4.8 Article

High-Temperature Pretreatment Effect on Co/SiO2 Active Sites and Ethane Dehydrogenation

期刊

ACS CATALYSIS
卷 12, 期 19, 页码 11749-11760

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c03180

关键词

ethylene; Lewis acid; earth-abundant catalysts; shale gas; dehydrogenation

资金

  1. Department of Energy's Office of Energy Efficient and Renewable Energy's Advanced Manufacturing Office [DE-SC0012704]
  2. State of Delaware toward the RAPID projects
  3. DOE Office of Science [NNCI-2025608]
  4. NSF National Nanotechnology Coordinated Infrastructure Program [DE-SC0012335]
  5. Laboratory for Research on the Structure of Matter (MRSEC) by the National Science Foundation
  6. U.S. DOE, Office of Basic Energy Sciences [DMR-1720530]
  7. [DE-EE0007888-8.3]

向作者/读者索取更多资源

We report the synthesis, optimization, and characterization of Co/SiO2 catalyst for ethane nonoxidative dehydrogenation. High-temperature pretreatment enhances the initial activity of the catalyst, and highly dispersed Co(II) clusters are found to have higher activity than Co0 or CoOx nanoparticles. Additionally, high-temperature treatment increases the density of active acid sites.
We report the synthesis, optimization, and characterization of Co/ SiO2 for ethane nonoxidative dehydrogenation. Co/SiO2 is synthesized via strong electrostatic adsorption using the widely available Co(NO3)2 as the precursor. We demonstrate that high-temperature pretreatment (900 degrees C) in an inert atmosphere can significantly enhance the initial activity of the Co/SiO2 catalyst. X-ray absorption near-edge spectroscopy (XANES), temperature-programmed reduction (TPR), and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) suggest that highly dispersed Co(II) clusters are more active than Co0 or CoOx nanoparticles. Fourier transform infrared (FTIR) and isopropanol (IPA) temperature-programmed desorption and density func-tional theory (DFT) calculations suggest that high-temperature treatment significantly increases the density of active Lewis acid sites, possibly via surface dehydroxylation of the catalyst.

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