CHARACTERIZATION OF POLYMERS BY TMA. W.J. Sichina, National Marketing Manager

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PERKIN ELMER Polymers technical note CHARACTERIZATION OF POLYMERS BY W.J. Sichina, National Marketing Manager Thermomechanical analysis () is one of the important characterization techniques in the field of thermal analysis. With, the dimensional properties of a sample are measured as the sample is heated, cooled or held under isothermal conditions. The loading or force applied to the sample can be varied with. The technique is used to assess the following important properties of polymers: Softening temperatures or Tg(s) Melting temperatures Stress relief effects at Tg Coefficients of thermal expansion (CTE) Dimensional compatibilities of two or more different materials Onset of foaming Relative degree of cure of thermosets Composite delamination temperatures Percent shrinkages of films and fibers Shrinkage forces Effectiveness of cling of films Testing of coatings on metals, films, optical fibers and electrical wires Assessment of transverse versus machine orientational properties of films With the technique, a number of different probe configurations are offered in order to optimize the test conditions for a specific sample and/or application. The probes offered by Perkin-Elmer include expansion, penetration, compression, flexure, extension and dilatometry. Some of the probe geometries are represented in Figure 1.

Figure 1. probe configurations Expansion Penetration Compression Flexure The most commonly used probe is the expansion probe. This probe rests on the surface of the test specimen under low loading conditions. As the sample expands, during heating, the probe is pushed up and the resulting expansion of the sample is measured. Displayed in Figure 2 are the results obtained on an epoxy fiberglass printed circuit board sample at the glass transition temperature (Tg) using the expansion probe. Figure 2. Measurement of Tg of epoxy printed circuit board Expansion Tg = 121 C 30 Temperature ( C) 200

At the glass transition event, the epoxy matrix exhibits a significant change in slope due to an increase in its rate of expansion. The onset temperature of this change in expansion behavior is the Tg of the resin. is significantly more sensitive than DSC for the measurement of Tg of crosslinked or filled materials, such as composites. One of the benefits of using the expansion probe is that coefficients of thermal expansion (CTE) can be easily measured by. The CTE is a quantitative assessment of the expansion of a material over a temperature interval. When manufacturing products that contain two different materials, it is oftentimes critical to ensure that the materials will have CTE values that are identical to avoid the build-up of thermal stresses or to prevent leaks or component malfunctions. Displayed in Figure 3 are the CTE values measured on an epoxy printed circuit board below and above Tg. Figure 3. results on epoxy PCB showing assessment of coefficients of thermal expansion Below Tg, the printed circuit board has a CTE value of 50.5 µm/m C, while above Tg, the value of the CTE increases to 270.7 µm/m C. For electronic materials, it is important that the other associated components have similar expansion coefficients to prevent the build-up of thermal stresses during operation. For example, better product lifetimes of electronic flip-chip packaging can be obtained on solder joints by ensuring that the CTE values of the solder and the epoxy underfill are identical. Figure 3 also shows the effects of residual thermal stresses on the measurements. During the 1 st heating segment, the expansion results show the occurrence of an

undulation in its expansion behavior in the region near Tg. This reflects the release of stresses, which are frozen-in during processing. When the printed circuit board sample is cooled, and then reheated, a simple change in expansion rate is observed at Tg which indicates that the material is now free of thermal stresses or other thermal history related effects. The high sensitivity of the technique allows it to detect weak transitions that may not be observed by DSC. An example is the characterization of brake linings, which are highly filled and crosslinked. The expansion results displayed in Figure 4 demonstrates that the can detect the glass transition temperature associated with these highly filled materials. Figure 4. expansion results on brake linings Measurement of Tg of Brake Linings Expansion Mode Tg = 85 C Failed Tg = 93 C Passed 25 Temperature ( C) 150 The penetration probe provides another means of assessing glass transition temperatures. When performing measurements with the penetration probe, loading is added to the probe so that it moves down through the material as it softens. The penetration probe is useful for measuring the glass transitions of coatings on a substrate. Displayed in Figure 5 are the penetration results generated on a wire sample with two coatings. The wire is used to produce electrical motor coils and the inner coating prevents electrical contact between adjacent wires and the outer coating is used to bond the coil.

