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Combining Coarse-Grained Reactive Molecular Dynamics with an Enhanced-Sampling Method for MFI Zeolite

Da Zheng1,2, Junfeng Wang1,3, Hongqiang Cui1,2

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Journal of Chemical Theory and Computation
|January 23, 2026
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Summary
This summary is machine-generated.

We developed a new model to simulate zeolite crystallization, revealing the microscopic steps from disordered materials to ordered crystals. This advances understanding of zeolite formation for catalysis and separation applications.

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Area of Science:

  • Materials Science
  • Chemical Engineering
  • Computational Chemistry

Background:

  • Zeolite crystallization kinetics, particularly nucleation, are crucial for chemical engineering but poorly understood at the microscopic level due to nucleation rarity.
  • Existing models struggle to capture the complex multicomponent dynamics of zeolite formation.

Purpose of the Study:

  • To develop a computational model simulating zeolite nucleation and growth.
  • To elucidate the microscopic mechanisms of MFI-type zeolite formation.
  • To provide insights for rational zeolite material design.

Main Methods:

  • Developed a coarse-grained reactive zeolite assembly model (CG-ReZAM).
  • Incorporated organic structure-directing agents (OSDAs) and silicate polymerization dynamics.
  • Utilized cluster-weighted root-mean-square deviation (cRMSD) and a ratcheting scheme for enhanced sampling of nucleation events.
  • Analyzed mean first-passage time (MFPT) to determine critical nucleus size.

Main Results:

  • Successfully reproduced the four stages of silicate polymerization: oligomerization, ring formation, cluster aggregation, and aging.
  • Observed ordered arrangements of tetrapropylammonium (TPA+) cations, confirming their structure-directing role.
  • Revealed the transformation pathway from amorphous aggregates to ordered MFI-type zeolite crystals.
  • Determined a critical nucleus size consistent with experimental data.

Conclusions:

  • The CG-ReZAM combined with enhanced sampling reliably simulates zeolite crystallization.
  • This framework provides valuable theoretical insights into zeolite nucleation and growth.
  • The findings support the rational design of zeolite materials for catalysis and separation.