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Au@Hg nanoalloy formation through direct amalgamation: Structural, spectroscopic, and computational evidence for slow nanoscale diffusion

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Au@Hg nanoalloy formation through direct amalgamation: Structural, spectroscopic, and computational evidence for slow nanoscale diffusion. / Mertens, S.F.L.; Gara, M.; Sologubenko, A.S. et al.
In: Advanced Functional Materials, Vol. 21, No. 17, 2011, p. 3259-3267.

Research output: Contribution to Journal/MagazineJournal articlepeer-review

Harvard

Mertens, SFL, Gara, M, Sologubenko, AS, Mayer, J, Szidat, S, Krämer, KW, Jacob, T, Schiffrin, DJ & Wandlowski, T 2011, 'Au@Hg nanoalloy formation through direct amalgamation: Structural, spectroscopic, and computational evidence for slow nanoscale diffusion', Advanced Functional Materials, vol. 21, no. 17, pp. 3259-3267. https://doi.org/10.1002/adfm.201100409

APA

Mertens, S. F. L., Gara, M., Sologubenko, A. S., Mayer, J., Szidat, S., Krämer, K. W., Jacob, T., Schiffrin, D. J., & Wandlowski, T. (2011). Au@Hg nanoalloy formation through direct amalgamation: Structural, spectroscopic, and computational evidence for slow nanoscale diffusion. Advanced Functional Materials, 21(17), 3259-3267. https://doi.org/10.1002/adfm.201100409

Vancouver

Mertens SFL, Gara M, Sologubenko AS, Mayer J, Szidat S, Krämer KW et al. Au@Hg nanoalloy formation through direct amalgamation: Structural, spectroscopic, and computational evidence for slow nanoscale diffusion. Advanced Functional Materials. 2011;21(17):3259-3267. doi: 10.1002/adfm.201100409

Author

Mertens, S.F.L. ; Gara, M. ; Sologubenko, A.S. et al. / Au@Hg nanoalloy formation through direct amalgamation: Structural, spectroscopic, and computational evidence for slow nanoscale diffusion. In: Advanced Functional Materials. 2011 ; Vol. 21, No. 17. pp. 3259-3267.

Bibtex

@article{8db5135264bf4adb9f53c639a53311aa,
title = "Au@Hg nanoalloy formation through direct amalgamation: Structural, spectroscopic, and computational evidence for slow nanoscale diffusion",
abstract = "Dynamic core-shell nanoparticles have received increasing attention in recent years. This paper presents a detailed study of Au-Hg nanoalloys, whose composing elements show a large difference in cohesive energy. A simple method to prepare Au@Hg particles with precise control over the composition up to 15 atom% mercury is introduced, based on reacting a citrate stabilized gold sol with elemental mercury. Transmission electron microscopy shows an increase of particle size with increasing mercury content and, together with X-ray powder diffraction, points towards the presence of a core-shell structure with a gold core surrounded by an Au-Hg solid solution layer. The amalgamation process is described by pseudo-zero-order reaction kinetics, which indicates slow dissolution of mercury in water as the rate determining step, followed by fast scavenging by nanoparticles in solution. Once adsorbed at the surface, slow diffusion of Hg into the particle lattice occurs, to a depth of ca. 3 nm, independent of Hg concentration. Discrete dipole approximation calculations relate the UV-vis spectra to the microscopic details of the nanoalloy structure. Segregation energies and metal distribution in the nanoalloys were modeled by density functional theory calculations. The results indicate slow metal interdiffusion at the nanoscale, which has important implications for synthetic methods aimed at core-shell particles. Interaction of an 11-nm gold hydrosol with metallic mercury leads to Au@Hg particles with up to 15 atom% Hg, following zero-order kinetics. The large difference in cohesive energy between the alloying elements causes slow inward diffusion of Hg over ca. 3 nm, decreasing the coherent face-centered cubic (fcc)-Au lattice length (indicated in red) as observed by X-ray diffraction. Copyright {\textcopyright} 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.",
keywords = "density functional theory, discrete dipole approximation, gold, mercury, nanoalloys, Amalgamation process, Cohesive energies, Core shell structure, Core-shell nanoparticles, Core-shell particle, Density functional theory calculations, Discrete dipole approximation, Discrete dipole approximation calculations, Elemental mercury, Face-centered cubic, Gold hydrosols, Hg concentrations, Inward diffusion, Lattice length, Mercury content, Metal distributions, Nano scale, Nano-alloys, Particle lattice, Precise control, Rate determining step, Segregation energies, SIMPLE method, Slow diffusion, Synthetic methods, UV-vis spectra, Zero order kinetics, Alloying elements, Density functional theory, Diffraction, Diffusion, Dissolution, Mercury (metal), Mercury compounds, Metals, Nanoparticles, Nanostructured materials, Nanotechnology, Reaction kinetics, Transmission electron microscopy, X ray diffraction, X ray powder diffraction, Gold",
author = "S.F.L. Mertens and M. Gara and A.S. Sologubenko and J. Mayer and S. Szidat and K.W. Kr{\"a}mer and T. Jacob and D.J. Schiffrin and T. Wandlowski",
note = "Cited By :23 Export Date: 17 April 2019 CODEN: AFMDC",
year = "2011",
doi = "10.1002/adfm.201100409",
language = "English",
volume = "21",
pages = "3259--3267",
journal = "Advanced Functional Materials",
issn = "1616-301X",
publisher = "John Wiley & Sons, Ltd",
number = "17",

}

RIS

TY - JOUR

T1 - Au@Hg nanoalloy formation through direct amalgamation: Structural, spectroscopic, and computational evidence for slow nanoscale diffusion

AU - Mertens, S.F.L.

