Journal
SCIENCE
Volume 344, Issue 6185, Pages 729-732Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1250984
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Funding
- NSF [CAREER-1151098, BRIGE-1032621, MRI-1040446]
- American Chemical Society [PRF 52422-DNI5]
- Welch Foundation [E-1794]
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1151098] Funding Source: National Science Foundation
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The growth mechanism of silicalite-1 (MFI zeolite) is juxtaposed between classical models that postulate silica molecules as primary growth units and nonclassical pathways based on the aggregation of metastable silica nanoparticle precursors. Although experimental evidence gathered over the past two decades suggests that precursor attachment is the dominant pathway, direct validation of this hypothesis and the relative roles of molecular and precursor species has remained elusive. We present an in situ study of silicalite-1 crystallization at characteristic synthesis conditions. Using time-resolved atomic force microscopy images, we observed silica precursor attachment to crystal surfaces, followed by concomitant structural rearrangement and three-dimensional growth by accretion of silica molecules. We confirm that silicalite-1 growth occurs via the addition of both silica molecules and precursors, bridging classical and nonclassical mechanisms.
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