Revealing nanoscale dynamics during an epoxy curing reaction with x-ray photon correlation spectroscopy
Abstract
In this work the evolution of nanoscale properties is measured during the thermally triggered curing of an industrial epoxy adhesive. We use x-ray photon correlation spectroscopy (XPCS) to track the progression of the curing reaction through the local dynamics of filler particles that reflect the formation of a thermoset network. Out-of-equilibrium dynamics are resolved through identification and analysis of the intensity– intensity autocorrelation functions obtained from XPCS. The characteristic time scale and local velocity of the filler is calculated as functions of time and temperature. We find that the dynamics speed up when approaching the curing temperature (Tcure), and decay rapidly once Tcure is reached. We compare the results from XPCS to conventional macroscale characterization by differential scanning calorimetry (DSC). The demonstration and implementation of nanoscale characterization of curing reactions by XPCS proves useful for future development and optimization of epoxy thermoset materials and other industrial adhesive systems.
- Authors:
-
- Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Stony Brook Univ., NY (United States)
- Cornell Univ., Ithaca, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Adhesive Technologies, Duesseldorf (Germany); Henkel AG & Co KGaA, Duesseldorf (Germany)
- Adhesive Technologies, Henkel Corporation, Bridgewater, NJ (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN) and National Synchrotron Light Source II (NSLS-II)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Henkel Corporation
- OSTI Identifier:
- 1614979
- Alternate Identifier(s):
- OSTI ID: 1605042
- Report Number(s):
- BNL-213842-2020-JAAM
Journal ID: ISSN 0021-8979; TRN: US2104970
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Applied Physics
- Additional Journal Information:
- Journal Volume: 127; Journal Issue: 11; Journal ID: ISSN 0021-8979
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; X ray photon correlation spectroscopy; Differential scanning calorimetry
Citation Formats
Yavitt, Benjamin M., Salatto, Daniel, Huang, Zhixing, Koga, Yuto T., Endoh, Maya K., Wiegart, Lutz, Poeller, Sascha, Petrash, Stanislas, and Koga, Tadanori. Revealing nanoscale dynamics during an epoxy curing reaction with x-ray photon correlation spectroscopy. United States: N. p., 2020.
Web. doi:10.1063/1.5141488.
Yavitt, Benjamin M., Salatto, Daniel, Huang, Zhixing, Koga, Yuto T., Endoh, Maya K., Wiegart, Lutz, Poeller, Sascha, Petrash, Stanislas, & Koga, Tadanori. Revealing nanoscale dynamics during an epoxy curing reaction with x-ray photon correlation spectroscopy. United States. https://doi.org/10.1063/1.5141488
Yavitt, Benjamin M., Salatto, Daniel, Huang, Zhixing, Koga, Yuto T., Endoh, Maya K., Wiegart, Lutz, Poeller, Sascha, Petrash, Stanislas, and Koga, Tadanori. Tue .
"Revealing nanoscale dynamics during an epoxy curing reaction with x-ray photon correlation spectroscopy". United States. https://doi.org/10.1063/1.5141488. https://www.osti.gov/servlets/purl/1614979.
@article{osti_1614979,
title = {Revealing nanoscale dynamics during an epoxy curing reaction with x-ray photon correlation spectroscopy},
author = {Yavitt, Benjamin M. and Salatto, Daniel and Huang, Zhixing and Koga, Yuto T. and Endoh, Maya K. and Wiegart, Lutz and Poeller, Sascha and Petrash, Stanislas and Koga, Tadanori},
abstractNote = {In this work the evolution of nanoscale properties is measured during the thermally triggered curing of an industrial epoxy adhesive. We use x-ray photon correlation spectroscopy (XPCS) to track the progression of the curing reaction through the local dynamics of filler particles that reflect the formation of a thermoset network. Out-of-equilibrium dynamics are resolved through identification and analysis of the intensity– intensity autocorrelation functions obtained from XPCS. The characteristic time scale and local velocity of the filler is calculated as functions of time and temperature. We find that the dynamics speed up when approaching the curing temperature (Tcure), and decay rapidly once Tcure is reached. We compare the results from XPCS to conventional macroscale characterization by differential scanning calorimetry (DSC). The demonstration and implementation of nanoscale characterization of curing reactions by XPCS proves useful for future development and optimization of epoxy thermoset materials and other industrial adhesive systems.},
doi = {10.1063/1.5141488},
journal = {Journal of Applied Physics},
number = 11,
volume = 127,
place = {United States},
year = {Tue Mar 17 00:00:00 EDT 2020},
month = {Tue Mar 17 00:00:00 EDT 2020}
}
Web of Science
Works referenced in this record:
X-ray cross correlation analysis uncovers hidden local symmetries in disordered matter
journal, June 2009
- Wochner, Peter; Gutt, Christian; Autenrieth, Tina
- Proceedings of the National Academy of Sciences, Vol. 106, Issue 28
Glass Transition as the Rheological Inverse of Gelation
journal, March 2013
- Winter, H. Henning
- Macromolecules, Vol. 46, Issue 6
50th Anniversary Perspective : Are Polymer Nanocomposites Practical for Applications?
