Mercaptoamine-assisted Post-encapsulation of Metal Nanoparticles within Preformed Zeolites and their Analogues for Hydroisomerization and Methane Decomposition
- Authors
- Song, Minseok; Eom, Eunji; Shin, Jae Won; Cho, Hae Sung; Kim, Jeong-Chul; Jo, Changbum
- Issue Date
- May-2023
- Publisher
- John Wiley & Sons Ltd.
- Keywords
- Encapsulation; Metal Nanoparticles; Supported Metal; Zeolite Analogues; Zeolites
- Citation
- Angewandte Chemie International Edition, v.62, no.27
- Journal Title
- Angewandte Chemie International Edition
- Volume
- 62
- Number
- 27
- URI
- https://scholarworks.bwise.kr/cau/handle/2019.sw.cau/69999
- DOI
- 10.1002/anie.202303503
- ISSN
- 1433-7851
1521-3773
- Abstract
- We report a general synthetic strategy for post-encapsulation of metal nanoparticles within preformed zeolites using post-synthetic modification. Both anionic and cationic precursors to metal nanoparticle are supported on 8- and 10-membered ring zeolites and analogues during wet impregnation using 2-aminoethanethiol (AET) as a bi-grafting agent. Thiol groups are coordinated to metal centers, whereas amine moieties are dynamically attached to micropore walls via acid-base interactions. The dynamic acid-base interactions cause the even distribution of the metal-AET complex throughout the zeolite matrix. These processes encapsulate Au, Rh, and Ni precursors within the CHA, *MRE, MFI zeolite, and SAPO-34 zeolite analogues, for which small channel apertures preclude the post-synthesis impregnation of metal precursors. Sequential activation forms small and uniform nanoparticles (1–2.5 nm in diameter), as confirmed through electron microscopy and X-ray absorption spectroscopy. Containment within the small micropores protected the nanoparticles against harsh thermal sintering conditions and prevented the fouling of the metal surface by coke, thus resulting in a high catalytic performance in n-dodecane hydroisomerization and methane decomposition. The remarkable specificity of the thiol to metal precursors and the dynamic acid-base interaction make these protocols extendable to various metal-zeolite systems, suitable for shape-selective catalysts in challenging chemical environments. © 2023 Wiley-VCH GmbH.
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