<p>Precise control over the acidic properties and pore architecture of zeolites is essential for the rational design of high-performance catalysts. Here, we demonstrate that simple post-synthetic treatment with ethanol solution can effectively reduce both strong and weak acid sites in silicoaluminophosphate (SAPO) zeolites. The hydroxyl groups in ethanol interact with terminal hydroxyls associated with Si islands and with bridging hydroxyls in Si–OH–Al species, leading to the elimination of these acid sites. Compared with the parent sample (S-P), the ethanol-treated sample (S-E3) retains only 34.4% of the strong acid sites and 29.0% of the weak acid sites. This approach is environmentally benign, straightforward, and cost-effective. Furthermore, treatment with mixed ethanol/amine solutions enables the simultaneous regulation of acidity and pore structure. With increasing ethanol concentration, the total number of acid sites initially decreases and then increases, while the total pore volume, including both micropore and mesopore volumes, generally decreases. The S-AE2 sample exhibits an optimal balance between acidity and pore volume. Compared with the S-P sample, its selectivity toward ethylene and propylene in the methanol to olefins (MTO) reaction increased by 6.92%, and its catalytic lifetime is extended by a factor of 2.33.</p>

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Green, Simple, and Economical Approaches for Regulating the Acidity and Pore Structure of Silicoaluminophosphate Zeolites

  • Yuhao Bai,
  • Jie Tao,
  • Meng Zhang

摘要

Precise control over the acidic properties and pore architecture of zeolites is essential for the rational design of high-performance catalysts. Here, we demonstrate that simple post-synthetic treatment with ethanol solution can effectively reduce both strong and weak acid sites in silicoaluminophosphate (SAPO) zeolites. The hydroxyl groups in ethanol interact with terminal hydroxyls associated with Si islands and with bridging hydroxyls in Si–OH–Al species, leading to the elimination of these acid sites. Compared with the parent sample (S-P), the ethanol-treated sample (S-E3) retains only 34.4% of the strong acid sites and 29.0% of the weak acid sites. This approach is environmentally benign, straightforward, and cost-effective. Furthermore, treatment with mixed ethanol/amine solutions enables the simultaneous regulation of acidity and pore structure. With increasing ethanol concentration, the total number of acid sites initially decreases and then increases, while the total pore volume, including both micropore and mesopore volumes, generally decreases. The S-AE2 sample exhibits an optimal balance between acidity and pore volume. Compared with the S-P sample, its selectivity toward ethylene and propylene in the methanol to olefins (MTO) reaction increased by 6.92%, and its catalytic lifetime is extended by a factor of 2.33.