4.8 Article

Highly efficient and enhanced sulfur resistance supported bimetallic single-atom palladium-cobalt catalysts for benzene oxidation

期刊

APPLIED CATALYSIS B-ENVIRONMENTAL
卷 285, 期 -, 页码 -

出版社

ELSEVIER
DOI: 10.1016/j.apcatb.2020.119844

关键词

Bimetallic single-atom catalyst; Sulfur resistance; Volatile organic compound; Benzene oxidation; Reaction mechanism

资金

  1. National Natural Science Foundation of China [21677004, 21877006, 21976009]
  2. National Natural Science Committee of China-Liaoning Provincial People's Government Joint Fund [U1908204]
  3. Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions [IDHT20190503]
  4. Development Program for the Youth Outstanding-Notch Talent of Beijing Municipal Commission of Education [CITTCD201904019]

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A novel Pd/Co single-atom catalyst (Pd1Co1/Al2O3) was prepared for benzene oxidation by the research team, achieving a benzene conversion of 90% at 250 degrees Celsius. The catalyst exhibited enhanced sulfur resistance performance and good regeneration ability of the active sites.
Catalytic oxidation is one of the effective pathways for completely eliminating volatile organic compounds (VOCs) emitted from industrial and transportation activities. Meanwhile, single-atom catalysts have excellent application prospects in numerous reactions due to their high metal atomic utilization efficiency. In this work, we adopted a novel strategy to prepare an active Pd/Co single-atom catalyst (i.e., Pd1Co1/Al2O3) for benzene oxidation. The successful formation of the atomically dispersed palladium and cobalt species on Al2O3 was verified by the aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure. By the in situ temperature-programmed techniques and in situ diffuse reflectance Fourier transform infrared spectroscopy, we observed a double effect of the palladium and cobalt oxide active sites, resulting in an enhanced performance for benzene oxidation. A benzene conversion of 90 % was achieved over the Pd1Co1/Al2O3 catalyst at 250 degrees C and a space velocity of 40,000 mL/(g h). Interestingly, the catalyst also possessed enhanced sulfur resistance performance. The good regeneration ability of the active sites in the catalyst was due to the single-atom dispersion of Pd and Co. In addition, we deduce that benzene oxidation might occur over Pd1Co1/Al2O3 via a pathway of benzene -> cyclohexadiene -> phenol -> quinone -> maleate -> acetate -> CO2 and H2O. We believe that the obtained results can provide a useful idea for rationally designing the double active site single-atom catalysts and understanding the mechanism of VOCs oxidation.

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