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December 30, 2021Chemistry of MaterialsOpen Access

Host–Guest Silicalite-1 Zeolites: Correlated Disorder and Phase Transition Inhibition by a Small Guest Modification

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Authors

MFMarco FabbianiSAShadi Al‐NahariLPLaura Piveteau

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Overview

Structural analysis reveals guest-induced correlated disorder in silicalite-1 zeolites, indicating complete inhibition of the low-temperature monoclinic-to-orthorhombic phase transition.

Key Points

  • Investigate how nanoscale disorder and guest molecule symmetry influence the low-temperature monoclinic–orthorhombic phase transition in silicalite-1 host–guest zeolites.
  • Synthesized four silicalite-1 zeolites differing in mineralizing agent (F⁻ vs OH⁻), synthesis method (hydrothermal vs solvent-free), and organic structure-directing agent (tetrapropylammonium [TPA] vs tripropylethylammonium [TPEA]).
  • Characterized structural organization across temperatures using X-ray diffraction, Raman spectroscopy, and multinuclear NMR (¹³C, ¹⁴N, and ²⁹Si).
  • Quantified host framework disorder via X-ray structure determinations, anisotropic atomic displacement parameter modeling, and 2D ²⁹Si–²⁹Si INADEQUATE correlation NMR fitting.
  • Positioning of the less symmetric TPEA guest induced correlated geometrical disorder across 50% of the silicalite-1 framework atom sites.
  • Guest-induced correlated framework disorder completely inhibited the monoclinic-to-orthorhombic phase transition at low temperatures.

Cite This Study

Fabbiani et al. (2021) studied this question.

synapsesocial.com/papers/6a82726caedbb2834ec6b27ehttps://doi.org/10.1021/acs.chemmater.1c03721
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