Influence of filler/matrix interactions on resin/hardener stoichiometry, molecular dynamics, and particle dispersion of silicon nitride/epoxy nanocomposites
Source abstract
Abstract
The addition of nanofillers can have a significant influence on the resin stoichiometry of thermosetting polymer systems. Based on differential scanning calorimetry (DSC) results, it is estimated that the inclusion of 2 and 5 wt% of silicon nitride nanofiller displaces the resin/hardener stoichiometry of an epoxy/amine network by 6.5 and 18%, respectively. Dielectric spectroscopy results confirm the above findings, in that the spectra of the nanocomposite samples were found to be equivalent to the spectra of unfilled samples when the above stoichiometric effect was taken into account. Therefore, this study provides clear evidence that the presence of a nanofiller can directly and significantly affect the curing process of an epoxy network. Consequently, this should always be considered when introducing nanofillers into thermosetting matrices. These results indicate the presence of covalent bonding between the nanoparticles and the surrounding polymer and, therefore, provide an opportunity to explore the influence of this bonding on the molecular dynamics of the polymer layer around the particles. However, the obtained DSC and dielectric spectroscopy results suggest that, in the system considered here, either the covalent bonding does not have an appreciable influence on the segmental dynamics of the polymer, as revealed by these techniques, or that the thickness of the affected layer is less than 1 nm and therefore too small to be distinguished from experimental uncertainties.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: High voltage insulation and dielectric phenomena · Polymer Nanocomposites and Properties · Dielectric materials and actuators
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (61)
Show source-provided references
1. Li Y, Zhang B, Pan X (2008) Preparation and characterization of PMMA–kaolinite intercalation composites. Compos Sci Technol 68(9):1954–1961. https://doi.org/10.1016/j.compscitech.2007.04.00310.1016/j.compscitech.2007.04.003 ↗
2. Miwa Y, Drews AR, Schlick S (2006) Detection of the direct effect of clay on polymer dynamics: the case of spin-labeled poly(methyl acrylate)/clay nanocomposites studied by ESR, XRD, and DSC. Macromolecules 39(9):3304–3311. https://doi.org/10.1021/ma060096310.1021/ma0600963 ↗
3. Virtanen S, Krentz TM, Nelson JK, Schadler LS, Bell M, Benicewicz B, Hillborg H, Zhao S (2014) Dielectric breakdown strength of epoxy bimodal-polymer-brush-grafted core functionalized silica nanocomposites. IEEE Trans Dielectr Electr Insul 21(2):563–570. https://doi.org/10.1109/tdei.2014.00441510.1109/tdei.2014.004415 ↗
4. Alhabill FN, Ayoob R, Andritsch T, Vaughan AS (2017) Effect of resin/hardener stoichiometry on electrical behavior of epoxy networks. IEEE Trans Dielectr Electr Insul (in press)10.1109/TDEI.2017.006828 ↗
5. Cheng G, Qian J, Tang Z, Ding G, Zhu J (2015) Dispersion stability of Si3N4 nano-particles modified by gamma-methacryloxypropyl trimethoxy silane (MAPTMS) in organic solvent. Ceram Int 41(1):1879–1884. https://doi.org/10.1016/j.ceramint.2014.09.01310.1016/j.ceramint.2014.09.013 ↗
6. Cerovic LS, Milonjic SK, Bahloul-Hourlier D, Doucey B (2002) Surface properties of silicon nitride powders. Colloids Surf A 197(1–3):147–156. https://doi.org/10.1016/s0927-7757(01)00863-910.1016/s0927-7757(01)00863-9 ↗
