Article ID | Journal | Published Year | Pages | File Type |
---|---|---|---|---|
73981 | Microporous and Mesoporous Materials | 2012 | 9 Pages |
Two different procedures were used to prepare dealuminated BEA zeolite. The first procedure realized in two steps consisted of first calcination of original tetraethylammonium (TEA) BEA(17) zeolite in air at 823 K for 15 h to remove organic template and then treatment of as resulted organic-free HAlBEA(17) zeolite with concentrated nitric acid solution for different times to remove part or all Al atoms. Two periods was distinguished in the removal of Al atoms from HAlBEA(17) framework during the first procedure. During initial period (up to 0.08 h), the dealumination was very fast and 94% of Al was removed. This period corresponded to the easy removal of extra framework octahedral and framework tetrahedral aluminum from T3-T9 sites. In the second period (from 0.08 to 4 h), the dealumination was much slower. It corresponded to a much more difficult removal of framework tetrahedral aluminum from T1 and T2 sites. The second procedure realized in one step consisted of direct treatment of original TEABEA zeolite with concentrated nitric acid solution to remove simultaneously organic template and Al atoms. To obtain partly or totally dealuminated BEA zeolite the treatment time was 0.08 and 4 h respectively. The influence of the nitric acid treatment on Al removal, framework composition and acidity of BEA zeolite were investigated by XRD, FTIR and NMR. 2D 27Al 3Q MAS NMR allowed distinguishing two kinds of framework tetrahedral Al atoms (AlTd(2a) and AlTd(2b)) in BEA zeolite which relative amounts depended on the Si/Al ratio. The Brønsted and Lewis acidic centers were evidenced in dealuminated BEA zeolites by FTIR spectra of adsorbed pyridine and CO use as probe molecules. Their relative amounts depended on the degree of dealumination and procedure used for removal Al atoms.
Graphical abstractFigure optionsDownload full-size imageDownload as PowerPoint slideHighlights► Two different procedures were successfully applied to remove Al from BEA zeolite. ► Two steps procedure showed that Al is easily removal from T3-T9 sites of BEA zeolite. ► 2D27Al 3Q MAS NMR allowed to distinguish two kinds of framework tetrahedral Al. ► Relative amounts of these framework sites depend on the Si/Al ratio. ► One step procedure allowed removing simultaneously organic template and Al.