Affiliation:
1. Innovation Center for Chemical Science College of Chemistry Chemical Engineering and Materials Science Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215123 P. R. China
2. PetroChina Lanzhou Petrochemical Company Lanzhou 730060 P. R. China
3. School of Chemical Engineering and Technology Hebei University of Technology Tianjin 300401 P. R. China
Abstract
AbstractProlonging the lifetime of SAPO‐34 catalysts and enhancing their olefin selectivity in methanol‐to‐olefin (MTO) reactions are critical yet challenging objectives. Here, a series of hierarchical SAPO‐34 catalysts were synthesized using a straightforward recrystallization method. The incorporation of triethylamine into the recrystallization mother liquor facilitated the formation of mesopores, achieving a high solid yield of up to 90%. Notably, the addition of phosphoric acid and ammonium polyvinyl phosphate alcohol during the recrystallization process significantly enhanced the crystallinity and regularity of the hierarchical SAPO‐34 crystals, consequently increasing the mesopore size. Due to the substantially improved mass transfer efficiency and moderated acidity, the SP34‐0.14P‐0.06R catalysts exhibited a prolonged lifetime of 344 min and 80.3% selectivity for ethylene and propylene at a weight hourly space velocity (WHSV) of 2 h−1. This performance markedly surpasses that of the parent SP34 catalyst, which demonstrated a lifetime of 136 min and a selectivity of 78.0%. Remarkably, the SP34‐0.14P‐0.06R maintained a lifetime of 166 min even at a high WHSV of 10 h−1, which is more than 5‐fold greater than that of the original microporous SP34. This research offers valuable insights into the design and development of hierarchically porous zeolites with high yields, enhancing the efficiency of MTO reactions and other applications.