Surface-Functionalized Cellulose Nanocrystals as Nanofillers for Crosslinking Processes: Implications for Thermosetting Resins
Abstract
Understanding the response of fillers in the epoxy resin crosslinking process and characterizing polymer–filler dynamics are the key features that guide the engineering of new thermosetting resin composites. Here, in this work, X-ray photon correlation spectroscopy (XPCS) is used as a thermal analysis tool to track the microscopic changes occurring during the cure of a functionalized cellulose nanocrystal (mCNC)–epoxy composite. In contrast, traditional methods such as differential scanning calorimetry (DSC) and curing rheology are used to understand the kinetics and properties on macroscopic length scales. Of interest is the influence of the mCNC on the curing kinetics and properties of the thermosetting resin. Two levels of modification (increasing hydrophobicity) were chosen to observe the effect of functionalization. Before cure, the highly functionalized CNC (mCNC3) shows a 44% increase in complex viscosity (η*), while the less functionalized CNC (mCNC2) shows a η* value similar to that of the neat resin. As the cure cycle progresses, results from DSC, rheology, and XPCS further show the enhancement in dispersion for mCNC3. The results show a clear difference in the maximum drift velocity, maximum heat flow, and complex viscosity during the ramp to the isothermal cure temperature (Tcure). Such results suggest that mCNC3 containsmore »
- Authors:
-
[1];
[2];
[1]
- FAMU-FSU Engineering, Tallahassee, FL (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1889158
- Report Number(s):
- BNL-223458-2022-JAAM
Journal ID: ISSN 2574-0970
- Grant/Contract Number:
- SC0012704; 1735968
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Nano Materials
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 2; Journal ID: ISSN 2574-0970
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; composites; differential scanning calorimetry; fluid dynamics; organic polymers; cellulose nanocrystals; x-ray photon correlation spectroscopy; epoxy composite; thermosetting resins; filler dynamics; curing kinetics
Citation Formats
Haney, Roneisha, Kollarigowda, Ravichandran H., Wiegart, Lutz, and Ramakrishnan, Subramanian. Surface-Functionalized Cellulose Nanocrystals as Nanofillers for Crosslinking Processes: Implications for Thermosetting Resins. United States: N. p., 2022.
Web. doi:10.1021/acsanm.1c03508.
Haney, Roneisha, Kollarigowda, Ravichandran H., Wiegart, Lutz, & Ramakrishnan, Subramanian. Surface-Functionalized Cellulose Nanocrystals as Nanofillers for Crosslinking Processes: Implications for Thermosetting Resins. United States. https://doi.org/10.1021/acsanm.1c03508
Haney, Roneisha, Kollarigowda, Ravichandran H., Wiegart, Lutz, and Ramakrishnan, Subramanian. Tue .
"Surface-Functionalized Cellulose Nanocrystals as Nanofillers for Crosslinking Processes: Implications for Thermosetting Resins". United States. https://doi.org/10.1021/acsanm.1c03508. https://www.osti.gov/servlets/purl/1889158.
@article{osti_1889158,
title = {Surface-Functionalized Cellulose Nanocrystals as Nanofillers for Crosslinking Processes: Implications for Thermosetting Resins},
author = {Haney, Roneisha and Kollarigowda, Ravichandran H. and Wiegart, Lutz and Ramakrishnan, Subramanian},
abstractNote = {Understanding the response of fillers in the epoxy resin crosslinking process and characterizing polymer–filler dynamics are the key features that guide the engineering of new thermosetting resin composites. Here, in this work, X-ray photon correlation spectroscopy (XPCS) is used as a thermal analysis tool to track the microscopic changes occurring during the cure of a functionalized cellulose nanocrystal (mCNC)–epoxy composite. In contrast, traditional methods such as differential scanning calorimetry (DSC) and curing rheology are used to understand the kinetics and properties on macroscopic length scales. Of interest is the influence of the mCNC on the curing kinetics and properties of the thermosetting resin. Two levels of modification (increasing hydrophobicity) were chosen to observe the effect of functionalization. Before cure, the highly functionalized CNC (mCNC3) shows a 44% increase in complex viscosity (η*), while the less functionalized CNC (mCNC2) shows a η* value similar to that of the neat resin. As the cure cycle progresses, results from DSC, rheology, and XPCS further show the enhancement in dispersion for mCNC3. The results show a clear difference in the maximum drift velocity, maximum heat flow, and complex viscosity during the ramp to the isothermal cure temperature (Tcure). Such results suggest that mCNC3 contains a well-dispersed network of particles due to the higher level of functionalization. During Tcure, a transition in elastic modulus (G') occurs only for the highly functionalized CNC particle system. We believe that heat-induced aggregation occurs, and the crosslinked resin ultimately dominates the macroscopic properties of the final cured system for all samples. The results from the three techniques are in good agreement and showcase XPCS as a beneficial experimental tool for characterizing the microscopic dynamics of particulate-filled thermosetting resins. Hence, we envision this to be a fundamental curing study for the design of thermosetting resin composites.},
doi = {10.1021/acsanm.1c03508},
journal = {ACS Applied Nano Materials},
number = 2,
volume = 5,
place = {United States},
year = {Tue Feb 15 00:00:00 EST 2022},
month = {Tue Feb 15 00:00:00 EST 2022}
}
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