Figure 5. penetration probe results on electrical coil wire Tg1 = 128 C Penetration L Measurement of Tg s of Electrical Coil Wire Tg2 = 176 C Decomposition 25 Temperature ( C) 300 The penetration results show that the outer coating has its Tg at 128 C and that of the inner coating occurs at 176 C. The decomposition of the resin is observed at approximately 260 C. The penetration probe provides excellent data on the softening properties of thermoplastics. Shown in Figure 6 are the penetration results on crosslinked and non-crosslinked polyethylenes. The sample with crosslinking exhibits a smaller degree of penetration due to the higher viscosity in the liquid region above the melting point. Figure 6. penetration results on crosslinked and non-crosslinked polyethylene With Crosslinking Penetration No Crosslinking 30 Temperature ( C) 160

In the next applications example, a sample of foam blown polyethylene was characterized using the compression mode of the. The results are displayed in Figure 7. Figure 7. Characterization of LDPE foam by compression mode Softening (Melting) Penetration Foaming 40 Temperature ( C) 180 The results show that the LDPE sample undergoes a small amount of expansion between 40 and the melting temperature. At approximately 100 C, the sample melts and the lightly loaded probe penetrates the sample and a rapid decrease in the thickness of the sample is observed. A quasi-linear response is obtained in the viscous region above the melting point and the slope of this reflects the degree of crosslinking achieved by the resin. Upon further heating a large increase in the expansion of the polymer is observed and this reflects the swelling causes by the release of the nitrogen gas from the blowing agent. These results demonstrate that the results can provide valuable information on the melting temperature, relative crosslink density and foaming temperature. For the characterization of films and fibers, the extension mode yields excellent results. With the extension mode of analysis, the sample is clamped between two fixtures which then hangs in the sample tube. Displayed in Figure 8 are the extension results generated on a sample of polyester (PET) partially oriented yarn.

Figure 8. extension results on polyester partially oriented fibers Expansion Tg Melt Cold crystallization 25 Temperature ( C) 275 The polyester yarn sample undergoes its glass transition event at approximately 75 C as reflected by the large amount of shrinkage or contraction that occurs beginning at this temperature. With continued heating, the amorphous phase in the fibers undergoes cold crystallization, which tends to stabilize the properties of the fibers. As crystallization takes place, the fibers undergo elongation. As the sample temperature approaches 250 C, the crystalline phase of the PET fibers melts, and substantial elongation takes place. provides valuable characterization information on fibers and yarns including heat set or texturing temperatures, percent shrinkages, shrinkage forces and defect analysis. The properties of oriented films are best studied using the extension mode of the. In the next example, a sample of biaxially oriented high density polyethylene (HDPE) film was characterized by. Test specimens were cut in the machine and perpendicular directions (transverse) in order to study the effects of processing on the biaxially stretched film. Displayed in Figure 9 are the results generated on the biaxially oriented HDPE film in the machine and transverse orientations using the extension mode.

Figure 9. results on biaxially oriented HDPE film in machine and transverse orientations Machine direction Elongation Transverse direction 25 Temperature ( C) 150 In the transverse direction, the film sample expands slightly up to 133 C, where rapid shrinkage or contraction occurs due to the frozen-in orientation which has been imposed on the film in that orientation. At about 138 C, the film undergoes elongation due to the melting of the crystalline phase since the film is no longer able to support any load. In the machine direction, the film undergoes gradual expansion until sample melting occurs at 134 C, producing rapid elongation. The results demonstrate that the biaxially oriented film exhibits distinctly different shrinkage/elongation characteristics depending on how the sample is cut and mounted in the. There is apparently a high degree of orientation in the transverse direction as compared to the machine direction, due to the particular processing conditions employed in the production of the film. The Perkin Elmer 7 provides state-of-the-art performance for the characterization of the dimensional properties of materials. The instrument offers the following key features to provide the best possible results: High resolution (3 nanometer) strain detector for the measurement of even the smallest or most subtle dimensional changes Electromagnetic probe control (rather than less performing springs) which provides constant, load force regardless of sample dimensional changes Computer-controlled loading (or force application) which eliminates the use of weights, improving reproducibility of results

Temperature-controlled detector (LVDT) for the elimination of baseline variability and better accuracy and reproducibility Automated cooling capability using ACA (automated cooling accessory) for ease of use and improved subambient performance Wide temperature range (-170 to 1000 C) using a single furnace eliminating the need for time consuming furnace changes Multiple probe types (including expansion, penetration, compression, flexure, extension and dilatometry) to permit the successful analyses of a wide range of samples and applications One-touch automated probe control for simplifying probe positioning and to provide the highest possible reproducibility of results Summary provides valuable characterization information on the dimensional properties of a wide range of materials. Used either alone or in conjunction with other thermal analysis techniques (DSC, TGA, DMA or thermoconductivity), the technique provides a large amount of valuable information on polymers and other materials which is difficult or even impossible to obtain by other analytical techniques. offers a higher degree of sensitivity as compared to DSC for the detection of the Tg of highly filled or highly crosslinked materials, such as composites, printed circuit boards or brake linings. The state-of-the-art Perkin Elmer 7 provides outstanding results on a wide variety of materials and applications for both research as well as quality assurance uses. PERKIIN ELMER 761 Main Street Norwalk, CT 06859-0010 (800) 762-4000 (203) 762-4228 FAX www.perkin-elmer.com The Thermal Analysis Leader