4.7 Article

A comparison of Al-rich Cu-SSZ-13 zeolites synthesized by different methods in their Al distribution, hydrothermal stability and catalytic performance in the selective catalytic reduction of NOx with NH3

Journal

MICROPOROUS AND MESOPOROUS MATERIALS
Volume 313, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.micromeso.2020.110851

Keywords

Cu-SSZ-13 zeolite; Preparation method; Selective catalytic reduction; NOx elimination; Hydrothermal stability; Aluminum distribution

Funding

  1. National Natural Science Foundation of China [21991092, 21773281, 21802157, U1862101, U1510104]
  2. Dalian National Laboratory for Clean Energy [DNL 180206]
  3. Strategic Program of Coal-based Technology of Shanxi Province of China [MQ2014-11, MQ2014-10]
  4. Innovative Talent Program of Shanxi Province [201605D211001]
  5. Strategic Priority Research Program of the Chinese Academy of Sciences [XDA21020500]
  6. CAS/SAFEA International Partnership Program for Creative Research Teams

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Cu-SSZ-13 zeolite has attracted great interest due to its excellent performance in NH3-SCR, but the high cost in synthesizing SSZ-13 remains a challenge. Different preparation methods were investigated to synthesize Al-rich Cu-SSZ-13 with varying Al distribution and catalytic performance. The Cu-SZ-F zeolite prepared with fluoride assistance showed the highest catalytic activity and stability, indicating potential as a low-cost catalyst in NOx elimination.
Cu-SSZ-13 zeolite has attracted great interest owing to its extraordinary performance in the selective catalytic reduction of NOx with NH3 (NH3-SCR); however, the high expense in the costly templates for synthesizing SSZ-13 remains a serious obstacle for its application in large scale, which exacts alternative methods to get SSZ-13 of high performance in NH3-SCR at reduced cost. In this work, a series of methods, including the interzeolite conversion from X and Y zeolites (to get SZ-XC and SZ-YC, respectively) and the assistance with seed crystal and fluorine ion (to get SZ-S and SZ-F, respectively), were used to synthesize the Al-rich Cu-SSZ-13 zeolites; the influence of preparation method on the Al distribution, hydrothermal stability and catalytic performance of CuSSZ-13 in NH3-SCR was then comparatively investigated. The results indicate that the Cu-SSZ-13 zeolites prepared by various methods are also rather different in the content of paired Al and active Cu2+-2Al species, following the order of SZ-F > SZ-S > SZ-YC > SZ-XC; a positive correlation is observed between the catalytic activity in NH3-SCR and the content of alpha-Cu2+-2Al species determined by the electron spinning resonance. In particular, the Cu-SSZ-13 zeolite prepared by using fluoride as an assistant (Cu-SZ-F) has much higher fraction of paired Al and active alpha-Cu2+-2Al species and thereby exhibits better catalytic performance in NH3-SCR, with an NO conversion of nearly 80% at 200 degrees C under a gaseous hourly space velocity (GHSV) of 240,000 h(-1). Moreover, the Cu-SSZ-13 zeolite prepared by the fluoride assistance method also displays less silanol defects and greater hydrothermal stability, showing enormous potential as a practicable catalyst of low cost in the elimination of NOx by NH3-SCR.

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