Au core functions as a light-harvesting plasmonic nanoantenna, the Pt satellites act as catalytically active reactors, and the C shell serves as a nanoscale dielectric spacer separating the reactors from the antenna, respectively. By adjusting several synthetic parameters, the size of the Au core, the thickness of the C shell, and the surface coverage of Pt satellites can all be tuned independently. Choosing Pt-catalyzed cascade oxidation of 3,3',5,5'-tetramethylbenzidine in an aerobic aqueous environment as a model reaction, we have systematically studied the detailed kinetic features of the catalytic reactions both in the dark and under visible light illumination over a broad range of reaction conditions, which sheds light on the interplay between plasmonic and catalytic effects in these antenna-reactor nanohybrids. The plasmonic antenna effect can be effectively harnessed to kinetically modulate multiple crucial steps during the cascade reactions, benefiting from plasmon-enhanced interband electronic transitions in the Pt satellites and plasmon-enhanced intramolecular electronic excitations in chromogenic intermediate species. In addition to the plasmonic antenna effect, photothermal transduction derived from plasmonic excitations can also provide significant contributions to the kinetic enhancements under visible light illumination. The knowledge gained from this work serves as important guiding principles for rational design and structural optimization of plasmonic antenna-reactor hybrid nanomaterials, endowing us with enhanced capabilities to kinetically modulate targeted catalytic/photocatalytic molecule-transforming processes through light illumination.

Project description:It is well-known that Ag-Au bimetallic nanoplates have attracted significant research interest due to their unique plasmonic properties and surface-enhanced Raman scattering (SERS). In recent years, there have been many studies on the fabrication of bimetallic nanostructures. However, controlling the shape, size, and structure of bimetallic nanostructures still has many challenges. In this work, we present the results of the synthesis of silver nanoplates (Ag NPls), and Ag-Au bimetallic core/shell and alloy nanostructures, using seed-mediated growth under green LED excitation and a gold salt (HAuCl4) as a precursor of gold. The results show that the optical properties and crystal structure strongly depend on the amount of added gold salt. Interestingly, when the amount of gold(x) in the sample was less than 0.6 μmol (x < 0.6 μmol), the structural nature of Ag-Au was core/shell, in contrast x > 0.6 μmol gave the alloy structure. The morphology of the obtained nanostructures was investigated using the field emission scanning electron microscopy (FESEM) technique. The UV-Vis extinction spectra of Ag-Au nanostructures showed localized surface plasmon resonance (LSPR) bands in the spectral range of 402-627 nm which changed from two peaks to one peak as the amount of gold increased. Ag-Au core/shell and alloy nanostructures were utilized as surface enhanced Raman scattering (SERS) substrates to detect methylene blue (MB) (10-7 M concentration). Our experimental observations indicated that the highest enhancement factor (EF) of about 1.2 × 107 was obtained with Ag-Au alloy. Our detailed investigations revealed that the Ag-Au alloy exhibited significant EF compared to pure metal Ag and Ag-Au core/shell nanostructures. Moreover, the analysis of the data revealed a linear dependence between the logarithm of concentration (log C) and the logarithm of SERS signal intensity (log I) in the range of 10-7-10-4 M with a correlation coefficient (R 2) of 0.994. This research helps us understand better the SERS mechanism and the application of Raman spectroscopy on a bimetallic surface.

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A self-supporting bimetallic Au@Pt core-shell nanoparticle electrocatalyst for the synergistic enhancement of methanol oxidation.

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