4.7 Article

The design of the highly active NH3-SCR catalyst Ce-W/UiO-66: Close coupling of active sites and acidic sites

Journal

SEPARATION AND PURIFICATION TECHNOLOGY
Volume 300, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.seppur.2022.121864

Keywords

NH3-SCR; UiO-66; Ce; W; Close coupling; Reaction mechanism

Funding

  1. National Natural Science Foundation of China [21876071, 52000093, 21667015]
  2. Yunnan Fundamental Research Projects [202101BE070001-001]

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Ce-based catalyst is an important catalyst for NH3-SCR reaction, with Ce3+ playing a crucial role. However, the specific atomic sites for Ce anchoring and the chemical mechanism of Ce3+ formation in CeO2 are not fully understood. This study reveals that UiO-66 has abundant hydroxyl groups on its surface, which serve as anchoring sites for Ce. Additionally, the introduction of highly dispersed acidic sites (WO3) around CeO2 enhances the catalytic activity and stability by tightly coupling the redox and acidic sites.
Ce based catalyst is one of the most important NH3-SCR catalysts. It has been widely recognized that Ce3+ plays a crucial role in NH3-SCR reaction. However, the specific atomic sites for anchoring Ce atoms and the chemical mechanism underlying the formation of Ce3+ in CeO2 are still incompletely known. Herein, we demonstrate that there are abundant hydroxyl groups on the surface of UiO-66, which are the anchoring sites of Ce. As the loading continues to increase, the insufficiently anchored Ce species will agglomerate and induce the formation of Ce3+- rich CeO2 clusters, which served as the redox sites in 10%Ce/UiO-66. On this basis, the strong interaction be-tween W and CeO(2 )was used to introduce highly dispersed acidic sites (WO3) around CeO2, and thus the redox site and the acidic site are tightly coupled. In situ DRIFTS results revealed that the NH3-SCR reaction pathway followed L-H mechanism on 10%Ce-10%W/UiO-66 catalyst, which is likely to be an important factor for the improved catalytic activity and stability.

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