posted on 2020-12-31, 20:08authored byYu Liang, Allan J. Jacobson, Jeffrey D. Rimer
Zeolite
crystallization often requires the presence of an organic
structure-directing agent (SDA) to facilitate the formation of nanoporous
cages and channels. Among the limited number of zeolites that can
be synthesized in organic-free media, alkali metals are most commonly
employed as inorganic SDAs. Many alkali metal zeolites are usually
prepared under moderate conditions using temperatures less than 100
°C and synthesis times on the order of hours. One notable exception
is zeolite chabazite (CHA), which is prepared from potassium ions
and requires atypically long crystallization times on the order of
weeks. Attaining practical synthesis times on the order of days necessitates
an alternative approach, such as the use of zeolite crystal seeds.
In this study, we show that growth solutions prepared via the partial
substitution of potassium with strontium generate purely-crystalline
chabazite within hours without the need for either organics or crystal
seeds. Studies of strontium inclusion in seed-assisted syntheses also
reveal shorter synthesis times. Notably, we show that strontium has
a pronounced impact on the kinetics of chabazite formation, leading
to 14- and 3-fold reductions in crystallization time compared with
pure potassium syntheses in the absence and presence of crystal seeds,
respectively. Using a combination of 29Si and 27Al MAS NMR spectroscopy, we also show that strontium functions as
a SDA based on its ability to alter Q4(nAl)29Si speciation, thereby redistributing tetrahedral Al sites in the
framework. Given the widespread application of chabazite in adsorption
and separation processes, designing facile and efficient synthesis
approaches with concomitant control of physicochemical properties
is commercially relevant.