4.8 Article

Pt Nanoparticles Embedded in Colloidal Crystal Template Derived 3D Ordered Macroporous Ce0.6Zr0.3Y0.1O2: Highly Efficient Catalysts for Methane Combustion

Journal

ACS CATALYSIS
Volume 5, Issue 3, Pages 1781-1793

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/cs501773h

Keywords

three-dimensionally ordered macropore; mesoporous wall; ceria-zirconia-yttria solid solution; supported Pt nanoparticle; methane combustion

Funding

  1. National Natural Science Fund of China [21221004, 21077007, 21377008]
  2. National High-Tech Research Development (863) Program of China [2013AA065304]
  3. Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions
  4. Scientific Research Base Construction-Science and Technology Creation Platform-National Materials Research Base Construction

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Three-dimensionally ordered macro/mesoporous Ce0.6Zr0.3Y0.1O2 (3DOM CZY) supported high-dispersion Pt nanoparticles (x wt % Pt/3DOM CZY, x = 0.6, 1.1, and 1.7) were successfully synthesized via the cetyltrimethylammonium bromide/triblock copolymer P123 assisted gas bubbling reduction route. The 3DOM CZY and x wt % Pt/3DOM CZY samples exhibited a high surface area of 84-94 m(2)/g. Pt nanoparticles (NPs) with a size of 2.6-4.2 nm were uniformly dispersed on the surface of 3DOM CZY. The 1.1 wt % Pt/3DOM CZY sample showed excellent catalytic performance, giving a T-90% value at 598 degrees C at gas hourly space velocity (GHSV) of 30000 mL/(g h) and the highest turnover frequency (TOFPt) of 6.98 X 10(-3) mol/(mol(Pt) s) at 400 degrees C for methane combustion. The apparent activation energy (64 kJ/mol) over 1.1 wt % Pt/3DOM CZY was much lower than that (95 kJ/mol) over Bulk CZY. The effects of water vapor and SO2 on the catalytic activity of 1.1 wt % Pt/3DOM CZY were also examined. It is concluded that the excellent catalytic activity of 1.1 wt % Pt/3DOM CZY was associated with its high oxygen adspecies concentration, good low-temperature reducibility, and strong interaction between Pt NPs and CZY as well as large surface area and unique nanovoid-walled 3DOM structure.

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