Revealing nanoscale dynamics during an epoxy curing reaction with x-ray photon correlation spectroscopy

Yavitt, Benjamin M.; Salatto, Daniel; Huang, Zhixing; Koga, Yuto T.; Endoh, Maya K.; Wiegart, Lutz; Poeller, Sascha; Petrash, Stanislas; Koga, Tadanori

doi:10.1063/1.5141488

Title: Revealing nanoscale dynamics during an epoxy curing reaction with x-ray photon correlation spectroscopy

Journal Article · 17 March 2020 · Journal of Applied Physics

DOI: https://doi.org/10.1063/1.5141488 · OSTI ID:1614979

^[1]; Salatto, Daniel ^[2]; Huang, Zhixing ^[2]; Koga, Yuto T. ^[3]; Endoh, Maya K. ^[2]; Wiegart, Lutz ^[4];

^[5]; Petrash, Stanislas ^[6];

^[2]

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)

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 (T_cure), and decay rapidly once T_cure 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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN) and National Synchrotron Light Source II (NSLS-II)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Henkel Corporation

Grant/Contract Number:: SC0012704

OSTI ID:: 1614979

Report Number(s):: BNL--213842-2020-JAAM

Journal Information:: Journal of Applied Physics, Journal Name: Journal of Applied Physics Journal Issue: 11 Vol. 127; ISSN 0021-8979

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (56)

