4.7 Article

Unveiling the role of high-valent copper cations in the selective catalytic reduction of NOx with NH3 at low temperature

Journal

FUEL
Volume 318, Issue -, Pages -

Publisher

ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2022.123607

Keywords

Cu3+ cation; NH3-SCR; Low temperature; In-situ DRIFTS

Funding

  1. National Natural Science Foundation of China [22002050]
  2. Postdoctoral Science Foundation of China [2020M683154]
  3. National Engineering Laboratory for Mobile Source Emission Control Technology [NELMS2020B01]
  4. Project of Jiangsu University Senior Talents Foundation [20JDG35]

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This study investigates the adsorption and activation of NOx and NH3 species in the NH3-SCR of NOx by Cu3+ cation. The results reveal that the LaCuO3-x/meso-Al2O3 catalyst with abundant Cu3+ species exhibits higher catalytic activity at low temperatures, which can be attributed to its unique properties of providing more acid sites and higher redox property.
Cu3+ cation is present in some particular materials, however, to the best of our knowledge, it remains unclear what role of Cu3+ plays during selective catalytic reduction of NOx by NH3 (NH3-SCR) to date yet. Herein, LaCuO3-x supported on mesoporous Al2O3 was designed and constructed via an incipient wetness method, and the effect of Cu3+ on the adsorption and activation of NOx and NH3 species in the NH3-SCR of NOx was systematically probed by experiment and in-situ DRIFTS for the first time. It unravels that LaCuO3-x/meso-Al2O3 with abundant Cu3+ species exhibits a remarkably higher catalytic activity for NH3-SCR of NOx at low temperature range (100 similar to 280 degrees C) than CuO/meso-Al2O3 counterpart because of the unique nature of Cu3+ species, which endows the more acid sites and higher redox property, thereby promoting the adsorption and activation of ammonia and NOx, and thereafter accelerating the intrinsic reaction rate of LaCuO3-x/meso-Al2O3. It should be the root reason resulting in the perceptibly higher catalytic activity of LaCuO3-x/meso-Al2O3 compared with that of CuO/meso-Al2O3 at low temperature. Therefore, the finding here offers great promise for the preparation of highly-efficient NH3-SCR catalyst with excellent catalytic activity at low temperatures in future.

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