4.8 Article

Time-resolved dissolution elucidates the mechanism of zeolite MFI crystallization

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SCIENCE ADVANCES
卷 7, 期 25, 页码 -

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AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.abg0454

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  1. Industrial Chair ANR-TOTAL NanoClean Energy [ANR-17-CHIN-0005-01]
  2. FEDER [18P01675]
  3. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0014468]
  4. Welch Foundation [E-1794]
  5. NSF [CBET-1626418]
  6. Office of the Vice-Chancellor of Research and Economic Development at the University of California at Riverside

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The study elucidated the growth mechanism of zeolite crystals through dissolution experiments and structural analysis, revealing the evolving mosaic structure within crystals during growth. Additionally, it showed that dissolution can be used as an effective ex situ technique to uncover details about crystal growth features inaccessible by other methods.
Zeolite crystal growth mechanisms are not fully elucidated owing to their complexity wherein the formation of a particular zeolite can occur by more than one crystallization pathway. Here, we have conducted time-resolved dissolution experiments of MFI-type zeolite crystals in ammonium fluoride medium where detailed structural analysis allowed us to extrapolate and elucidate the possible mechanism of nucleation and crystal growth. A combination of electron and scanning probe microscopy shows that dissolution initiates preferentially at lattice defects and progressively removes defect zones to reveal a mosaic structure of crystalline domains within each zeolite crystal. This mosaic architecture evolves during the growth process, reflecting the changing conditions of zeolite formation that can be retroactively assessed during zeolite crystal dissolution. Moreover, a more general implication of this study is the establishment that dissolution can be used successfully as an ex situ technique to uncover details about crystal growth features inaccessible by other methods.

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