Demonstration of chemistry at a point through restructuring and catalytic activation at anchored nanoparticles

Dragos Neagu; Evangelos I. Papaioannou; Wan K. W. Ramli; David N. Miller; Billy J. Murdoch; Hervé Ménard; Ahmed Umar; Anders J. Barlow; Peter J. Cumpson; John T. S. Irvine; Ian S. Metcalfe

doi:10.1038/s41467-017-01880-y

Demonstration of chemistry at a point through restructuring and catalytic activation at anchored nanoparticles

Dragos Neagu, Evangelos I. Papaioannou, Wan K. W. Ramli, David N. Miller, Billy J. Murdoch, Hervé Ménard, Ahmed Umar, Anders J. Barlow, Peter J. Cumpson, John T. S. Irvine, Ian S. Metcalfe

Research output: Contribution to journal › Article › peer-review

Abstract

Metal nanoparticles prepared by exsolution at the surface of perovskite oxides have been recently shown to enable new dimensions in catalysis and energy conversion and storage technologies owing to their socketed, well-anchored structure. Here we show that contrary to general belief, exsolved particles do not necessarily re-dissolve back into the underlying perovskite upon oxidation. Instead, they may remain pinned to their initial locations, allowing one to subject them to further chemical transformations to alter their composition, structure and functionality dramatically, while preserving their initial spatial arrangement. We refer to this concept as chemistry at a point and illustrate it by tracking individual nanoparticles throughout various chemical transformations. We demonstrate its remarkable practical utility by preparing a nanostructured earth abundant metal catalyst which rivals platinum on a weight basis over hundreds of hours of operation. Our concept enables the design of compositionally diverse confined oxide particles with superior stability and catalytic reactivity.

Original language	English
Article number	1855
Number of pages	8
Journal	Nature Communications
Volume	8
DOIs	https://doi.org/10.1038/s41467-017-01880-y
Publication status	Published - 30 Nov 2017

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Neagu, D., Papaioannou, E. I., Ramli, W. K. W., Miller, D. N., Murdoch, B. J., Ménard, H., Umar, A., Barlow, A. J., Cumpson, P. J., Irvine, J. T. S., & Metcalfe, I. S. (2017). Demonstration of chemistry at a point through restructuring and catalytic activation at anchored nanoparticles. Nature Communications, 8, Article 1855. https://doi.org/10.1038/s41467-017-01880-y

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title = "Demonstration of chemistry at a point through restructuring and catalytic activation at anchored nanoparticles",

abstract = "Metal nanoparticles prepared by exsolution at the surface of perovskite oxides have been recently shown to enable new dimensions in catalysis and energy conversion and storage technologies owing to their socketed, well-anchored structure. Here we show that contrary to general belief, exsolved particles do not necessarily re-dissolve back into the underlying perovskite upon oxidation. Instead, they may remain pinned to their initial locations, allowing one to subject them to further chemical transformations to alter their composition, structure and functionality dramatically, while preserving their initial spatial arrangement. We refer to this concept as chemistry at a point and illustrate it by tracking individual nanoparticles throughout various chemical transformations. We demonstrate its remarkable practical utility by preparing a nanostructured earth abundant metal catalyst which rivals platinum on a weight basis over hundreds of hours of operation. Our concept enables the design of compositionally diverse confined oxide particles with superior stability and catalytic reactivity.",

author = "Dragos Neagu and Papaioannou, {Evangelos I.} and Ramli, {Wan K. W.} and Miller, {David N.} and Murdoch, {Billy J.} and Herv{\'e} M{\'e}nard and Ahmed Umar and Barlow, {Anders J.} and Cumpson, {Peter J.} and Irvine, {John T. S.} and Metcalfe, {Ian S.}",

note = "The research leading to these results has received funding from the European Research Council under the European Union's Seventh Framework Programme (FP/2007-2013) / ERC Grant Agreement Number 320725 and from the EPSRC via the research grants EP/J016454/1, EP/G01244X/1, EP/K015540/1, EP/J018414/1, as well as EPSRC Capital for Great Technologies grants EP/L017008/1 and EP/K022679/1, and a Royal Society Wolfson Merit Award (WRMA 2012/R2).",

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doi = "10.1038/s41467-017-01880-y",

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T1 - Demonstration of chemistry at a point through restructuring and catalytic activation at anchored nanoparticles

AU - Neagu, Dragos

AU - Papaioannou, Evangelos I.

AU - Ramli, Wan K. W.

AU - Miller, David N.

AU - Murdoch, Billy J.

AU - Ménard, Hervé

AU - Umar, Ahmed

AU - Barlow, Anders J.

AU - Cumpson, Peter J.

AU - Irvine, John T. S.

AU - Metcalfe, Ian S.

N1 - The research leading to these results has received funding from the European Research Council under the European Union's Seventh Framework Programme (FP/2007-2013) / ERC Grant Agreement Number 320725 and from the EPSRC via the research grants EP/J016454/1, EP/G01244X/1, EP/K015540/1, EP/J018414/1, as well as EPSRC Capital for Great Technologies grants EP/L017008/1 and EP/K022679/1, and a Royal Society Wolfson Merit Award (WRMA 2012/R2).

PY - 2017/11/30

Y1 - 2017/11/30

N2 - Metal nanoparticles prepared by exsolution at the surface of perovskite oxides have been recently shown to enable new dimensions in catalysis and energy conversion and storage technologies owing to their socketed, well-anchored structure. Here we show that contrary to general belief, exsolved particles do not necessarily re-dissolve back into the underlying perovskite upon oxidation. Instead, they may remain pinned to their initial locations, allowing one to subject them to further chemical transformations to alter their composition, structure and functionality dramatically, while preserving their initial spatial arrangement. We refer to this concept as chemistry at a point and illustrate it by tracking individual nanoparticles throughout various chemical transformations. We demonstrate its remarkable practical utility by preparing a nanostructured earth abundant metal catalyst which rivals platinum on a weight basis over hundreds of hours of operation. Our concept enables the design of compositionally diverse confined oxide particles with superior stability and catalytic reactivity.

AB - Metal nanoparticles prepared by exsolution at the surface of perovskite oxides have been recently shown to enable new dimensions in catalysis and energy conversion and storage technologies owing to their socketed, well-anchored structure. Here we show that contrary to general belief, exsolved particles do not necessarily re-dissolve back into the underlying perovskite upon oxidation. Instead, they may remain pinned to their initial locations, allowing one to subject them to further chemical transformations to alter their composition, structure and functionality dramatically, while preserving their initial spatial arrangement. We refer to this concept as chemistry at a point and illustrate it by tracking individual nanoparticles throughout various chemical transformations. We demonstrate its remarkable practical utility by preparing a nanostructured earth abundant metal catalyst which rivals platinum on a weight basis over hundreds of hours of operation. Our concept enables the design of compositionally diverse confined oxide particles with superior stability and catalytic reactivity.

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U2 - 10.1038/s41467-017-01880-y

DO - 10.1038/s41467-017-01880-y

M3 - Article

SN - 2041-1723

VL - 8

JO - Nature Communications

JF - Nature Communications

M1 - 1855

ER -

Demonstration of chemistry at a point through restructuring and catalytic activation at anchored nanoparticles

Abstract

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