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Confining Gold Nanoparticles in Preformed Zeolites by Post-Synthetic Modification Enhances Stability and Catalytic Reactivity and Selectivity

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Title
Confining Gold Nanoparticles in Preformed Zeolites by Post-Synthetic Modification Enhances Stability and Catalytic Reactivity and Selectivity
Author(s)
Eom, Eunji; Song, Minseok; Jeong-Chul Kim; Kwon, Dong-Il; Rainer, Daniel N.; Gołąbek, Kinga; Nam, Sung Chan; Ryoo, Ryong; Mazur, Michal; Jo, Changbum
Publication Date
2022-10
Journal
Journal of the American Chemical Society, v.2, no.10, pp.2327 - 2338
Publisher
American Chemical Society
Abstract
© 2022 American Chemical Society. All rights reserved.Confining Au nanoparticles (NPs) in a restricted space (e.g., zeolite micropores) is a promising way of overcoming their inherent thermal instability and susceptibility to aggregation, which limit catalytic applications. However, such approaches involve complex, multistep encapsulation processes. Here, we describe a successful strategy and its guiding principles for confining small (<2 nm) and monodisperse Au NPs within commercially available beta and MFI zeolites, which can oxidize CO at 40 °C and show size-selective catalysis. This protocol involves post-synthetic modification of the zeolite internal surface with thiol groups, which confines AuClx species inside microporous frameworks during the activation process whereby Au precursors are converted into Au nanoparticles. The resulting beta and MFI zeolites contain uniformly dispersed Au NPs throughout the void space, indicating that the intrinsic stability of the framework promotes resistance to sintering. By contrast, in situ scanning transmission electron microscopy (STEM) studies evidenced that Au precursors in bare zeolites migrate from the matrix to the external surface during activation, thereby forming large and poorly dispersed agglomerates. Furthermore, the resistance of confined Au NPs against sintering is likely relevant to the intrinsic stability of the framework, supported by extended X-ray absorption fine structure (EXAFS), H2 chemisorption, and CO Fourier transform infrared (FT-IR) studies. The Au NPs supported on commercial MFI maintain their uniform dispersity to a large extent after treatment at 700 °C that sinters Au clusters on mesoporous silicas or beta zeolites. Low-temperature CO oxidation and size-selective reactions highlight that most gold NPs are present inside the zeolite matrix with a diameter smaller than 2 nm. These findings illustrate how confinement favors small, uniquely stable, and monodisperse NPs, even for metals such as Au susceptible to cluster growth under conditions often required for catalytic use. Moreover, this strategy may be readily adapted to other zeolite frameworks that can be functionalized by thiol groups.
URI
https://pr.ibs.re.kr/handle/8788114/12691
DOI
10.1021/jacsau.2c00380
ISSN
0002-7863
Appears in Collections:
Center for Nanomaterials and Chemical Reactions(나노물질 및 화학반응 연구단) > 1. Journal Papers (저널논문)
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