journal, January 2017
- Kumar, Sanat K.; Benicewicz, Brian C.; Vaia, Richard A.
- Macromolecules, Vol. 50, Issue 3
A Study of Reaction Kinetics by Near-Infrared Spectroscopy. 1. Comprehensive Analysis of a Model Epoxy/Amine System
journal, April 1995
- Mijovic, Jovan; Andjelic, Sasa
- Macromolecules, Vol. 28, Issue 8
X-ray Photon Correlation Spectroscopy of Filler in Rubber
journal, March 2007
- Shinohara, Yuya; Kishimoto, Hiroyuki; Maejima, Taketo
- Japanese Journal of Applied Physics, Vol. 46, Issue No. 4
Enhanced gel formation in binary mixtures of nanocolloids with short-range attraction
journal, January 2018
- Harden, James L.; Guo, Hongyu; Bertrand, Martine
- The Journal of Chemical Physics, Vol. 148, Issue 4
Epoxy clay nanocomposites – processing, properties and applications: A review
journal, February 2013
- Azeez, Asif Abdul; Rhee, Kyong Yop; Park, Soo Jin
- Composites Part B: Engineering, Vol. 45, Issue 1
Reduced Viscosity of the Free Surface in Entangled Polymer Melt Films
journal, February 2010
- Koga, Tadanori; Li, C.; Endoh, M. K.
- Physical Review Letters, Vol. 104, Issue 6
Slow dynamics and aging in colloidal gels studied by x-ray photon correlation spectroscopy
journal, July 2007
- Fluerasu, Andrei; Moussaïd, Abdellatif; Madsen, Anders
- Physical Review E, Vol. 76, Issue 1
Selective transformations of 2,3-epoxy alcohols and related derivatives. Strategies for nucleophilic attack at carbon-3 or carbon-2
journal, December 1985
- Behrens, Carl H.; Sharpless, K. Barry
- The Journal of Organic Chemistry, Vol. 50, Issue 26
A study by Raman, near-infrared and dynamic-mechanical spectroscopies on the curing behaviour, molecular structure and viscoelastic properties of epoxy/anhydride networks
journal, June 2007
- Musto, Pellegrino; Abbate, Mario; Ragosta, Giuseppe
- Polymer, Vol. 48, Issue 13
Nanoparticle Motion within Glassy Polymer Melts
journal, February 2009
- Guo, Hongyu; Bourret, Gilles; Corbierre, Muriel K.
- Physical Review Letters, Vol. 102, Issue 7
The phase diagram of colloidal silica–PNIPAm core–shell nanogels
journal, January 2020
- Frenzel, Lara; Lehmkühler, Felix; Koof, Michael
- Soft Matter, Vol. 16, Issue 2
Anomalous Dynamics of Concentrated Silica-PNIPAm Nanogels
journal, August 2019
- Frenzel, Lara; Lehmkühler, Felix; Lokteva, Irina
- The Journal of Physical Chemistry Letters, Vol. 10, Issue 17
Beyond simple exponential correlation functions and equilibrium dynamics in x-ray photon correlation spectroscopy
journal, May 2010
- Madsen, Anders; Leheny, Robert L.; Guo, Hongyu
- New Journal of Physics, Vol. 12, Issue 5
Structure and dynamics of polymer nanocomposites studied by X-ray and neutron scattering techniques
journal, August 2015
- Genix, Anne-Caroline; Oberdisse, Julian
- Current Opinion in Colloid & Interface Science, Vol. 20, Issue 4
XPCS: Nanoscale motion and rheology
journal, February 2012
- Leheny, Robert L.
