4.6 Article

Mechanism and Enhancement of the Low-Temperature Selective Catalytic Reduction of NOx with NH3 by Bifunctional Catalytic Mixtures

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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
卷 60, 期 18, 页码 6446-6454

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AMER CHEMICAL SOC
DOI: 10.1021/acs.iecr.0c05214

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  1. National Natural Science Foundation of China [51836006, U1609212]

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The study focused on enhancing the low-temperature performance of selective catalytic reduction (SCR) of NOx with NH3 by using a bifunctional catalytic system mixing V-W/Ti with an oxidative component, MnOx/CeO2. The results showed that a synergistic enhancement is significant when V-W/Ti and MnOx/CeO2 are in intimate contact, facilitating a bifunctional LT-SCR pathway mediated by a short-lived, mobile nitrite-precursor intermediate. This mechanism can effectively improve NH3 selectivity in SCR reactions.
Enhancement of the low-temperature (LT) performance of selective catalytic reduction (SCR) of NOx with NH3 has been a spotlight in environmental catalysis. Here, we use a bifunctional catalytic system mixing V-W/Ti with an oxidative component, i.e., MnOx/CeO2, to achieve both improved LT-SCR activity and N-2 selectivity. An integrated approach of steady-state kinetic measurements, chemical trapping techniques, time-resolved in situ FTIR spectroscopy, and density functional theory (DFT) calculations reveals that such a synergistic enhancement is at a short distance and is significant when V-W/Ti and MnOx/CeO2 are in intimate contact. These findings further suggest a bifunctional LT-SCR pathway mediated by a short-lived, mobile nitrite-precursor intermediate, which is facilely generated on the oxidative component and then communicates with the adjacent SCR phase through reacting with the abundant NH3 adsorbates there. Assembling such a mechanism with commercial SCR catalysts, accordingly, acts as a promising way to enhance the LT-SCR performance.

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