Balancing Ge de-intercalation and Si re-insertion rates stabilizes hydrolytically labile germanosilicate zeolites

Abstract

Germanosilicate zeolites are attractive adsorbents and catalysts, thanks to their diverse structures and versatile textural properties. However, hydrolytic instability of such zeolites, even under ambient conditions, restricts their practical applications. In this study, we report dynamic changes in the state of the zeolite framework atoms due to Ge de-intercalation and Si re-insertion in aqueous medium and propose a strategy for stabilizing zeolites with planar and orthogonal locations of Ge-rich domains by managing both processes. Adjusting the acidity or temperature of the aqueous environment enabled Ge and Si atoms to reach balanced mobility, allowing Ge atoms to be leached and Si atoms to be inserted into the released positions, thereby stabilizing the zeolite framework. The developed approach offers a practical and controllable method for structural stabilization of any labile germanosilicate material, with potential applications in catalysis, as demonstrated after the incorporation of Al-associated acid centers.