Steering Interzeolite Conversion with Alkali Metal Cations: Lithium Maximizes Al Proximity in SSZ-13 Zeolite Genesis
Sven Robijns, Julien Devos, Thibaut Donckels, Rodrigo de Oliveira Silva, Niels De Witte, Dimitrios Sakellariou, Tom Van Assche, Michiel Dusselier
Abstract
Zeolites have long been regarded as difficult to modify during synthesis, as their synthesis is governed by kinetic processes. Recent breakthroughs have made it possible to exert a certain degree of control over zeolite properties with more performant materials as a result. Here, we investigate the effects alkali cations have on high-silica FAU-to-CHA interzeolite conversion (IZC) and on the resulting aluminum distributions. In this way, by using Li-cations in conjunction with an organic structure directing agent, the first route to a “fully paired” (divalent cation capacity, Co2+/Al = 0.48) high-silica SSZ-13 zeolite is demonstrated. Lithium shows great potential in steering IZC synthesis as it speeds up crystallization, and evidence was gathered in favor of a more elaborate mechanism of IZC in which dissolved Al-rich oligomers crash out of solution first and possibly spark nucleation. These findings help in gaining insights into a more general theory on zeolite nucleation in heterogeneous environments such as IZC. Furthermore, the “fully paired” sample has great potential for ion-exchanged zeolite catalysis or in adsorbents.