• Korea-Australia Rheology Journal
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• v.14 no.1
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• pp.25-32
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• 2002

We report the first steps of a collaborative project between the University of Queensland, Polyflow, Michelin, SK Chemicals, and RMIT University, on simulation, validation and application of a recently introduced constitutive model designed to describe branched polymers. Whereas much progress has been made on predicting the complex flow behaviour of many - in particular linear - polymers, it sometimes appears difficult to predict simultaneously shear thinning and extensional strain hardening behaviour using traditional constitutive models. Recently a new viscoelastic model based on molecular topology, was proposed by McLeish and carson (1998). We explore the predictive power of a differential multi-mode version of the porn-pom model for the flow behaviour of two commercial polymer melts: a (long-chain branched) low-density polyethylene (LDPE) and a (linear) high-density polyethylene (HDPE). The model responses are compared to elongational recovery experiments published by Langouche and Debbaut (19c99), and start-up of simple shear flow, stress relaxation after simple and reverse step strain experiments carried out in our laboratory.

• Korea-Australia Rheology Journal
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• v.14 no.1
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• pp.33-45
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• 2002

Recent results obtained for the port-pom model and the constitutive equations with time-strain separability are examined. The time-strain separability in viscoelastic systems Is not a rule derived from fundamental principles but merely a hypothesis based on experimental phenomena, stress relaxation at long times. The violation of separability in the short-time response just after a step strain is also well understood (Archer, 1999). In constitutive modeling, time-strain separability has been extensively employed because of its theoretical simplicity and practical convenience. Here we present a simple analysis that verifies this hypothesis inevitably incurs mathematical inconsistency in the viewpoint of stability. Employing an asymptotic analysis, we show that both differential and integral constitutive equations based on time-strain separability are either Hadamard-type unstable or dissipative unstable. The conclusion drawn in this study is shown to be applicable to the Doi-Edwards model (with independent alignment approximation). Hence, the Hadamardtype instability of the Doi-Edwards model results from the time-strain separability in its formulation, and its remedy may lie in the transition mechanism from Rouse to reptational relaxation supposed by Doi and Edwards. Recently in order to describe the complex rheological behavior of polymer melts with long side branches like low density polyethylene, new constitutive equations called the port-pom equations have been derived in the integral/differential form and also in the simplifled differential type by McLeish and carson on the basis of the reptation dynamics with simplifled branch structure taken into account. In this study mathematical stability analysis under short and high frequency wave disturbances has been performed for these constitutive equations. It is proved that the differential model is globally Hadamard stable, and the integral model seems stable, as long as the orientation tensor remains positive definite or the smooth strain history in the flow is previously given. However cautious attention has to be paid when one employs the simplified version of the constitutive equations without arm withdrawal, since neglecting the arm withdrawal immediately yields Hadamard instability. In the flow regime of creep shear flow where the applied constant shear stress exceeds the maximum achievable value in the steady flow curves, the constitutive equations exhibit severe instability that the solution possesses strong discontinuity at the moment of change of chain dynamics mechanisms.