AU - Gara, M.

AU - Sologubenko, A.S.

AU - Mayer, J.

AU - Szidat, S.

AU - Krämer, K.W.

AU - Jacob, T.

AU - Schiffrin, D.J.

AU - Wandlowski, T.

N1 - Cited By :23 Export Date: 17 April 2019 CODEN: AFMDC

PY - 2011

Y1 - 2011

N2 - Dynamic core-shell nanoparticles have received increasing attention in recent years. This paper presents a detailed study of Au-Hg nanoalloys, whose composing elements show a large difference in cohesive energy. A simple method to prepare Au@Hg particles with precise control over the composition up to 15 atom% mercury is introduced, based on reacting a citrate stabilized gold sol with elemental mercury. Transmission electron microscopy shows an increase of particle size with increasing mercury content and, together with X-ray powder diffraction, points towards the presence of a core-shell structure with a gold core surrounded by an Au-Hg solid solution layer. The amalgamation process is described by pseudo-zero-order reaction kinetics, which indicates slow dissolution of mercury in water as the rate determining step, followed by fast scavenging by nanoparticles in solution. Once adsorbed at the surface, slow diffusion of Hg into the particle lattice occurs, to a depth of ca. 3 nm, independent of Hg concentration. Discrete dipole approximation calculations relate the UV-vis spectra to the microscopic details of the nanoalloy structure. Segregation energies and metal distribution in the nanoalloys were modeled by density functional theory calculations. The results indicate slow metal interdiffusion at the nanoscale, which has important implications for synthetic methods aimed at core-shell particles. Interaction of an 11-nm gold hydrosol with metallic mercury leads to Au@Hg particles with up to 15 atom% Hg, following zero-order kinetics. The large difference in cohesive energy between the alloying elements causes slow inward diffusion of Hg over ca. 3 nm, decreasing the coherent face-centered cubic (fcc)-Au lattice length (indicated in red) as observed by X-ray diffraction. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

AB - Dynamic core-shell nanoparticles have received increasing attention in recent years. This paper presents a detailed study of Au-Hg nanoalloys, whose composing elements show a large difference in cohesive energy. A simple method to prepare Au@Hg particles with precise control over the composition up to 15 atom% mercury is introduced, based on reacting a citrate stabilized gold sol with elemental mercury. Transmission electron microscopy shows an increase of particle size with increasing mercury content and, together with X-ray powder diffraction, points towards the presence of a core-shell structure with a gold core surrounded by an Au-Hg solid solution layer. The amalgamation process is described by pseudo-zero-order reaction kinetics, which indicates slow dissolution of mercury in water as the rate determining step, followed by fast scavenging by nanoparticles in solution. Once adsorbed at the surface, slow diffusion of Hg into the particle lattice occurs, to a depth of ca. 3 nm, independent of Hg concentration. Discrete dipole approximation calculations relate the UV-vis spectra to the microscopic details of the nanoalloy structure. Segregation energies and metal distribution in the nanoalloys were modeled by density functional theory calculations. The results indicate slow metal interdiffusion at the nanoscale, which has important implications for synthetic methods aimed at core-shell particles. Interaction of an 11-nm gold hydrosol with metallic mercury leads to Au@Hg particles with up to 15 atom% Hg, following zero-order kinetics. The large difference in cohesive energy between the alloying elements causes slow inward diffusion of Hg over ca. 3 nm, decreasing the coherent face-centered cubic (fcc)-Au lattice length (indicated in red) as observed by X-ray diffraction. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

KW - density functional theory

KW - discrete dipole approximation

KW - gold

KW - mercury

KW - nanoalloys

KW - Amalgamation process

KW - Cohesive energies

KW - Core shell structure

KW - Core-shell nanoparticles

KW - Core-shell particle

KW - Density functional theory calculations

KW - Discrete dipole approximation

KW - Discrete dipole approximation calculations

KW - Elemental mercury

KW - Face-centered cubic

KW - Gold hydrosols

KW - Hg concentrations

KW - Inward diffusion

KW - Lattice length

KW - Mercury content

KW - Metal distributions

KW - Nano scale

KW - Nano-alloys

KW - Particle lattice

KW - Precise control

KW - Rate determining step

KW - Segregation energies

KW - SIMPLE method

KW - Slow diffusion

KW - Synthetic methods

KW - UV-vis spectra

KW - Zero order kinetics

KW - Alloying elements

KW - Density functional theory

KW - Diffraction

KW - Diffusion

KW - Dissolution

KW - Mercury (metal)

KW - Mercury compounds

KW - Metals

KW - Nanoparticles

KW - Nanostructured materials

KW - Nanotechnology

KW - Reaction kinetics

KW - Transmission electron microscopy

KW - X ray diffraction

KW - X ray powder diffraction

KW - Gold

U2 - 10.1002/adfm.201100409

DO - 10.1002/adfm.201100409

M3 - Journal article

VL - 21

SP - 3259

EP - 3267

JO - Advanced Functional Materials

JF - Advanced Functional Materials

SN - 1616-301X

IS - 17

ER -