Coupling of organic and inorganic chemistry presents a new degree of freedom in nano-engineering of thermo-mechanical properties of cement-based materials. Despite these vast technological benefits, molecular scale cross-linking of calcium-silicate-hydrate (C-S-H) gel with organic molecules still presents a significant challenge. Herein, we report experimental results on sol-gel synthesis, structure and morphology of nanocrystalline C-S-H cross-linked with dipodal organosilanes. These novel organic-inorganic gels have layered turbostratic molecular structure with similarities to C-S-H precipitating in hydrating cement paste. The organic molecules' chain length controls the interlayer spacing, which shows little to no shrinkage upon dehydration up to 105 °C. However, the structure gets distorted in the basal crystallite plane, in which dimer and trimer Si-polyhedra structures condense on a 2D hexagonal Ca-polyhedra layer. Cross-linked C-S-H gels display plate-like morphology with tendency toward stacking into agglomerates at the larger scale. If successfully realized in cement environment, e.g. high concentration seed, such novel organic-inorganic C-S-H gels could potentially provide cement-based matrices with unique properties unmatched by classical inorganic systems.
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Parametric Control of Melting Gel Morphology and Chemistry via Electrospray Deposition
Melting gels are a class of hybrid organic-inorganic silica based gels prepared via the sol-gel process that are solid below their glass transition temperatures, near room temperature, but show thermoplastic behavior when heated. While this phase change can be repeated multiple times, heating the gel past its consolidation temperatures, typically above 130 oC initiates an irreversible reaction that produces highly crosslinked glassy organic-inorganic materials via hydrolysis and poly-condensation. This ability makes melting gels uniquely compatible with processing techniques inaccessible to other sol-gels. By properly tuning their properties, it should be possible to create protective coatings for electronics and anti-corrosive coatings for metals that are highly hydrophobic and insulating. However, melting gel consolidation reactions are highly dependent on charge interactions, raising the question of how these materials will respond to a processing technique, like electrospray deposition (ESD), which is dependent on charge delivery. In this study, we focus on the role that substrate temperature and charge polarity play on film morphology, consolidation chemistry, and surface properties. Optical images, film thickness measurements, nanoindentation, and FTIR were used to characterize the sprayed melting gel with the goal of developing a robust processing space for producing highly cross linked, hydrophobic, dielectric coatings.
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- Award ID(s):
- 1911509
- NSF-PAR ID:
- 10293459
- Date Published:
- Journal Name:
- ASME 2021 16th International Manufacturing Science and Engineering Conference
- Volume:
- 2
- Issue:
- 1
- Page Range / eLocation ID:
- 1-5
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Conference Paper:
- https://doi.org/https://doi.org/10.1115/MSEC2021-63347