In situ real-time monitoring of epoxy/amine kinetics by remote near infrared spectroscopy Mijović, Jovan; Andjelić, Saša; Kenny, José M. Polymers for Advanced Technologies, Vol. 7, Issue 1 https://doi.org/10.1002/(SICI)1099-1581(199601)7:1<1::AID-PAT480>3.0.CO;2-N	journal	January 1996
Epoxy resin composites with surface-modified silicon dioxide nanoparticles: A review Sprenger, Stephan Journal of Applied Polymer Science, Vol. 130, Issue 3 https://doi.org/10.1002/app.39208	journal	April 2013
Observations of Gelation and Vitrification of a Thermosetting Resin during the Evolution of Polymerization Shrinkage Yu, Hong; Mhaisalkar, Subodh G.; Wong, Ee Hua Macromolecular Rapid Communications, Vol. 26, Issue 18 https://doi.org/10.1002/marc.200500333	journal	September 2005
Glass transition temperature versus conversion relationships for thermosetting polymers Pascault, J. P.; Williams, R. J. J. Journal of Polymer Science Part B: Polymer Physics, Vol. 28, Issue 1 https://doi.org/10.1002/polb.1990.090280107	journal	January 1990
Learning about epoxy cure mechanisms from isoconversional analysis of DSC data Sbirrazzuoli, Nicolas; Vyazovkin, Sergey Thermochimica Acta, Vol. 388, Issue 1-2 https://doi.org/10.1016/S0040-6031(02)00053-9	journal	June 2002
XPCS: Nanoscale motion and rheology Leheny, Robert L. Current Opinion in Colloid & Interface Science, Vol. 17, Issue 1 https://doi.org/10.1016/j.cocis.2011.11.002	journal	February 2012
Structure and dynamics of polymer nanocomposites studied by X-ray and neutron scattering techniques Genix, Anne-Caroline; Oberdisse, Julian Current Opinion in Colloid & Interface Science, Vol. 20, Issue 4 https://doi.org/10.1016/j.cocis.2015.10.002	journal	August 2015
Cure kinetics characterization and monitoring of an epoxy resin using DSC, Raman spectroscopy, and DEA Hardis, Ricky; Jessop, Julie L. P.; Peters, Frank E. Composites Part A: Applied Science and Manufacturing, Vol. 49 https://doi.org/10.1016/j.compositesa.2013.01.021	journal	June 2013
Epoxy clay nanocomposites – processing, properties and applications: A review Azeez, Asif Abdul; Rhee, Kyong Yop; Park, Soo Jin Composites Part B: Engineering, Vol. 45, Issue 1 https://doi.org/10.1016/j.compositesb.2012.04.012	journal	February 2013
X Ray Photon Correlation Spectroscopy for the study of polymer dynamics Nogales, Aurora; Fluerasu, Andrei European Polymer Journal, Vol. 81 https://doi.org/10.1016/j.eurpolymj.2016.03.032	journal	August 2016
Synthesis and application of epoxy resins: A review Jin, Fan-Long; Li, Xiang; Park, Soo-Jin Journal of Industrial and Engineering Chemistry, Vol. 29 https://doi.org/10.1016/j.jiec.2015.03.026	journal	September 2015
A study by Raman, near-infrared and dynamic-mechanical spectroscopies on the curing behaviour, molecular structure and viscoelastic properties of epoxy/anhydride networks Musto, Pellegrino; Abbate, Mario; Ragosta, Giuseppe Polymer, Vol. 48, Issue 13 https://doi.org/10.1016/j.polymer.2007.04.042	journal	June 2007
Advances in addition-cure phenolic resins Nair, C. Progress in Polymer Science, Vol. 29, Issue 5 https://doi.org/10.1016/j.progpolymsci.2004.01.004	journal	May 2004
Anomalous Dynamics of Concentrated Silica-PNIPAm Nanogels Frenzel, Lara; Lehmkühler, Felix; Lokteva, Irina The Journal of Physical Chemistry Letters, Vol. 10, Issue 17 https://doi.org/10.1021/acs.jpclett.9b01690	journal	August 2019
Size-Dependent Particle Dynamics in Entangled Polymer Nanocomposites Mangal, Rahul; Srivastava, Samanvaya; Narayanan, Suresh Langmuir, Vol. 32, Issue 2 https://doi.org/10.1021/acs.langmuir.5b03311	journal	January 2016
In Operando Monitoring of Dynamic Recovery in 3D-Printed Thermoset Nanocomposites by XPCS Johnson, Kyle J.; Wiegart, Lutz; Abbott, Andrew C. Langmuir, Vol. 35, Issue 26 https://doi.org/10.1021/acs.langmuir.9b00766	journal	June 2019
50th Anniversary Perspective : Are Polymer Nanocomposites Practical for Applications? Kumar, Sanat K.; Benicewicz, Brian C.; Vaia, Richard A. Macromolecules, Vol. 50, Issue 3 https://doi.org/10.1021/acs.macromol.6b02330	journal	January 2017
In Situ Vibrational Probes of Epoxy Gelation Granado, Lérys; Kempa, Stefan; Gregoriades, Laurence John ACS Macro Letters, Vol. 8, Issue 8 https://doi.org/10.1021/acsmacrolett.9b00508	journal	July 2019
