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Use of a pressurized water treatment to prevent cracking of internal gelation sol-gel microspheres

  • Original Paper: Fundamentals of sol-gel and hybrid materials processing
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Abstract

Pressurized water treatments were investigated as a means to prevent cracking of internal gelation sol-gel microspheres upon drying and heating. A batch of gelled cerium oxide microspheres was prepared, split into two samples that were processed with and without a pressurized water treatment, and dried in air at room temperature. Thermogravimetric analysis was used to compare the mass loss profiles between the two samples and to understand volatile emissions from cerium oxide microspheres during heat treatments up to 600 °C. Microspheres that were processed without a pressurized water treatment lost ~4.6 times more mass upon heating than microspheres that were subjected to a pressurized water treatment. Comparison of the cracking behavior of microspheres prepared with and without a pressurized water treatment indicated that microspheres subjected to a pressurized water treatment were virtually crack-free after heat treatments. Conversely, microspheres processed without a pressurized water treatment, which is typical of traditional washing processes, exhibited extensive cracking. Analysis of residues dried from pressurized water treatment effluents indicated that hexamethylenetetramine and urea, which are excess reactants from the internal gelation process, were removed from gelled microspheres during the pressurized water treatment step. Traditional processing methods for preparing internal gelation microspheres use specific feed solution and gelation parameters to reduce subsequent cracking upon drying and heating. Results from this study indicate that more aggressive gel-forming conditions may be used to produce crack-free microspheres, if a pressurized water treatment step is included after washing and before air-drying.

A hydrothermal treatment on gelled microspheres removes species that otherwise cause cracking upon drying the heating.

Highlights

  • High-quality, crack-free microspheres of CeO2 were produced

  • Pressurized water treatments prevented cracking of sol-gel microspheres

  • Pressurized water treatments removed hexamine and urea prior to drying

  • Cracking was attributed to the release of volatile species while drying and heating

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Acknowledgements

Brian Kitchen, Bruce Pierson, Dr Michael Hartman, Dr Gary Was, and Dr John Foster of the University of Michigan Nuclear Engineering and Radiological Sciences Department provided useful ideas and input during the course of this work. The author would like to acknowledge and thank Ted Huston, W. M. Keck Elemental Geochemistry Laboratory, in the University of Michigan Department of Earth and Environmental Sciences, for ICP-HRMS analyses. In addition, the author would like to acknowledge and thank James Windak of the University of Michigan Chemistry Department for operating an electron impact mass spectrometer for experiments and Ian Schwerdt of the Pacific Northwest National Laboratory for paper review. This research was conducted with government support under and awarded by DoD, Air Force Office of Scientific Research, National Defense Science and Engineering Graduate (NDSEG) Fellowship, 32 CFR 168a. This material is based on work supported by the National Science Foundation Graduate Research Fellowship under Grant No. DGE 1256260. Any opinion, findings, and conclusions or recommendations expressed in this material is that of the author and does not necessarily reflect the views of the National Science Foundation. This material is based on work supported by the Center for Space Nuclear Research (CSNR) under the Universities Space Research Association (USRA) Subcontract 06711–003. The USRA operates the CSNR for the Idaho National Laboratory. This research was supported by a research seed grant received from the Michigan Space Grant Consortium with matching funds from the University of Michigan Department of Nuclear Engineering and Radiological Sciences. Pacific Northwest National Laboratory is operated for the United States Department of Energy by Battelle Memorial Institute under contract DE-AC05-76RL01830.

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  1. Jeffrey A. Katalenich

    Present address: Pacific Northwest National Laboratory, 3230 Innovation Blvd., MSIN K8-34, Richland, WA, 99354, USA

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  1. Department of Nuclear Engineering and Radiological Sciences, University of Michigan, 2355 Bonisteel Blvd., Ann Arbor, MI, 48109, USA

    Jeffrey A. Katalenich

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Katalenich, J.A. Use of a pressurized water treatment to prevent cracking of internal gelation sol-gel microspheres. J Sol-Gel Sci Technol 94, 298–309 (2020). https://doi.org/10.1007/s10971-020-05230-1

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