4.8 Article

Steering the structure and reactivity of Ag/Al2O3 by the addition of multi-functional WOx for NOx reduction by ethanol

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APPLIED CATALYSIS B-ENVIRONMENTAL
卷 330, 期 -, 页码 -

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ELSEVIER
DOI: 10.1016/j.apcatb.2023.122527

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Tungstate; Ethanol-SCR; Lean NO x reduction; DFT calculation

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AgW/Al2O3 exhibits higher reactivity for ethanol SCR compared to Ag/Al2O3 throughout the entire reaction temperature range. STEM-EDS confirms the hierarchical structure of AgW/Al2O3 with highly dispersed W on Al2O3 and narrow size distribution of Ag species in contact with W. UV-vis, H2-TPR, and DRIFT results show that abundant metallic Ag in AgW/Al2O3 accelerates the activation of ethanol into acetaldehyde at low to medium temperatures, while ethylene formed over W-induced Bronsted acid sites contributes to high-temperature deNOx capacity. DFT calculations support the higher reactivity of AgW/Al2O3 towards acetaldehyde formation, with predominantly metallic Ag and Ag ionically bonded with WO3 predicted as the active phases.
Ag/Al2O3 has shown promising deNOx activity for (O)HC-SCR but has not yet been commercialized due to its narrow operating temperature range. Here, we developed AgW/Al2O3 exhibiting superior reactivity for ethanolSCR compared to Ag/Al2O3 in the entire reaction temperature range. STEM-EDS visibly confirmed the hierarchical structure of AgW/Al2O3 where W was highly dispersed over Al2O3, and Ag species in contact with W had a narrow size distribution. UV-vis, H2-TPR, and DRIFT results demonstrated that the abundant metallic Ag in AgW/Al2O3 accelerated the activation of ethanol into acetaldehyde, leading to improved NOx conversion at low to medium temperatures, while ethylene formed over W-induced Bronsted acid sites appeared to contribute to maintaining the high-temperature deNOx capacity. DFT calculations further supported that AgW/Al2O3 is more reactive toward acetaldehyde formation than Ag/Al2O3, and the corresponding active phases of AgW/Al2O3 were predicted to be predominantly metallic Ag along with Ag ionically bonded with WO3.

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