Stereoselective Epoxide Polymerization and Copolymerization Childers, M. Ian; Longo, Julie M.; Van Zee, Nathan J. Chemical Reviews, Vol. 114, Issue 16 https://doi.org/10.1021/cr400725x	journal	July 2014
Glycidyl Ether Reactions with Alcohols, Phenols, Carboxylic Acids, and Acid Anhydrides Shechter, Leon; Wynstra, John Industrial & Engineering Chemistry, Vol. 48, Issue 1 https://doi.org/10.1021/ie50553a028	journal	January 1956
Selective transformations of 2,3-epoxy alcohols and related derivatives. Strategies for nucleophilic attack at carbon-3 or carbon-2 Behrens, Carl H.; Sharpless, K. Barry The Journal of Organic Chemistry, Vol. 50, Issue 26 https://doi.org/10.1021/jo00350a051	journal	December 1985
Anhydride-cured epoxies via chain reaction. 1. The phenyl glycidyl ether/phthalic acid anhydride system Trappe, V.; Burchard, W.; Steinmann, B. Macromolecules, Vol. 24, Issue 17 https://doi.org/10.1021/ma00017a002	journal	August 1991
Rheological behavior of an epoxy/amine system near the gel point Lairez, D.; Adam, M.; Emery, J. R. Macromolecules, Vol. 25, Issue 1 https://doi.org/10.1021/ma00027a046	journal	January 1992
A Study of Reaction Kinetics by Near-Infrared Spectroscopy. 1. Comprehensive Analysis of a Model Epoxy/Amine System Mijovic, Jovan; Andjelic, Sasa Macromolecules, Vol. 28, Issue 8 https://doi.org/10.1021/ma00112a026	journal	April 1995
Glass Transition as the Rheological Inverse of Gelation Winter, H. Henning Macromolecules, Vol. 46, Issue 6 https://doi.org/10.1021/ma400086v	journal	March 2013
In Situ Analysis of the Relationship between Cure Kinetics and the Mechanical Modulus of an Epoxy Resin Aldridge, Michael; Wineman, Alan; Waas, Anthony Macromolecules, Vol. 47, Issue 23 https://doi.org/10.1021/ma501441c	journal	November 2014
Temperature Dependence of the Behavior of an Epoxy−Amine System near the Gel Point through Viscoelastic Study. 1. Low- T _g Epoxy−Amine System Eloundou, J. P.; Feve, M.; Gerard, J. F. Macromolecules, Vol. 29, Issue 21 https://doi.org/10.1021/ma960287d	journal	January 1996
Analysis of the reaction mechanism of the thiol–epoxy addition initiated by nucleophilic tertiary amines Konuray, Ali Osman; Fernández-Francos, Xavier; Ramis, Xavier Polymer Chemistry, Vol. 8, Issue 38 https://doi.org/10.1039/C7PY01263B	journal	January 2017
Reaction mechanism, cure behavior and properties of a multifunctional epoxy resin, TGDDM, with latent curing agent dicyandiamide Wu, Feng; Zhou, Xingping; Yu, Xinhai RSC Advances, Vol. 8, Issue 15 https://doi.org/10.1039/C7RA13233F	journal	January 2018
Nanoparticle self-assembly: from interactions in suspension to polymer nanocomposites Genix, Anne-Caroline; Oberdisse, Julian Soft Matter, Vol. 14, Issue 25 https://doi.org/10.1039/C8SM00430G	journal	January 2018
The phase diagram of colloidal silica–PNIPAm core–shell nanogels Frenzel, Lara; Lehmkühler, Felix; Koof, Michael Soft Matter, Vol. 16, Issue 2 https://doi.org/10.1039/C9SM01884K	journal	January 2020
Universal non-diffusive slow dynamics in aging soft matter Cipelletti, Luca; Ramos, Laurence; Manley, S. Faraday Discussions, Vol. 123 https://doi.org/10.1039/b204495a	journal	September 2002
Silica nanoparticles as tracers of the gelation dynamics of a natural biopolymer physical gel Ruta, B.; Czakkel, O.; Chushkin, Y. Soft Matter, Vol. 10, Issue 25 https://doi.org/10.1039/c4sm00704b	journal	January 2014
Gel formation and aging in weakly attractive nanocolloid suspensions at intermediate concentrations Guo, Hongyu; Ramakrishnan, S.; Harden, James L. The Journal of Chemical Physics, Vol. 135, Issue 15 https://doi.org/10.1063/1.3653380	journal	October 2011
Theory of dynamic light scattering from polydisperse systems Aragón, S. R. The Journal of Chemical Physics, Vol. 64, Issue 6 https://doi.org/10.1063/1.432528	journal	January 1976
Mode amplitudes in dynamic light scattering by concentrated liquid suspensions of polydisperse hard spheres Pusey, P. N.; Fijnaut, H. M.; Vrij, A. The Journal of Chemical Physics, Vol. 77, Issue 9 https://doi.org/10.1063/1.444428	journal	November 1982
Enhanced gel formation in binary mixtures of nanocolloids with short-range attraction Harden, James L.; Guo, Hongyu; Bertrand, Martine The Journal of Chemical Physics, Vol. 148, Issue 4 https://doi.org/10.1063/1.5007038	journal	January 2018
