Stress growth and relaxation of a molten polyethylene in a modified weissenberg rheogoniometer

Abstract

AbstractA Weissenberg rheogoniometer was modified1‐3 to improve sample temperature uniformity and constancy (to within ±0.5°C) and to give a quicker response to normal thrust changes (estimated gap change ≤0.1 μm/kg thrust; gap angle = 8.046°; gap radius = 1.2 cm; servomechanism replaced by an open‐loop cantilever spring of 10 kg/μm stiffness). Low‐density polyethylenes (IUPAC samples A and C, melt index at 190°C = 1.6) at 150°C were used in step‐function shear rate experiments. Inspection of marked sectors in the samples showed substantial uniformity of shear at values of Ṡ = 0.1, 2, and 5 sec−1; for Ṡ = 10 sec−1 and S ≤ 2 shear units (S = Ṡt), the shear was highly nonuniform at and near the free boundary. Using selected premolded samples A, scatter in seven replicate tests at Ṡ = 1.0 sec−1 did not exceed ±6% for N1(t) and ±5% for σ(t) (N1 = primary normal stress difference; σ = shear stress; t = time of deformation from the initiation of experiment at zero time). N1(t) and σ(t) data agreed with Meissner's1; for Ṡ = 0.1, 2.0, 5.0, and 10.0 sec−1, torque maxima occurred at S = 6 shear units, and thrust maxima occurred in the range of 10 to 20 shear units. σ(t) and N1(t) data do not satisfy the van Es and Christensen4 test for rubber‐like liquids with strain rate invariants included in the memory function. On cessation of shear (after a shear strain S at constant shear rate Ṡ), initial values of −dσ(t)/dt and −dN1(t)/dt were found to depend strongly on S, in some cases passing through maxima as S was increased. After shearing at Ṡ = 0.1 sec−1 for 500 sec, such that stresses became constant, stress relaxation data satisfied Yamamoto's5 equation of dN1(t)/dt = −2Ṡσ(t).