4.8 Article

Enhancing the Catalytic Activity of Palladium Nanoparticles via Sandwich-Like Confinement by Thin Titanate Nanosheets

期刊

ACS CATALYSIS
卷 11, 期 5, 页码 2754-2762

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c00031

关键词

layered titanate; palladium nanoparticles; CO oxidation; support-metal interaction; heterogeneous catalysis

资金

  1. Deutsche Forschungsgemeinschaft [SFB 840]
  2. Elite Network of Bavaria
  3. Keylab for Optical and Electron Microscopy of the Bavarian Polymer Institute (BPI)
  4. Fonds zur Forderung der wissenschaftlichen Forschung (FWF, Austrian Science Fund) [J4278]
  5. Austrian Science Fund (FWF) [J4278] Funding Source: Austrian Science Fund (FWF)

向作者/读者索取更多资源

In this study, researchers aimed to mimic the effect of atomically thin oxide layers on the electronic structure and catalytic activity of metals at a bulk scale by intercalating Pd nanoparticles into a nematic liquid crystalline phase. The resulting mesoporous architecture showed good accessibility to the Pd nanoparticles, leading to high catalytic activity in the oxidation of CO. The electron interaction between nanoparticles and nanosheets was observed, indicating a unique metal-support interaction that contributed to the catalyst's performance.
As atomically thin oxide layers deposited on flat (noble) metal surfaces have been proven to have a significant influence on the electronic structure and thus the catalytic activity of the metal, we sought to mimic this architecture at the bulk scale. This could be achieved by intercalating small positively charged Pd nanoparticles of size 3.8 nm into a nematic liquid crystalline phase of lepidocrocite-type layered titanate. Upon intercalation the galleries collapsed and Pd nanoparticles were captured in a sandwichlike mesoporous architecture showing good accessibility to Pd nanoparticles. On the basis of X-ray photoelectron spectroscopy (XPS) and CO diffuse reflectance Fourier transform infrared spectroscopy (DRIFTS) Pd was found to be in a partially oxidized state, while a reduced Ti species indicated an electronic interaction between nanoparticles and nanosheets. The close contact of titanate sandwiching Pd nanoparticles, moreover, allows for the donation of a lattice oxygen to the noble metal (inverse spillover). Due to the metal-support interactions of this peculiar support, the catalyst exhibited the oxidation of CO with a turnover frequency as high as 0.17 s(-1) at a temperature of 100 degrees C.

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