4.6 Article

Sulfate promotion of selective catalytic reduction of nitric oxide by ammonia on ceria

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CATALYSIS SCIENCE & TECHNOLOGY
卷 9, 期 8, 页码 1802-1815

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ROYAL SOC CHEMISTRY
DOI: 10.1039/c8cy02590h

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  1. U. S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences program [DE-SC0016367]
  2. IU Department of Chemistry
  3. IU Graduate School as part of the IU International Summer Research Program (IU-ISuRP)
  4. U.S. Department of Energy (DOE) [DE-SC0016367] Funding Source: U.S. Department of Energy (DOE)

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Selective catalytic reduction of nitric oxide by ammonia (NH3-SCR) is a promising technology for NOx emission control. In this work, the recently discovered sulfate promotion effect in this reaction was thoroughly investigated on ceria. Sulfates derived from different organic S precursors all exhibit a promotion effect. Mechanistic studies generate a reaction network including both Langmuir-Hinshelwood and Eley-Rideal mechanisms. Sulfates were shown to be versatile promoters with multiple functions: they tune the adsorption of reactants towards a more balanced intermediate coverage by creating strong Lewis acid sites, facilitate *NH2 formation, and suppress ammonia oxidation through surface oxygen deactivation. The comparison between sulfates and the classic inorganic promoter FeOx revealed that sulfates are more effective, especially at high temperature. This is mainly attributed to the high coverages of Eley-Rideal intermediates and low ammonia oxidation activity on sulfated ceria. This work provides fundamental understanding of the role of surface sulfates in NH3-SCR, which are essential under actual operation conditions. This understanding presents an exciting opportunity for future catalyst design with high durability and low cost.

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