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Dominance of heat transfer limitations in conventional sol-gel synthesis of LTA revealed by microcrystallization

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Abstract

The non-classical nucleation and growth mechanism for hydrothermal zeolite synthesis is a complex convolution of thermodynamic phase transformations, kinetic chemical condensations, three-phase mass transfer and spatial-temporal thermal gradients. The process is typically studied in batch autoclaves heated with laboratory ovens before being scaled in high temperature batch crystallizers. The experimental and theoretical work presented here proposes that transport limitations dominate batch process syntheses. Thus, kinetically-controlled, scalable crystallization must be achieved for accurate elucidation of the underlying crystallization mechanism. A segmented microdroplet crystallizer is used to remove internal and external heat transfer gradients during the synthesis of LTA zeolite crystals. The heat transfer regimes are carefully mapped, and specific criteria are established for overcoming thermal limitations.

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The datasets generated during and/or analyzed during the current study are available from the corresponding author on reasonable request.

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Acknowledgements

The authors acknowledge the American Chemical Society Petroleum Research Fund for financial support, ACS PRF 58609-DNI5.

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The authors acknowledge the American Chemical Society Petroleum Research Fund for financial support, ACS PRF 58609-DNI5.

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Authors and Affiliations

  1. Department of Chemical Engineering, Worcester Polytechnic Institute, 100 Institute Road, Worcester, MA, 01609, USA

    Jacob C. Crislip, Jim Vicens, Thang Pham, Geoffrey Tompsett & Andrew R. Teixeira

  2. Department of Mechanical Engineering, Worcester Polytechnic Institute, 100 Institute Road, Worcester, MA, 01609, USA

    Yifan Zhang

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  1. Jacob C. Crislip
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Highlights

• Five reactor designs that create distinct heat transfer regimes have been used to reveal heat transfer limitations during zeolite crystallization

• Segmented microdroplet microbatch crystallizers used to remove heat transfer limitations

• Nondimensional analysis performed to establish criteria and a regime map for isothermal, kinetically-limited environment

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Crislip, J.C., Vicens, J., Pham, T. et al. Dominance of heat transfer limitations in conventional sol-gel synthesis of LTA revealed by microcrystallization. J Flow Chem 12, 397–408 (2022). https://doi.org/10.1007/s41981-022-00217-1

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