Taking advantage of their inherent abrasion resistant, weather resistant, and outstanding mechanical strength, film-grade thermoplastic polyurethanes (TPU) are currently being used as paint protective films but are also being considered for paint replacement within the automotive industry. Special grades of TPU with shape memory behaviour offer an additional feature of self-healing to decorative coatings but there are concerns of shape fixity at service temperatures which are above their glass transition temperature (Tg).
In this study, the shape memory behaviour of a developmental TPU film with Tg around room temperature was investigated. In order to understand the shape memory behaviour, the TPU film was laminated to a rigid polymer substrate of either polypropylene (PP) or acrylonitrile butadiene styrene (ABS). Three different acrylic based pressure sensitive adhesives were tested to bond the film to the substrate, namely a commercial high shear strength transfer tape and two solvent based adhesives of high and low shear strength that were manually cast. The influence of the adhesive was given significant attention as a variable of study in this thesis.
The characterization of all the polymeric films and substrates was based on a series of thermo-mechanical tests (tensile test, stress relaxation test, DSC and DMA). The adhesives were characterized by lap-shear test, peel test, and parallel plate rheometry. The results of material characterization were used to support the analysis and interpretation of shape memory behaviour.
The TPU based laminate was deformed by a matched mold thermoforming process with a pair of arched matched molds. The recovery behaviour of formed samples was quantified with a newly designed measurement method and the results were reported as recovery ratio and recovery rate. During recovery, the surrounding temperature was considered to be an important variable. The recovery behaviour of specimens was investigated in a controlled environment at setpoint temperatures of 15oC, 45oC or 65oC. No shape memory effect was found at 15oC (below TPU’s Tg), and yet both recovery ratio and recovery rate increased with temperature, from 45oC to 65oC (both above the TPU’s Tg). Since the recovery process was related to the elastic response of the hard segment phase within the TPU, the recovery stress was strongly related to strain conditions. By varying the draw depth into the mold from 6 mm, to 10 mm or 12 mm (8.86%, 15.90% or 19.88% strain, respectively), the recovery measurement results showed that the shape memory effect was weaker with lower strain as less recovery stresses were generated in the TPU film. With the draw depth of 10 mm, the highest recovery ratio and recovery rate were observed, and yet an inexplicable decrease in the recovery ratio and recovery rate occurred as the draw depth increased further from 10mm to 12mm. In regards to the influence by a substrate, TPU/PP laminate showed a more significant recovery behaviour than TPU/ABS laminates at both 45oC and 65oC. The elastic modulus of the substrate was found to have a key role on the recovery process; the recovery nature of formed laminate decreased with stiffer substrate.
Three adhesives with differing rheological and adhesion properties were tested to bond the TPU film to a substrate. The formed laminates with “strongest” adhesive (transfer tape) in terms of stiffness and adhesion strength showed the highest recovery ratio/rate over laminates made with “weaker” solvent cast adhesives, at both 45oC and 65oC. A finite element analysis (FEA) was employed to simulate the stress transfer within a multilayer structure bonded by a viscoelastic adhesive layer of varying stiffness; the simulated result showed that the relatively low stiffness adhesive could reduce the stress transfer efficiency within layers of a laminate. It suggested that more recovery stresses were transferred from TPU to substrate with a stiffer adhesive layer (transfer tape) and hence increased the recovery ratio and recovery rate. Therefore, adhesive with relatively low stiffness and adhesion strength could be a better choice to reduce the recovery effect of TPU laminate after forming. However, TPU was found to slide at the unsealed edge of formed laminate when the solvent based adhesives were used; the sliding behavior reduced the recovery by releasing stored recovery stress. In the case of HS and LS adhesives at high temperature (65oC), cohesive failure was observed when the edge of specimen was sealed led to a higher bending moment thus increased the recovery ratio over 24 hours investigations. Therefore, adhesives of weaker shear strength do not necessarily overcome the nature of shape recovery by the TPU when formed part shape needs to be preserved. / Thesis / Master of Applied Science (MASc) / Nowadays, smart materials in particular shape-memory polymers have been widely used in the industrial and medical applications. Thermoplastic polyurethane (TPU) is one of the significant shape memory polymer groups. The two-phase morphology of a typical TPU gives a unique shape memory behaviour over a defined temperature range. However, this shape memory effect affects the shape fixity of formed TPU. In this study, a special-grade TPU film was laminated to a rigid polymer substrate using selected pressure sensitive adhesives (PSAs). In order to investigate the effect of adhesive layer on the shape memory behaviour of this TPU based laminate, three PSAs with varying properties were applied. The laminate was thermoformed, quenched and processed in a temperature-controlled chamber with a designed recovery measurement method. The shape memory effect was observed at temperatures above the transition temperature of TPU, and this recovery effect was enhanced at higher temperature. Furthermore, the mechanical property of the substrate material was considered as a key factor on the recovery behaviour of the laminate; the recovery of the formed laminate was restricted with a stiffer substrate. The most significant discovery from the recovery results indicated that the shape memory effect was reduced with the adhesive with relatively low adhesion strength, however, the delamination of the laminate occurs with weaker adhesives.
| Identifer | oai:union.ndltd.org:mcmaster.ca/oai:macsphere.mcmaster.ca:11375/18183 |
| Date | 11 1900 |
| Creators | XU, WENSEN |
| Contributors | THOMPSON, MICHAEL, Chemical Engineering |
| Source Sets | McMaster University |
| Language | English |
| Detected Language | English |
| Type | Thesis |
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