7. Busca G, Lorenzelli V, Baraton MI, Quintard P, Marchand R (1986) FT-IR characterization of silicon nitride Si3N4 and silicon oxynitride SI2ON2 surfaces. J Mol Struct 143:525–528. https://doi.org/10.1016/0022-2860(86)85316-910.1016/0022-2860(86)85316-9 ↗
8. Tai YL, Qian JS, Miao JB, Xia R, Zhang YC, Yang ZG (2012) Preparation and characterization of Si3N4/SBR nanocomposites with high performance. Mater Des 34:522–527. https://doi.org/10.1016/j.matdes.2011.05.00210.1016/j.matdes.2011.05.002 ↗
9. Li YL, Liang Y, Zheng F, Xiao K, Hu ZQ, Shun T (1995) Fourier transformation infrared investigation of surface oxidation of ultrafine Si3N4 powders. J Mater Sci Lett 14(10):713–715
10. Baller J, Thomassey M, Ziehmer M, Sanctuary R (2011) The catalytic influence of alumina nanoparticles on epoxy curing. Thermochim Acta 517(1–2):34–39. https://doi.org/10.1016/j.tca.2011.01.02910.1016/j.tca.2011.01.029 ↗
11. Supova M, Martynkova GS, Barabaszova K (2011) Effect of nanofillers dispersion in polymer matrices: a review. Sci Adv Mater 3(1):1–25. https://doi.org/10.1166/sam.2011.113610.1166/sam.2011.1136 ↗
12. Starr FW, Douglas JF, Glotzer SC (2003) Origin of particle clustering in a simulated polymer nanocomposite and its impact on rheology. J Chem Phys 119(3):1777–1788. https://doi.org/10.1063/1.158009910.1063/1.1580099 ↗
13. Sekhavat Pour Z, Ghaemy M (2014) Fabrication and characterization of superparamagnetic nanocomposites based on epoxy resin and surface-modified γ-Fe2O3 by epoxide functionalization. J Mater Sci 49(12):4191–4201. https://doi.org/10.1007/s10853-014-8114-610.1007/s10853-014-8114-6 ↗
14. Ribeiro H, Silva WM, Rodrigues M-TF, Neves JC, Paniago R, Fantini C, Calado HDR, Seara LM, Silva GG (2013) Glass transition improvement in epoxy/graphene composites. J Mater Sci 48(22):7883–7892. https://doi.org/10.1007/s10853-013-7478-310.1007/s10853-013-7478-3 ↗
15. He L, Chuang W, Zihao G, Haoran W, Yuxuan Z, Rui H (2016) Zongren P (2016) Effects of silane coupling agents on the electrical properties of silica/epoxy nanocomposites. IEEE Int Conf Dielectr (ICD) 2:1036–1039. https://doi.org/10.1109/ICD.2016.754779510.1109/ICD.2016.7547795 ↗
16. Zhang L, Zhou YX, Cui XY, Sha YC, Le TH, Ye Q, Tian JH (2014) Effect of nanoparticle surface modification on breakdown and space charge behavior of XLPE/SiO2 nanocomposites. IEEE Trans Dielectr Electr Insul 21(4):1554–1564. https://doi.org/10.1109/tdei.2014.00436110.1109/tdei.2014.004361 ↗
17. Roy M, Nelson JK, MacCrone RK, Schadler LS (2007) Candidate mechanisms controlling the electrical characteristics of silica/XLPE nanodielectrics. J Mater Sci 42(11):3789–3799. https://doi.org/10.1007/s10853-006-0413-010.1007/s10853-006-0413-0 ↗
18. Tanaka T, Kozako M, Fuse N, Ohki Y (2005) Proposal of a multi-core model for polymer nanocomposite dielectrics. IEEE Trans Dielectr Electr Insul 12(4):669–681. https://doi.org/10.1109/tdei.2005.151109210.1109/tdei.2005.1511092 ↗
19. Li K, Li Y, Lian QS, Cheng J, Zhang JY (2016) Influence of cross-linking density on the structure and properties of the interphase within supported ultrathin epoxy films. J Mater Sci 51(19):9019–9030. https://doi.org/10.1007/s10853-016-0155-610.1007/s10853-016-0155-6 ↗
20. Andritsch T, Kochetov R, Morshuis PHF, Smit JJ (2011) Proposal of the polymer chain alignment model. In: Annual report conference on electrical insulation and dielectric phenomena, 16–19 Oct 2011. pp 624–627. https://doi.org/10.1109/CEIDP.2011.623273410.1109/CEIDP.2011.6232734 ↗
