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Role of Ce in promoting low-temperature performance and hydrothermal stability of Ce/Cu-SSZ-13 in the selective catalytic reduction of NOx with NH3

SEPARATION AND PURIFICATION TECHNOLOGY(2023)

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摘要
With the increase of car ownership, new challenges are posed to the treatment of mobile source exhaust gas, especially denitration (de-NOx). It is urgent to develop highly efficient de-NOx catalyst with a wide working temperature window. In this work, a series of Ce modified Cu-SSZ-13 molecular sieves (Ce/Cu-SSZ-13) are prepared by ion exchange method with different exchange times (x = 1, 2, 4, 8 h), and the role of Ce in pro-moting low-temperature de-NOx performance and hydrothermal stability of Ce/Cu-SSZ-13 in the selective cat-alytic reduction (SCR) of NOx are investigated. Both the low-temperature de-NOx performance and the hydrothermal stability of Cu-SSZ-13 are enhanced due to the modification of Ce, especially the Ce/Cu-SSZ-13 with an exchange time of 2 h. Both Ce/Cu-SSZ-13 and Cu-SSZ-13 present more than 95 % NOx conversion in the temperature region of 210-600 degrees C, and Ce modification significantly improves the NOx conversion in the low-temperature range (120-210 degrees C). It is revealed that the acidity, the surface Cu2+/Cu+ ratio and the NH3 adsorption amount on Cu-SSZ-13 increase after Ce ion exchange, and the active component Cu2+ migrates to the more stable six-membered ring due to the modification of Ce, all of which have promote the improvement of NH3-SCR de-NOx performance. Furthermore, in the process of hydrothermal aging, the presence of Ce protects the framework of Cu-SSZ-13, acidic sites and active component Cu2+, which greatly improves the hydrothermal stability of Cu-SSZ-13 molecular sieve. In addition, in-situ DRIFTS shows that the developed Ce/Cu-SSZ-13 fol-lows dual mechanisms of Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) to undergo NH3-SCR reaction. This work provides a new idea for improving the low-temperature de-NOx performance and hydrothermal stability of Cu-SSZ-13.
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关键词
Selective catalytic reduction,Cu-SSZ-13,De-NOx,Hydrothermal stability,Ion exchange
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