Effect of defect-healing treatment on layered silicate precursors toward well-defined crosslinked frameworks

Abstract

The synthesis of zeolites from two-dimensional layered precursors through interlayer crosslinking of the layers is a promising avenue for realizing meticulously designed synthesis routes. However, the presence of defective silanol species in the precursors hinders the achievement of desirable synthesis outcomes. This study focuses on PREFER—a layered precursor for FER-type zeolites—which was synthesized and subjected to a liquid-mediated defect-healing treatment that we recently developed. The defect-healing process involves the use of fluoride compounds for reconstruction and organic pore fillers to stabilize the framework. The effects of the treatment on the structure, composition, and iron insertion behavior of PREFER were examined. Characterization results revealed a reduction in the number of intralayer silanol defects, whereas interlayer silanols were unaffected by the defect-healing treatment. Furthermore, the subsequent alterations observed in the crosslinking behavior with iron atoms indicated that the defect-healing treatment may enhance the insertion of iron species between the layers in more homogeneous environments compared with the untreated precursor. These findings provide valuable insights into the prospects of controlled interlayer linkage in two-dimensional zeolite materials.