21. Tsekmes IA, Kochetov R, Morshuis PHF, Smit JJ (2014) A unified model for the permittivity and thermal conductivity of epoxy based composites. J Phys D Appl Phys 47(41):415502. https://doi.org/10.1088/0022-3727/47/41/41550210.1088/0022-3727/47/41/415502 ↗
22. Raetzke S, Kindersberger J (2010) Role of interphase on the resistance to high-voltage arcing, on tracking and erosion of silicone/SiO2 nanocomposites. IEEE Trans Dielectr Electr Insul 17(2):607–614. https://doi.org/10.1109/TDEI.2010.544811810.1109/TDEI.2010.5448118 ↗
23. Praeger M, Andritsch T, Swingler SG, Vaughan AS (2014) A simple theoretical model for the bulk properties of nanocomposite materials. In: Paper presented at the 2014 IEEE conference on electrical insulation and dielectric phenomena10.1109/CEIDP.2014.6995750 ↗
24. Kochetov R, Andritsch T, Morshuis PHF, Smit JJ (2012) Anomalous behaviour of the dielectric spectroscopy response of nanocomposites. IEEE Trans Dielectr Electr Insul 19(1):107–117. https://doi.org/10.1109/TDEI.2012.614850810.1109/TDEI.2012.6148508 ↗
25. Kurimoto M, Okubo H, Kato K, Hanai M, Hoshina Y, Takei M, Hayakawa N (2010) Permittivity characteristics of epoxy/alumina nanocomposite with high particle dispersibility by combining ultrasonic wave and centrifugal force. IEEE Trans Dielectr Electr Insul 17(4):1268–1275. https://doi.org/10.1109/TDEI.2010.553969910.1109/TDEI.2010.5539699 ↗
26. Zhou W, Yu D (2013) Fabrication, thermal, and dielectric properties of self-passivated Al/epoxy nanocomposites. J Mater Sci 48(22):7960–7968. https://doi.org/10.1007/s10853-013-7606-010.1007/s10853-013-7606-0 ↗
27. Starr FW, Schrøder TB, Glotzer SC (2002) Molecular dynamics simulation of a polymer melt with a nanoscopic particle. Macromolecules 35(11):4481–4492. https://doi.org/10.1021/ma010626p10.1021/ma010626p ↗
28. Desai T, Keblinski P, Kumar SK (2005) Molecular dynamics simulations of polymer transport in nanocomposites. J Chem Phys 122(13):134910. https://doi.org/10.1063/1.187485210.1063/1.1874852 ↗
29. Simone N, Emmanouil G, Nicholas BT (2017) Glass transition of polymers in bulk, confined geometries, and near interfaces. Rep Prog Phys 80(3):036602. https://doi.org/10.1088/1361-6633/aa528410.1088/1361-6633/aa5284 ↗
30. Fedtke M, Domaratius F (1986) Curing of epoxide-resins by anhydrides of dicarboxylic-acids: model reactions. Polym Bull 15(1):13–1910.1007/BF00263486 ↗
31. Matejka L, Lovy J, Pokorny S, Bouchal K, Dusek K (1983) Curing epoxy-resins with anhydrides: model reactions and reaction-mechanism. J Polym Sci Part a: Polym Chem 21(10):2873–2885. https://doi.org/10.1002/pol.1983.17021100310.1002/pol.1983.170211003 ↗
32. Nguyen VT, Vaughan AS, Lewin PL, Krivda A (2015) The effect of resin stoichiometry and nanoparticle addition on epoxy/silica nanodielectrics. IEEE Trans Dielectr Electr Insul 22(2):895–905. https://doi.org/10.1109/tdei.2014.00478510.1109/tdei.2014.004785 ↗
33. Rittigstein P, Torkelson JM (2006) Polymer-nanoparticle interfacial interactions in polymer nanocomposites: confinement effects on glass transition temperature and suppression of physical aging. J Polym Sci Part B: Polym Phys 44(20):2935–2943. https://doi.org/10.1002/polb.2092510.1002/polb.20925 ↗
34. Bansal A, Yang HC, Li CZ, Cho KW, Benicewicz BC, Kumar SK, Schadler LS (2005) Quantitative equivalence between polymer nanocomposites and thin polymer films. Nat Mater 4(9):693–698. https://doi.org/10.1038/nmat144710.1038/nmat1447 ↗
