<p>Zeolite molecular sieve catalysts are extensively used in areas of petrochemical and environmental catalysis, <i>etc</i>. In addition to the unique channel system, morphology and acidic properties, the Al distribution has an important influence on the targeted catalytic reactions. This study focuses on an exquisite case of LEV zeolites for ammonia selective catalytic reduction reaction (NH<sub>3</sub>-SCR)—from novel OSDA predictions to the experimental synthesis of LEV zeolites and the mapping of atomic conformational properties, <i>e.g.</i>, Al distributions, to the catalytic properties of NH<sub>3</sub>-SCR. Employing <i>N,N</i>-dimethylmorpholine as the organic template for the synthesis of Cu-LEV-(OSDA1) catalysts, the <i>T</i><sub>90</sub> range spans from 220 °C to 550 °C, while that of hydrothermally aged samples ranges from 225 °C to 500 °C, aligning closely with the commercial Cu-SSZ-13. Under comparable physicochemical properties, catalysts biased towards the Al site at the T2 position within the LEV framework demonstrate heightened hydrothermal stability. Yet, in other NO<sub><i>x</i></sub> elimination reactions, such as CH<sub>3</sub>OH-SCR, the most optimal sites for reaction activity entail the T1-T2 Al pair (Al<sub>pair</sub>). These findings highlight that LEV zeolites with distinct Al atom conformation could be modulated by organic templates, thereby yielding refined catalysts for targeted reactions.</p>

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Organic template-based modulation of Al atom conformation in LEV zeolites to enhance NOx elimination

  • Yanhua Wang,
  • Yan Zhang,
  • Liehao Wei,
  • Xinying Liu,
  • Lijing Fang,
  • Caixia Liu,
  • Weichao Wang,
  • Qingling Liu

摘要

Zeolite molecular sieve catalysts are extensively used in areas of petrochemical and environmental catalysis, etc. In addition to the unique channel system, morphology and acidic properties, the Al distribution has an important influence on the targeted catalytic reactions. This study focuses on an exquisite case of LEV zeolites for ammonia selective catalytic reduction reaction (NH3-SCR)—from novel OSDA predictions to the experimental synthesis of LEV zeolites and the mapping of atomic conformational properties, e.g., Al distributions, to the catalytic properties of NH3-SCR. Employing N,N-dimethylmorpholine as the organic template for the synthesis of Cu-LEV-(OSDA1) catalysts, the T90 range spans from 220 °C to 550 °C, while that of hydrothermally aged samples ranges from 225 °C to 500 °C, aligning closely with the commercial Cu-SSZ-13. Under comparable physicochemical properties, catalysts biased towards the Al site at the T2 position within the LEV framework demonstrate heightened hydrothermal stability. Yet, in other NOx elimination reactions, such as CH3OH-SCR, the most optimal sites for reaction activity entail the T1-T2 Al pair (Alpair). These findings highlight that LEV zeolites with distinct Al atom conformation could be modulated by organic templates, thereby yielding refined catalysts for targeted reactions.