- Current Opinion in Colloid & Interface Science, Vol. 17, Issue 1
In situ real-time monitoring of epoxy/amine kinetics by remote near infrared spectroscopy
journal, January 1996
- Mijović, Jovan; Andjelić, Saša; Kenny, José M.
- Polymers for Advanced Technologies, Vol. 7, Issue 1
Nanoparticle self-assembly: from interactions in suspension to polymer nanocomposites
journal, January 2018
- Genix, Anne-Caroline; Oberdisse, Julian
- Soft Matter, Vol. 14, Issue 25
Sub-microsecond-resolved multi-speckle X-ray photon correlation spectroscopy with a pixel array detector
journal, August 2018
- Zhang, Qingteng; Dufresne, Eric M.; Narayanan, Suresh
- Journal of Synchrotron Radiation, Vol. 25, Issue 5
Mode amplitudes in dynamic light scattering by concentrated liquid suspensions of polydisperse hard spheres
journal, November 1982
- Pusey, P. N.; Fijnaut, H. M.; Vrij, A.
- The Journal of Chemical Physics, Vol. 77, Issue 9
Rheological behavior of an epoxy/amine system near the gel point
journal, January 1992
- Lairez, D.; Adam, M.; Emery, J. R.
- Macromolecules, Vol. 25, Issue 1
Glass transition temperature versus conversion relationships for thermosetting polymers
journal, January 1990
- Pascault, J. P.; Williams, R. J. J.
- Journal of Polymer Science Part B: Polymer Physics, Vol. 28, Issue 1
Advances in addition-cure phenolic resins
journal, May 2004
- Nair, C.
- Progress in Polymer Science, Vol. 29, Issue 5
Analysis of the reaction mechanism of the thiol–epoxy addition initiated by nucleophilic tertiary amines
journal, January 2017
- Konuray, Ali Osman; Fernández-Francos, Xavier; Ramis, Xavier
- Polymer Chemistry, Vol. 8, Issue 38
X Ray Photon Correlation Spectroscopy for the study of polymer dynamics
journal, August 2016
- Nogales, Aurora; Fluerasu, Andrei
- European Polymer Journal, Vol. 81
X-ray photon correlation spectroscopy
journal, August 2014
- Shpyrko, Oleg G.
- Journal of Synchrotron Radiation, Vol. 21, Issue 5
Theory of dynamic light scattering from polydisperse systems
journal, January 1976
- Aragón, S. R.
- The Journal of Chemical Physics, Vol. 64, Issue 6
Gel point determination of gelatin hydrogels by dynamic light scattering and rheological measurements
journal, September 2007
- Matsunaga, Takuro; Shibayama, Mitsuhiro
- Physical Review E, Vol. 76, Issue 3
Evolution of Particle-Scale Dynamics in an Aging Clay Suspension
journal, November 2004
- Bandyopadhyay, R.; Liang, D.; Yardimci, H.
- Physical Review Letters, Vol. 93, Issue 22
Silica nanoparticles as tracers of the gelation dynamics of a natural biopolymer physical gel
journal, January 2014
- Ruta, B.; Czakkel, O.; Chushkin, Y.
- Soft Matter, Vol. 10, Issue 25
Gel formation and aging in weakly attractive nanocolloid suspensions at intermediate concentrations
journal, October 2011
- Guo, Hongyu; Ramakrishnan, S.; Harden, James L.
- The Journal of Chemical Physics, Vol. 135, Issue 15
Universal non-diffusive slow dynamics in aging soft matter
journal, September 2002
- Cipelletti, Luca; Ramos, Laurence; Manley, S.
- Faraday Discussions, Vol. 123
Anisotropic de Gennes Narrowing in Confined Fluids
journal, April 2016
- Nygård, Kim; Buitenhuis, Johan; Kagias, Matias
- Physical Review Letters, Vol. 116, Issue 16
In Operando Monitoring of Dynamic Recovery in 3D-Printed Thermoset Nanocomposites by XPCS
journal, June 2019
- Johnson, Kyle J.; Wiegart, Lutz; Abbott, Andrew C.
- Langmuir, Vol. 35, Issue 26
Dynamic light-scattering study of the glass transition in a colloidal suspension
journal, May 1991
- van Megen, W.; Pusey, P. N.
