Measurement and prediction of LDPE/CO2 solution viscosity

• Published in: Polymer engineering and science Vol. 42; no. 11; pp. 2234 - 2245
• Main Authors: Areerat, Surat, Nagata, Takefumi, Ohshima, Masahiro
• Format: Journal Article
• Language: English
• Published: Hoboken Wiley Subscription Services, Inc., A Wiley Company 01.11.2002; Wiley Subscription Services
• Subjects: Applied sciences; Exact sciences and technology; Organic polymers; Physicochemistry of polymers; Properties and characterization; Rheology and viscoelasticity; Viscosity; Molten state; Stress strain relation; Carbon dioxide; Solubility; Free volume; Experimental study; Dissolution; Gas liquid equilibrium; Low density ethylene polymer; Supercritical process; Rheological properties; Interaction parameter
• ISSN: 0032-3888; 1548-2634
• DOI: 10.1002/pen.11113

When CO2 is dissolved into a polymer, the viscosity of the polymer is drastically reduced. In this paper, the melt viscosities of low‐density polyethylene (LDPE)/supercritical CO2 solutions were measured with a capillary rheometer equipped at a foaming extruder, where CO2 was injected into a middle of its barrel and dissolved into the molten LDPE. The viscosity measurements were performed by varying the content of CO2 in the range of 0 to 5.0 wt% and temperature in the range of 150°C to 175°C, while monitoring the dissolved CO2 concentration on‐line by Near Infrared spectroscopy. Pressures in the capillary tube were maintained higher than an equilibrium saturation pressure so as to prevent foaming in the tube and to realize single‐phase polymer/CO2 solutions. By measuring the pressure drop and flow rate of polymer running through the tube, the melt viscosities were calculated. The experimental results indicated that the viscosity of LDPE/CO2 solution was reduced to 30% of the neat polymer by dissolving CO2 up to 5.0 wt% at temperature 150°C. A mathematical model was proposed to predict viscosity reduction owing to CO2 dissolution. The model was developed by combining the Cross‐Carreau model with Doolittle's equation in terms of the free volume concept. With the Sanchez‐Lacombe equation of state and the solubility data measured by a magnetic suspension balance, the free volume fractions of LDPE/CO2 solutions were calculated to accommodate the effects of temperature, pressure and CO2 content. The developed model can successfully predict the viscosity of LDPE/CO2 solutions from PVT data of the neat polymer and CO2 solubility data.