Kai Fan,Qinming Wu,Shuo Liu,Haiyu Kong,Sen Wang,Eduard Kunkes,Trees De Baerdemaeker,Andrei-Nicolae Parvulescu,Nils Bottke,Toshiyuki Yokoi,Dirk E. De Vos,Xiangju Meng,Weiping Zhang,Feng-Shou Xiao
Adjusting location and distribution of Al sites in the zeolite framework is critical for catalysis, and typical strategies include using zeolites as starting Al source. However, this approach is still challenging for aluminosilicate ITH zeolite. Herein, the distribution of Al species in the framework of ITH was efficiently regulated by implementing LTA zeolite as the aluminum source added in the starting gels (LTA-ITH). The obtained LTA-ITH zeolites have similar nanosheet morphology, textual parameters, and acidic properties to those of conventional ITH synthesized from boehmite (C-ITH), while the results of 27 Al MAS NMR spectra and 1-hexene cracking indicate that they have a different Al distribution. The use of LTA zeolite in starting gel is favorable for the formation of more Al species in sinusoidal and straight channels, compared with the C-ITH. Catalytic tests in the conversion of methanol to light olefin showed that LTA-ITH exhibited enhanced catalyst lifetime and propene selectivity compared with the C-ITH, which is reasonably attributed to the different locations of Al species in their respective ITH frameworks.
Despite very successful synthesis of many pure silica or germanosilicate zeolites, there are still challenges for direct synthesis of their aluminosilicate forms. As a typical example, it is easy to synthesize germanosilicate ITH, but difficult for direct synthesis of its aluminosilicate form. Recently, cationic oligomer has been successfully templated for direct formation of aluminosilicate ITH, but relatively complex steps for controlling molecular weight of the cationic oligomer strongly hinder the practical production of zeolite products. Herein, it is shown an alternative route for direct synthesis of aluminosilicate ITH zeolite in the presence of a small organic template with both structural directing ability for the ITH structure and strong interaction ability to aluminum species. Characterizations of the zeolite products with Si/Al ratios from 46 to 148 show high crystallinity, nanosheet-like crystal morphology, large microporous surface area (338 m 2 /g), high micropore volume (0.16 cm 3 /g), four-coordinated Al species, controllable acidic sites, and extraordinary hydrothermal stability (hydrothermal aging at 800 °C for 5 h with 10% water steaming). Catalytic tests in methanol-to-propylene (MTP) show that the aluminosilicate ITH zeolite has higher selectivity for propylene than that of commercial ZSM-5 zeolite with similar Si/Al ratio, which provides a candidate catalyst for MTP reaction in the near future.
危险品化学品经营许可证（带存储）