35. Bignotti F, Pandini S, Baldi F, De Santis R (2011) Effect of the resin/hardener ratio on curing, structure and glass transition temperature of nanofilled epoxies. Polym Compos 32(7):1034–1048. https://doi.org/10.1002/pc.2112010.1002/pc.21120 ↗
36. Yeung C, Vaughan AS (2016) On the effect of nanoparticle surface chemistry on the electrical characteristics of epoxy-based nanocomposites. Polymers 8(4):126. https://doi.org/10.3390/polym804012610.3390/polym8040126 ↗
37. Sargsyan A, Tonoyan A, Davtyan S, Schick C (2007) The amount of immobilized polymer in PMMA SiO2 nanocomposites determined from calorimetric data. Eur Polym J 43(8):3113–3127. https://doi.org/10.1016/j.eurpolymj.2007.05.01110.1016/j.eurpolymj.2007.05.011 ↗
38. Moll J, Kumar SK (2012) Glass transitions in highly attractive highly filled polymer nanocomposites. Macromolecules 45(2):1131–1135. https://doi.org/10.1021/ma202218x10.1021/ma202218x ↗
39. Siddabattuni S, Schuman TP, Dogan F (2013) Dielectric properties of polymer-particle nanocomposites influenced by electronic nature of filler surfaces. ACS Appl Mater Interfaces 5(6):1917–1927. https://doi.org/10.1021/am303023910.1021/am3030239 ↗
40. Preghenella M, Pegoretti A, Migliaresi C (2005) Thermo-mechanical characterization of fumed silica-epoxy nanocomposites. Polymer 46(26):12065–12072. https://doi.org/10.1016/j.polymer.2005.10.09810.1016/j.polymer.2005.10.098 ↗
41. Umboh MK, Adachi T, Oishi K, Higuchi M, Major Z (2013) Mechanical properties of nano-silica particulate-reinforced epoxy composites considered in terms of crosslinking effect in matrix resins. J Mater Sci 48(15):5148–5156. https://doi.org/10.1007/s10853-013-7300-210.1007/s10853-013-7300-2 ↗
42. Blum FD, Lin W-Y, Porter CE (2003) Dynamics of adsorbed poly(methyl acrylate) and poly(methyl methacrylate) on silica. Colloid Polym Sci 281(3):197–202. https://doi.org/10.1007/s00396-002-0795-810.1007/s00396-002-0795-8 ↗
43. Harton SE, Kumar SK, Yang HC, Koga T, Hicks K, Lee E, Mijovic J, Liu M, Vallery RS, Gidley DW (2010) Immobilized polymer layers on spherical nanoparticles. Macromolecules 43(7):3415–3421. https://doi.org/10.1021/ma902484d10.1021/ma902484d ↗
44. Prasad A, Grover T, Basu S (2010) Coarse–grained molecular dynamics simulation of cross–linking of DGEBA epoxy resin and estimation of the adhesive strength. Int J Eng Sci Technol 2(4):17–3010.4314/ijest.v2i4.59196 ↗
45. Holt AP, Griffin PJ, Bocharova V, Agapov AL, Imel AE, Dadmun MD, Sangoro JR, Sokolov AP (2014) Dynamics at the polymer/nanoparticle interface in poly(2-vinylpyridine)/silica nanocomposites. Macromolecules 47(5):1837–1843. https://doi.org/10.1021/ma500031710.1021/ma5000317 ↗
46. Bershtein V, Gun’ko V, Egorova L, Guzenko N, Pakhlov E, Ryzhov V, Zarko V (2009) Well-defined silica core-poly(vinyl pyrrolidone) shell nanoparticles: interactions and multi-modal glass transition dynamics at interfaces. Polymer 50(3):860–871. https://doi.org/10.1016/j.polymer.2008.12.02410.1016/j.polymer.2008.12.024 ↗
47. Chen L, Zheng K, Tian XY, Hu K, Wang RX, Liu C, Li Y, Cui P (2010) Double glass transitions and interfacial immobilized layer in in-situ-synthesized poly(vinyl alcohol)/silica nanocomposites. Macromolecules 43(2):1076–1082. https://doi.org/10.1021/ma901267s10.1021/ma901267s ↗
48. Chouhan DK, Rath SK, Kumar A, Alegaonkar PS, Kumar S, Harikrishnan G, Patro TU (2015) Structure-reinforcement correlation and chain dynamics in graphene oxide and Laponite-filled epoxy nanocomposites. J Mater Sci 50(22):7458–7472. https://doi.org/10.1007/s10853-015-9305-510.1007/s10853-015-9305-5 ↗
