4.6 Article

Improving the ammonia synthesis activity of Ru/CeO2 through enhancement of the metal-support interaction

Journal

JOURNAL OF ENERGY CHEMISTRY
Volume 60, Issue -, Pages 403-409

Publisher

ELSEVIER
DOI: 10.1016/j.jechem.2021.01.031

Keywords

Ammonia synthesis; NaBH4 treatment; Metal-support interaction; Ru/CeO2

Funding

  1. National Science Foundation of China [21776047, 21825801, 21978051]
  2. Program for Qishan Scholar of Fuzhou University [XRC-18033]

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NaBH4 treatment enhances the metallic Ru content, proportion of Ce3+ ions, and amount of exposed Ru species in Ru/CeO2 catalysts, resulting in a weaker inhibition effect of hydrogen species on ammonia synthesis and higher ammonia synthesis rates.
The metal-support interactions induced by high-temperature hydrogen reduction have a strong influence on the catalytic performance of ceria-supported Ru catalysts. However, the appearance of the strong metal-support interaction leads to covering of the Ru species by Ce suboxides, which is detrimental to the ammonia synthesis reaction that requires metallic species as active sites. In the present work, the interaction between Ru and ceria in the Ru/CeO2 catalyst was induced by NaBH4 treatment. NaBH4 treatment enhanced the fraction of metallic Ru, proportion of Ce3+, content of exposed Ru species, and amount of surface oxygen species. As a result, a larger amount of hydrogen species would desorb by the H-2-formation pathway and the strength of hydrogen adsorption would be weaker, weakening the inhibition effect of the hydrogen species on ammonia synthesis. In addition, the strong electronic metal-support interaction aids in nitrogen dissociation. Consequently, Ru/CeO2 with NaBH4 treatment showed higher ammonia synthesis rates than that with only hydrogen reduction. (C) 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.

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