Dynamic restructuring of supported metal nanoparticles and its implications for structure insensitive catalysis

Some fundamental concepts of catalysis are not fully explained but are of paramount importance for the development of improved catalysts. An example is the concept of structure insensitive reactions, where surface-normalized activity does not change with catalyst metal particle size. Here we explore...

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Vydáno v:Nature communications Ročník 12; číslo 1; s. 7096 - 10
Hlavní autoři: Vogt, Charlotte, Meirer, Florian, Monai, Matteo, Groeneveld, Esther, Ferri, Davide, van Santen, Rutger A., Nachtegaal, Maarten, Unocic, Raymond R., Frenkel, Anatoly I., Weckhuysen, Bert M.
Médium: Journal Article
Jazyk:angličtina
Vydáno: London Nature Publishing Group UK 07.12.2021
Nature Publishing Group
Nature Portfolio
Témata:
147/28
639/638/77/885
639/638/77/887
639/925/357/354
Absorption spectroscopy
Carbon dioxide
Catalysis
Catalysts
catalytic mechanisms
Diffusion rate
Ethene
Ethylene
heterogeneous catalysis
Humanities and Social Sciences
Hydrogenation
Metal particles
multidisciplinary
Nanoparticles
NANOSCIENCE AND NANOTECHNOLOGY
Nickel
Particle size
Science
Science (multidisciplinary)
Silica
Silicon dioxide
X ray absorption
X-ray absorption spectroscopy
ISSN:2041-1723, 2041-1723
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Shrnutí:Some fundamental concepts of catalysis are not fully explained but are of paramount importance for the development of improved catalysts. An example is the concept of structure insensitive reactions, where surface-normalized activity does not change with catalyst metal particle size. Here we explore this concept and its relation to surface reconstruction on a set of silica-supported Ni metal nanoparticles (mean particle sizes 1–6 nm) by spectroscopically discerning a structure sensitive (CO 2 hydrogenation) from a structure insensitive (ethene hydrogenation) reaction. Using state-of-the-art techniques, inter alia in-situ STEM, and quick-X-ray absorption spectroscopy with sub-second time resolution, we have observed particle-size-dependent effects like restructuring which increases with increasing particle size, and faster restructuring for larger particle sizes during ethene hydrogenation while for CO 2 no such restructuring effects were observed. Furthermore, a degree of restructuring is irreversible, and we also show that the rate of carbon diffusion on, and into nanoparticles increases with particle size. We finally show that these particle size-dependent effects induced by ethene hydrogenation, can make a structure sensitive reaction (CO 2 hydrogenation), structure insensitive. We thus postulate that structure insensitive reactions are actually apparently structure insensitive, which changes our fundamental understanding of the empirical observation of structure insensitivity. Structure insensitivity in catalysis has been empirically observed, but no satisfactory theoretical explanation could be given. By studying different nanoparticle sizes under dynamic catalytic conditions reaction-dependent particle size dependent restructuring was linked to the aforementioned.
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Dutch Research Council (NWO)
SC0022199
Niels Stensen Fellowship
BASF
USDOE Office of Science (SC), Basic Energy Sciences (BES)
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-021-27474-3