- Physical Review A, Vol. 43, Issue 10
Learning about epoxy cure mechanisms from isoconversional analysis of DSC data
journal, June 2002
- Sbirrazzuoli, Nicolas; Vyazovkin, Sergey
- Thermochimica Acta, Vol. 388, Issue 1-2
Observations of Gelation and Vitrification of a Thermosetting Resin during the Evolution of Polymerization Shrinkage
journal, September 2005
- Yu, Hong; Mhaisalkar, Subodh G.; Wong, Ee Hua
- Macromolecular Rapid Communications, Vol. 26, Issue 18
Glycidyl Ether Reactions with Alcohols, Phenols, Carboxylic Acids, and Acid Anhydrides
journal, January 1956
- Shechter, Leon; Wynstra, John
- Industrial & Engineering Chemistry, Vol. 48, Issue 1
Epoxy resin composites with surface-modified silicon dioxide nanoparticles: A review
journal, April 2013
- Sprenger, Stephan
- Journal of Applied Polymer Science, Vol. 130, Issue 3
Observation of Filler Dynamics in Rubber with X-ray Photon Correlation Spectroscopy
journal, September 2011
- Shinohara, Yuya; Kishimoto, Hiroyuki; Maejima, Taketo
- IOP Conference Series: Materials Science and Engineering, Vol. 24
Anhydride-cured epoxies via chain reaction. 1. The phenyl glycidyl ether/phthalic acid anhydride system
journal, August 1991
- Trappe, V.; Burchard, W.; Steinmann, B.
- Macromolecules, Vol. 24, Issue 17
Evolution of dynamics and structure during formation of a cross-linked polymer gel
journal, June 2011
- Czakkel, O.; Madsen, A.
- EPL (Europhysics Letters), Vol. 95, Issue 2
Universal Aging Features in the Restructuring of Fractal Colloidal Gels
journal, March 2000
- Cipelletti, Luca; Manley, S.; Ball, R. C.
- Physical Review Letters, Vol. 84, Issue 10
Size-Dependent Particle Dynamics in Entangled Polymer Nanocomposites
journal, January 2016
- Mangal, Rahul; Srivastava, Samanvaya; Narayanan, Suresh
- Langmuir, Vol. 32, Issue 2
In Situ Analysis of the Relationship between Cure Kinetics and the Mechanical Modulus of an Epoxy Resin
journal, November 2014
- Aldridge, Michael; Wineman, Alan; Waas, Anthony
- Macromolecules, Vol. 47, Issue 23
Cure kinetics characterization and monitoring of an epoxy resin using DSC, Raman spectroscopy, and DEA
journal, June 2013
- Hardis, Ricky; Jessop, Julie L. P.; Peters, Frank E.
- Composites Part A: Applied Science and Manufacturing, Vol. 49
Software tools for X-ray photon correlation and X-ray speckle visibility spectroscopy
conference, August 2016
- Abeykoon, Sameera K.; Zhang, Yugang; Dill, Eric D.
- 2016 New York Scientific Data Summit (NYSDS)
Temperature Dependence of the Behavior of an Epoxy−Amine System near the Gel Point through Viscoelastic Study. 1. Low- T g Epoxy−Amine System
journal, January 1996
- Eloundou, J. P.; Feve, M.; Gerard, J. F.
- Macromolecules, Vol. 29, Issue 21
Synthesis and application of epoxy resins: A review
journal, September 2015
- Jin, Fan-Long; Li, Xiang; Park, Soo-Jin
- Journal of Industrial and Engineering Chemistry, Vol. 29
Stereoselective Epoxide Polymerization and Copolymerization
journal, July 2014
- Childers, M. Ian; Longo, Julie M.; Van Zee, Nathan J.
- Chemical Reviews, Vol. 114, Issue 16
Reaction mechanism, cure behavior and properties of a multifunctional epoxy resin, TGDDM, with latent curing agent dicyandiamide
journal, January 2018
- Wu, Feng; Zhou, Xingping; Yu, Xinhai
- RSC Advances, Vol. 8, Issue 15
In Situ Vibrational Probes of Epoxy Gelation
journal, July 2019
- Granado, Lérys; Kempa, Stefan; Gregoriades, Laurence John
- ACS Macro Letters, Vol. 8, Issue 8