4.8 Article

Overcoming Limitations in the Strong Interaction between Pt and Irreducible SiO2 Enables Efficient and Selective Hydrogenation of Anthracene

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 1, Pages 590-602

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c16965

Keywords

strong metal-support interactions; silicide; selective hydrogenation; anthracene; electrostatic adsorption

Funding

  1. National Key Research & Development Program of China [2016YFB0600305]
  2. National Natural Science Foundation of China [22038008, 22172016]
  3. Liaoning Revitalization Talent Program [XLYC1908033]
  4. Science and Technology Innovation Fund in Dalian City [2019J12GX028]
  5. Fundamental Research Funds for the Central Universities [DUT2021TB03, DUT21LK02]

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This study reports a significant enhancement of intermediate selectivity and stability in the hydrogenation of anthracene over an irreducible SiO2 supported Pt catalyst due to SMSI-induced formation of intermetallic Pt silicide and Pt-SiO2 interface. The isolated Pt active sites by Si atoms lead to a preferential transfer of activated H species to the outer ring of anthracene, resulting in a high yield of symmetric octahydroanthracene. Furthermore, the Pt2Si/SiO2 catalyst shows excellent stability and broadens the understanding of SMSI effect in irreducible oxide supported metal particle catalysts.
Interactions between metals and oxide supports are crucial in determining catalytic activity, selectivity, and stability. For reducible oxide supported noble metals, a strong metal-support interaction (SMSI) has been widely recognized. Herein we report the intermediate selectivity and stability over an irreducible SiO2 supported Pt catalyst in the hydrogenation of anthracene that are significantly boosted due to the SMSI-induced formation of intermetallic Pt silicide and Pt-SiO2 interface. The limitation in the strong interaction between Pt nanoparticles and irreducible SiO2 has been breached by combining the strong electrostatic adsorption method and following the high temperature reduction strategy. Due to the isolated Pt active sites by Si atoms, the activated H species produced over the Pt2Si/SiO2 catalyst with an initial catalytic activity of 2.49 mu mol/(m(2)/g)/h as well as TOF of 0.95 s(-1) preferentially transfer to the outer ring of anthracene to 87% yield of symmetric octahydroanthracene (sym-OHA) by subsequent hydrogenation. In addition, the Pt2Si/SiO2 catalyst presents an excellent stability after five cycles, which can be attributed to the fact that intermetallic Pt2Si nanoparticles are anchored firmly onto the surface of the SiO2 support. The discovery contributes to broaden the horizons on the SMSI effect in the irreducible oxide supported metal particle catalysts and provides guidance to design the metal-SiO2 interface and tune the surface chemical properties in diverse application conditions.

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