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CeO2/Al2O3 and Ce/BEA passive NOx adsorbers: Strong support effects on Ce speciation and NOx adsorption mechanisms
Xinyu Li1, Meiqing Shen2, Chunjuan Zhang1
1School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China.
Abstract:
This study investigates the NO adsorption mechanisms of two highly dispersed cerium-based passive NOx adsorbers (PNAs), Ce/BEA and CeO2/Al2O3, with identical Ce loadings. Combining PNA performance evaluations, in situ DRIFTS, UV Raman, and DFT calculations, we reveal distinct pathways dictated by the cerium speciation and support. On Ce/BEA, isolated [Ce4+O22-]2+ species activate NO in two pathways, oxidize NO to NO2 and surface bidentate nitrate, processes strongly inhibited by H2O. Conversely, on CeO2/Al2O3, H2O promotes NO activation by forming surface Ce-OH groups, which react with NO to form an HONO intermediate that transforms into nitrite on the alumina support. The divergent cerium dispersion and support properties yield fundamentally different H2O effects-inhibition versus promotion-governing their overall PNA performance.
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