Til hovedinnhold

Mechanistic Comparison of the Dealumination in SSZ-13 and the Desilication in SAPO-34

Mechanistic Comparison of the Dealumination in SSZ-13 and the Desilication in SAPO-34

Kategori
Vitenskapelig artikkel
Sammendrag
With the purpose of understanding the behavior of aluminosilicate zeolites and silicoaluminophosphates (SAPOs) in the presence of steam, we carried out a computational density functional theory (DFT) study on the desilication of SAPO-34. The mechanism studied was a stepwise hydrolysis of the four bonds to the Si heteroatom. An analogous process to the desilication of SAPO-34 is the dealumination of SSZ-13. To investigate possible mechanistic differences between the two processes, we compared the results of this study with the results of a previous study on dealumination in SSZ-13. We found that the intermediates along the dealumination path of SSZ-13 have one of the protons bonded to a bridging oxygen atom. In the corresponding intermediates of the desilication path in SAPO-34, the same proton prefers to be part of an aqua ligand coordinated to an Al atom. The principal factor determining the different proton locations is the electronic requirement of the atoms surrounding the proton. The different proton locations in SSZ-13 and SAPO-34 put clear conditions on possible mechanisms, thus causing them to be different for the two materials. We expect the principles determining the proton location also to be valid for other mechanisms of dealumination in SSZ-13 and desilication in SAPO-34.
Oppdragsgiver
  • Notur/NorStore / nn4683k
  • Notur/NorStore / NN4683K
Språk
Engelsk
Forfatter(e)
Institusjon(er)
  • Universitetet i Oslo
  • SINTEF Industri / Materialer og nanoteknologi
År
Publisert i
Journal of Physical Chemistry C
ISSN
1932-7447
Forlag
American Chemical Society (ACS)
Årgang
117
Hefte nr.
26
Side(r)
13442 - 13451