49. Jordan C, Galy J, Pascault JP (1992) Measurement of the extent of reaction of an epoxy-cycloaliphatic amine system and influence of the extent of reaction on its dynamic and static mechanical-properties. J Appl Polym Sci 46(5):859–871. https://doi.org/10.1002/app.1992.07046051310.1002/app.1992.070460513 ↗
50. Soles CL, Yee AF (2000) A discussion of the molecular mechanisms of moisture transport in epoxy resins. J Polym Sci Part B: Polym Phys 38(5):792–802. https://doi.org/10.1002/(sici)1099-0488(20000301)38:5<792:aid-polb16>3.0.co;2-h10.1002/(sici)1099-0488(20000301)38:5<792::aid-polb16>3.0.co;2-h ↗
51. Kosmidou TV, Vatalis AS, Delides CG, Logakis E, Pissis P, Papanicolaou GC (2008) Structural, mechanical and electrical characterization of epoxy-amine/carbon black nanocomposites. Express Polym Lett 2(5):364–372. https://doi.org/10.3144/expresspolymlett.2008.4310.3144/expresspolymlett.2008.43 ↗
52. Panaitescu DM, Vuluga Z, Notingher PV, Nicolae C (2013) The effect of poly styrene-b-(ethylene-co-butylene)-b-styrene on dielectric, thermal, and morphological characteristics of polypropylene/silica nanocomposites. Polym Eng Sci 53(10):2081–2092. https://doi.org/10.1002/pen.2347510.1002/pen.23475 ↗
53. Hui L, Schadler LS, Nelson JK (2013) The influence of moisture on the electrical properties of crosslinked polyethylene/silica nanocomposites. IEEE Trans Dielectr Electr Insul 20(2):641–653. https://doi.org/10.1109/TDEI.2013.650876810.1109/TDEI.2013.6508768 ↗
54. Couderc H, Frechette M, Savoie S, Reading M, Vaughan AS (2012) Dielectric and thermal properties of boron nitride and silica epoxy composites. In: Conference record of the 2012 IEEE international symposium on electrical insulation (Isei), pp 64–6810.1109/ELINSL.2012.6251427 ↗
55. Hosier IL, Praeger M, Vaughan AS, Swingler SG (2015) Electrical properties of polymer nano-composites based on oxide and nitride fillers. IEEE Electr Insul Conf, pp 438–441. https://doi.org/10.1109/ICACACT.2014.722351510.1109/ICACACT.2014.7223515 ↗
56. Hosier IL, Praeger M, Vaughan AS, Swingler SG (2017) The effects of water on the dielectric properties of silicon-based nanocomposites. IEEE Trans Nanotechnol 16(2):169–179. https://doi.org/10.1109/TNANO.2016.264281910.1109/TNANO.2016.2642819 ↗
57. Alhabill FN, Andritsch T, Vaughan AS (2017) Moisture absorption behavior in silicon nitride epoxy nanocomposites. IEEE electrical insulation conference (EIC), 2011, pp 471–474. https://doi.org/10.1109/EIC.2017.800463810.1109/EIC.2017.8004638 ↗
58. Shukla DK, Parameswaran V (2007) Epoxy composites with 200 nm thick alumina platelets as reinforcements. J Mater Sci 42(15):5964–5972. https://doi.org/10.1007/s10853-006-1110-810.1007/s10853-006-1110-8 ↗
59. Qiang D, He M, Chen G, Andritsch T (2015) Influence of nano-SiO2 and BN on space charge and AC/DC performance of epoxy nanocomposites. In: IEEE electrical insulation conference, pp 492–495. https://doi.org/10.1109/ICACACT.2014.722351910.1109/ICACACT.2014.7223519 ↗
60. Marx P, Wanner A, Zhang Z, Jin H, Tsekmes I-A, Smit J, Kern W, Wiesbrock F (2017) Effect of interfacial polarization and water absorption on the dielectric properties of epoxy-nanocomposites. Polymers 9(6):19510.3390/polym9060195 ↗
61. Xu GC, Wang J, Ji XL, Xiong JY, Li F (2007) Effect of nano-silicon nitride on the mechanical and electric properties of polypropylene nanocomposite. J Compos Mater 41(18):2213–2223. https://doi.org/10.1177/002199830707418510.1177/0021998307074185 ↗