4.8 Article

Intra-crystalline mesoporous zeolite encapsulation-derived thermally robust metal nanocatalyst in deep oxidation of light alkanes

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NATURE COMMUNICATIONS
卷 13, 期 1, 页码 -

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NATURE PORTFOLIO
DOI: 10.1038/s41467-021-27828-x

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资金

  1. National Natural Science Foundation of China [21976078, 21922606, 21876139, 21773016]
  2. National Key R&D Program of China [2016YFC0205900]
  3. Natural Science Foundation of Jiangxi Province [20202ACB213001]
  4. Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy
  5. Guangdong Provincial Key RD Program [2019B110206002]

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The study presents a facile strategy to design and synthesize palladium nanoparticles enveloped within a single-crystalline zeolite with intra-mesopores. The resulting material exhibits remarkable performances in light alkane deep oxidation reactions, attributed to the confinement and guarding effect of the zeolite shell and the improvement in mass-transfer efficiency and active metal sites accessibility.
Zeolite-confined metal nanoparticles (NPs) have attracted much attention owing to their superior sintering resistance and broad applications for thermal and environmental catalytic reactions. However, the pore size of the conventional zeolites is usually below 2 nm, and reactants are easily blocked to access the active sites. Herein, a facile in situ mesoporogen-free strategy is developed to design and synthesize palladium (Pd) NPs enveloped in a single-crystalline zeolite (silicalite-1, S-1) with intra-mesopores (termed Pd@IM-S-1). Pd@IM-S-1 exhibited remarkable light alkanes deep oxidation performances, and it should be attributed to the confinement and guarding effect of the zeolite shell and the improvement in mass-transfer efficiency and active metal sites accessibility. The Pd-PdO interfaces as a new active site can provide active oxygen species to the first C-H cleavage of light alkanes. This work exemplifies a promising strategy to design other high-performance intra-crystalline mesoporous zeolite-confined metal/metal oxide catalysts for high-temperature industrial thermal catalysis. Zeolite-confined metal nanoparticles (NPs) have attracted much attention owing to their superior sintering resistance and broad applications. Here the authors develop a facile in situ mesoporogen-free strategy to design and synthesize palladium NPs enveloped within a single-crystalline zeolite with intra-mesopores.

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