Beta zeolite (nominal Si/Al = 19) has been treated with HF/NH4F solutions under different HF concentration, temperature and reaction time. It has been found that the crystallinity of the resulting materials is > 80% for HF concentration up to 0.5 M, but it drops below this value for the most severe condition (HF = 1 M and 40 degrees C). The treatment dissolves selectively aluminum, in such a way that the Si/Al increases to 34 for the most attacked material. As a consequence of these treatments, the mesopore volume increases by up to 80% respect to the parent Beta for samples retaining high crystallinity, corresponding to newly created mesopores in the range of 5-20 nm. Detailed STEM-HAADF studies reveal that the chemical attack of the Beta crystals by the acidic fluoride solution progresses slowly along the crystals, leaving behind highly corroded and porous “sponge-like” crystals where the structure of the zeolite is nevertheless retained. Pyridine adsorption/desorption experiments show that a fraction of the extraframework Al present in the starting Beta is reinserted in framework sites, a process that would be mediated by aluminum-fluoride soluble species. As a consequence of this process, the Bronsted/Lewis ratio of the strong acid sites increases from 1 in the starting Beta to close to 3. The concentration of total and strong Bronsted acid sites associated to framework Al increases with the treatment. However, the activity of the samples in the isomerization/disproportionation of m-xylene is lower than that of the parent Beta zeolite, a result that could be due to the higher B/L ratio..
Privacy & Cookies Policy
Necessary cookies are absolutely essential for the website to function properly. This category only includes cookies that ensures basic functionalities and security features of the website. These cookies do not store any personal information.