Abstract

The preparation of redox-active metal-organic framework (ra-MOF)-supported Pd nanoparticles (NPs) via the redox couple-driven method is reported, which can yield unprotected metallic NPs at room temperature within 10 min without the use of reducing agents. The Pd@ra-MOF has been exploited as a precursor of an active catalyst for CO oxidation. Under the CO oxidation reaction condition, Pd@ra-MOF is transformed into a PdOx-NiOy/C nanocomposite to generate catalytically active species in situ, and the resultant nanocatalyst shows sustainable activity through synergistic stabilization.

Highlights

  • Metal-organic frameworks (MOFs) constitute an important class of porous crystalline materials

  • We found that the Pd@redox-active metal-organic framework (ra-MOF) transformed into PdOx-NiOy/C nanocatalyst during gas phase CO oxidation reaction

  • The CO oxidation activities over Pd@ra-MOF were repeatedly tested, and the Pd@ra-MOF exhibited further lowered conversion temperatures in the second run, with T50 and T100 dropping down to 125°C and 150°C, respectively, revealing significantly enhanced CO oxidation activity as compared to the first run (Figure 3). This implied the formation of new species from the ra-MOF and Pd NPs during the first catalytic reaction

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Summary

Background

Metal-organic frameworks (MOFs) constitute an important class of porous crystalline materials. The incorporation of metal NPs into porous supports, such as zeolites, mesoporous materials, and MOF, can be achieved by various methods, including solution impregnation [11,12,13], chemical vapor deposition [14,15,16], and solid grinding [17] These methods have long been useful for generating heterogeneous catalysts, the high-temperature heating steps involved in these methods inevitably yield a wide distribution of particle sizes [18,19]. The redox potential-driven method can readily yield highly monodisperse, surface-naked metal NPs at room temperature without the help of any reducing agent or surface capping molecules, which would be advantageous for catalytic applications. The resulting metal oxide nanocomposite showed high and sustainable catalytic activity toward CO oxidation

Methods
Conclusions
28. Suh MP
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