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 (Lead / Corresponding author), Ian S. Metcalfe (Lead / Corresponding author)

Research output: Contribution to journalArticle

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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 languageEnglish
Pages (from-to)1855
Number of pages1
JournalNature Communications
Volume8
Issue number1
DOIs
Publication statusPublished - 30 Nov 2017

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Nanoparticles
Oxides
Demonstrations
Chemical activation
activation
Metal Nanoparticles
chemistry
nanoparticles
oxides
Metal nanoparticles
energy conversion
energy storage
Platinum
Catalysis
Energy conversion
metals
Energy storage
preserving
catalysis
platinum

Keywords

  • Catalyst synthesis
  • Heterogeneous catalysis
  • Nanoparticles

Cite this

Neagu, Dragos ; Papaioannou, Evangelos I. ; Ramli, Wan K. W. ; Miller, David N. ; Murdoch, Billy J. ; Ménard, Hervé ; Umar, Ahmed ; Barlow, Anders J. ; Cumpson, Peter J. ; Irvine, John T. S. ; Metcalfe, Ian S. / Demonstration of chemistry at a point through restructuring and catalytic activation at anchored nanoparticles. In: Nature Communications. 2017 ; Vol. 8, No. 1. pp. 1855.
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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.",
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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). We thank the National EPSRC XPS Users’ Service, an EPSRC Mid-Range Facility and Sasol St Andrews for XPS data acquisition.",
year = "2017",
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Neagu, D, Papaioannou, EI, Ramli, WKW, Miller, DN, Murdoch, BJ, Ménard, H, Umar, A, Barlow, AJ, Cumpson, PJ, Irvine, JTS & Metcalfe, IS 2017, 'Demonstration of chemistry at a point through restructuring and catalytic activation at anchored nanoparticles', Nature Communications, vol. 8, no. 1, pp. 1855. https://doi.org/10.1038/s41467-017-01880-y

Demonstration of chemistry at a point through restructuring and catalytic activation at anchored nanoparticles. / Neagu, Dragos; Papaioannou, Evangelos I.; Ramli, Wan K. W.; Miller, David N.; Murdoch, Billy J.; Ménard, Hervé; Umar, Ahmed; Barlow, Anders J.; Cumpson, Peter J.; Irvine, John T. S. (Lead / Corresponding author); Metcalfe, Ian S. (Lead / Corresponding author).

In: Nature Communications, Vol. 8, No. 1, 30.11.2017, p. 1855.

Research output: Contribution to journalArticle

TY - JOUR

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). We thank the National EPSRC XPS Users’ Service, an EPSRC Mid-Range Facility and Sasol St Andrews for XPS data acquisition.

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.

KW - Catalyst synthesis

KW - Heterogeneous catalysis

KW - Nanoparticles

U2 - 10.1038/s41467-017-01880-y

DO - 10.1038/s41467-017-01880-y

M3 - Article

VL - 8

SP - 1855

JO - Nature Communications

JF - Nature Communications

SN - 2041-1723

IS - 1

ER -