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Differentiating the structure of PtNi octahedral nanoparticles through combined ADF-EDX simulations.

ABSTRACT: Advances in catalysis rely on the synthesis and characterisation of nanoparticles that have tailored structures and compositions. Although energy-dispersive X-ray (EDX) spectroscopy can be used to study local variations in the compositions of individual supported nanoparticles on the atomic-scale in the scanning transmission electron microscope, electron beam induced damage and contamination can preclude the use of long exposure times and tomographic approaches. Here, we perform simulations of EDX maps of seven different octahedral PtNi nanoparticles for a selection of crystallographic orientations and tilts, to evaluate which of them can be distinguished from elemental mapping performed in only one orientation.

SUBMITTER: MacArthur KE

PROVIDER: S-EPMC5820384 | biostudies-literature | 2018

REPOSITORIES: biostudies-literature

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Differentiating the structure of PtNi octahedral nanoparticles through combined ADF-EDX simulations.

MacArthur Katherine E KE Heggen Marc M Dunin-Borkowski Rafal E RE

Advanced structural and chemical imaging 20180220 1

Advances in catalysis rely on the synthesis and characterisation of nanoparticles that have tailored structures and compositions. Although energy-dispersive X-ray (EDX) spectroscopy can be used to study local variations in the compositions of individual supported nanoparticles on the atomic-scale in the scanning transmission electron microscope, electron beam induced damage and contamination can preclude the use of long exposure times and tomographic approaches. Here, we perform simulations of E ...[more]

PMID: 29497598

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Project description:Interactions of nanoparticles (NPs) with their environment may have a pronounced effect on their structure and shape as well as on their functionality in applications such as catalysis. It is therefore crucial to disentangle the particle-adsorbate and particle-support interaction effects on the particle shape, its local structure, atomic dynamics, and its possible anisotropies. In order to gain insight into the support effect, we carried out an X-ray absorption fine-structure spectroscopy (XAFS) investigation of adsorbate- and ligand-free size-selected Pt NPs deposited on two different supports in ultrahigh vacuum. Polarization-dependent XAFS measurements, neural network-based analysis of X-ray absorption near-edge structure data, and reverse Monte Carlo (RMC) simulations of extended X-ray absorption fine structure (EXAFS) were used to resolve the 3D shape of the NPs and details of their local structure. A synergetic combination of advanced in situ XAFS analysis with atomic force microscopy and scanning tunneling microscopy (STM) imaging provides uniquely detailed information about the particle-support interactions and the NP/support buried interface, not accessible to any experimental technique, when considered alone. In particular, our combined approach reveals differences in the structure of Pt NPs deposited on TiO2(110) and SiO2/Si(111). Pt NPs on SiO2 assume a spherical-like 3D shape and weakly interact with the support. In contrast, the effective shape of analogously synthesized Pt NPs on TiO2(110) after annealing at 600 °C is found to be a truncated octahedron with (100) top and interfacial facets that are encapsulated by the TiO2 support. Modeling disorder effects in these NPs using an RMC approach reveals differences in bond-length distributions for NPs on different supports and allows us to analyze their anisotropy, which may be crucial for the interpretation of support-dependent atomic dynamics and can have an impact on the understanding of the catalytic properties of these NPs.

Project description:Octahedral anatase particles (OAPs), prepared by ultrasonication-hydrothermal reaction (US-HT), were modified with 2 wt% of gold by photodeposition. Conditions of US-HT process such as durations of US and durations of HT were varied to obtain OAPs products different by physicochemical and morphological properties. Au/OAPs samples were characterized by X-ray diffraction (XRD), scanning transmission electron microscopy (STEM), X-ray photoelectron spectroscopy (XPS) and diffuse reflectance spectroscopy (DRS). The photocatalytic activity was tested under UV irradiation for decomposition of acetic acid (CO2 system) and dehydrogenation of methanol (H2 system) under aerobic and anaerobic conditions, respectively, and for oxidation of 2-propanol under visible light irradiation. Photodeposition of gold was very fast for all OAPs samples (0.5-10 min) under Ar atmosphere, and the clear correlation between the content of electron traps (ETs) and the induction period, during which nanoparticles (NPs) of gold are formed, indicates that ETs in titania samples are a key-factor for rapidity of gold photodeposition on titania surface. It was found that better morphology of titania (larger content of faceted particles) resulted in formation of larger gold NPs, while small gold NPs were deposited on structural defects. Modification of OAPs with gold NPs resulted in significant enhancement of photocatalytic activity, being e.g., 1.5 (CO2 system), 7.7 (H2 system), and even more than 40 under vis irradiation. It was found that both the properties of titania and gold are crucial for resultant photocatalytic activity, but a direct correlation between one structural/physical property and photocatalytic activity could not be obtained since all structural properties changed simultaneously when conditions of photocatalyst preparation (US-HT) were changed. Therefore, gold NPs of controlled sizes were deposited on OAPs product with the best morphology by modified photodeposition method. Clear correlation between photocatalytic activity under visible light and the size of gold NPs indicates that gold properties are decisive for visible light activity rather than titania properties. 3D-FDTD simulations confirm that an increase in the size of gold NPs results in extended surface areas with field enhancement.

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Differentiating the structure of PtNi octahedral nanoparticles through combined ADF-EDX simulations.

Publications

Differentiating the structure of PtNi octahedral nanoparticles through combined ADF-EDX simulations.

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