4.7 Article

A superior cerium-tungsten bimetal oxide catalyst with flower-like structure for selective catalytic reduction of NOx by NH3

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 435, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.134892

Keywords

Tungsten-cerium catalyst; NH3-SCR; Flower-like structure; Oxidizability; Reducibility

Funding

  1. National Natural Science Foundation of China [21876157]
  2. National Key Research and Development Program of China [2017YFC0210904, 2017YFC0210403, 2018YFC0214102]

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A flower-like 0.1%WO3/CeO2 catalyst was fabricated with high-efficiency for the selective reduction of NOx by NH3. The flower-like structure promoted a more uniform dispersion of tungsten species on the support and a stronger interaction between WO3 and CeO2, resulting in increased acid sites and surface vacancies. The catalyst exhibited significant SCR performance, with 90% NOx conversion and 95% N2 selectivity within a wide temperature range. The study provides a new strategy for developing high-efficiency ceria supported NH3-SCR catalyst.
A novel flower-like 0.1%WO3/CeO2(f) catalyst with high-efficiency was fabricated for the selective reduction of NOx by NH3. In contrast to traditional WO3/CeO2, this catalyst exhibited a significant SCR performance of 90% NOx conversion and 95% N2 selectivity within a wide temperature range of 175-450.C and great H2O and/or SO2 resistance under a high GHSV of 177,000 h 1. A variety of analytical techniques including SEM, XRD, XPS, NH3-TPD, H2-TPR and in situ DRIFTS-MS were employed for the catalysts characterization to fully understand the reaction mechanism over WO3/CeO2 catalysts. It was found that the flower-like structure promoted a more uniform dispersion of tungsten species on the support and a stronger interaction between WO3 and CeO2, thereby increasing the acid sites and surface vacancies. Moreover, more chemical active oxygen and trivalent cerium species were presented on 0.1% WO3/CeO2(f). In situ DRIFTS-MS and H2-TPR revealed that the reducibility was optimized for 0.1% WO3/CeO2(f). Then NH3 oxidation species could react with gaseous or adsorbed NOx during Eley-Rideal (E-R) pathway for 0.1%WO3/CeO2(f) at a high temperature (300. C). Meanwhile, NOx was reduced into more active bridged nitrates participating in the reaction via Langmuir-Hinshelwood (L-H) route, contributing to its superior deNOx performance. In comparison, the formation of inert adsorbed NH3 oxidization/ deformation species and bridged nitrates suppressed the SCR reaction over 0.1%WO3/CeO2, resulting in its inferior deNOx activity. This study not only provides a new strategy for developing high-efficiency ceria supported NH3-SCR catalyst, but also lays a foundation for investigating the reaction mechanism of cerium-based catalyst for further practical applications.

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