X-ray cross correlation analysis uncovers hidden local symmetries in disordered matter Wochner, Peter; Gutt, Christian; Autenrieth, Tina Proceedings of the National Academy of Sciences, Vol. 106, Issue 28 https://doi.org/10.1073/pnas.0905337106	journal	June 2009
Beyond simple exponential correlation functions and equilibrium dynamics in x-ray photon correlation spectroscopy Madsen, Anders; Leheny, Robert L.; Guo, Hongyu New Journal of Physics, Vol. 12, Issue 5 https://doi.org/10.1088/1367-2630/12/5/055001	journal	May 2010
Observation of Filler Dynamics in Rubber with X-ray Photon Correlation Spectroscopy Shinohara, Yuya; Kishimoto, Hiroyuki; Maejima, Taketo IOP Conference Series: Materials Science and Engineering, Vol. 24 https://doi.org/10.1088/1757-899X/24/1/012005	journal	September 2011
Dynamic light-scattering study of the glass transition in a colloidal suspension van Megen, W.; Pusey, P. N. Physical Review A, Vol. 43, Issue 10 https://doi.org/10.1103/PhysRevA.43.5429	journal	May 1991
Structure and dynamics of concentrated dispersions of polystyrene latex spheres in glycerol: Static and dynamic x-ray scattering Lumma, D.; Lurio, L. B.; Borthwick, M. A. Physical Review E, Vol. 62, Issue 6 https://doi.org/10.1103/PhysRevE.62.8258	journal	December 2000
Slow dynamics and aging in colloidal gels studied by x-ray photon correlation spectroscopy Fluerasu, Andrei; Moussaïd, Abdellatif; Madsen, Anders Physical Review E, Vol. 76, Issue 1 https://doi.org/10.1103/PhysRevE.76.010401	journal	July 2007
Gel point determination of gelatin hydrogels by dynamic light scattering and rheological measurements Matsunaga, Takuro; Shibayama, Mitsuhiro Physical Review E, Vol. 76, Issue 3 https://doi.org/10.1103/PhysRevE.76.030401	journal	September 2007
Nanoparticle Motion within Glassy Polymer Melts Guo, Hongyu; Bourret, Gilles; Corbierre, Muriel K. Physical Review Letters, Vol. 102, Issue 7 https://doi.org/10.1103/PhysRevLett.102.075702	journal	February 2009
Reduced Viscosity of the Free Surface in Entangled Polymer Melt Films Koga, Tadanori; Li, C.; Endoh, M. K. Physical Review Letters, Vol. 104, Issue 6 https://doi.org/10.1103/PhysRevLett.104.066101	journal	February 2010
Anisotropic de Gennes Narrowing in Confined Fluids Nygård, Kim; Buitenhuis, Johan; Kagias, Matias Physical Review Letters, Vol. 116, Issue 16 https://doi.org/10.1103/PhysRevLett.116.167801	journal	April 2016
Dynamic Scaling of Colloidal Gel Formation at Intermediate Concentrations Zhang, Qingteng; Bahadur, Divya; Dufresne, Eric M. Physical Review Letters, Vol. 119, Issue 17 https://doi.org/10.1103/PhysRevLett.119.178006	journal	October 2017
Coherent X-Ray Study of Fluctuations during Domain Coarsening Malik, A.; Sandy, A. R.; Lurio, L. B. Physical Review Letters, Vol. 81, Issue 26 https://doi.org/10.1103/PhysRevLett.81.5832	journal	December 1998
Universal Aging Features in the Restructuring of Fractal Colloidal Gels Cipelletti, Luca; Manley, S.; Ball, R. C. Physical Review Letters, Vol. 84, Issue 10 https://doi.org/10.1103/PhysRevLett.84.2275	journal	March 2000
Evolution of Particle-Scale Dynamics in an Aging Clay Suspension Bandyopadhyay, R.; Liang, D.; Yardimci, H. Physical Review Letters, Vol. 93, Issue 22 https://doi.org/10.1103/PhysRevLett.93.228302	journal	November 2004
X-ray photon correlation spectroscopy Shpyrko, Oleg G. Journal of Synchrotron Radiation, Vol. 21, Issue 5 https://doi.org/10.1107/S1600577514018232	journal	August 2014
Sub-microsecond-resolved multi-speckle X-ray photon correlation spectroscopy with a pixel array detector Zhang, Qingteng; Dufresne, Eric M.; Narayanan, Suresh Journal of Synchrotron Radiation, Vol. 25, Issue 5 https://doi.org/10.1107/S1600577518009074	journal	August 2018
Software tools for X-ray photon correlation and X-ray speckle visibility spectroscopy Abeykoon, Sameera K.; Zhang, Yugang; Dill, Eric D. 2016 New York Scientific Data Summit (NYSDS) https://doi.org/10.1109/NYSDS.2016.7747815	conference	August 2016
X-ray Photon Correlation Spectroscopy of Filler in Rubber Shinohara, Yuya; Kishimoto, Hiroyuki; Maejima, Taketo Japanese Journal of Applied Physics, Vol. 46, Issue No. 4 https://doi.org/10.1143/JJAP.46.L300	journal	March 2007
Evolution of dynamics and structure during formation of a cross-linked polymer gel Czakkel, O.; Madsen, A. EPL (Europhysics Letters), Vol. 95, Issue 2 https://doi.org/10.1209/0295-5075/95/28001	journal	June 2011

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