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Experimental Study of LDPE Melting in a Twin Screw Extruder using On-Line Visualization and Axial Pressure and Temperature Measurements

Mark D. Wetzel, E. I. du Pont de Nemours and Co., Inc.

This paper is also available in pdf format via download here: BEST PAPER 2002.pdf

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Abstract

The melting of polymers in a twin-screw (T/S)extruder is an important operation in many industrial processes. Recent research by Shih, Gogos, Geng and others has identified the physical phenomena that take place during the phase transition. This paper describes an experimental study of Low Density Polyethylene (LDPE) melting in a corotating, intermeshing T/S extruder using on-line visualization and axial scanning of pressure and temperature techniques. The LDPE melting sequence observed included solid transportin a partially filled screw channel with conductive heating, compaction, pellet deformation, and viscous energy dissipation in the melt with un-melted solids. The effects of throughput (Q) and screw rotational speed (N) are examined. Low and high Q/N ratios have significantly different axial pressure profiles.

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Introduction

Twin-screw extruders are used in the plastics, food and allied industries to perform a variety of critical unit operations. Unit steps on a modular screw configuration include solid transport, melting, mixing, reaction, degassing and melt pumping. The melting function can consume the majority of mechanical energy input by the rotating screws.

Until recently, little was known about the melting process. Shih (1)described four fundamental steps in the melting of semi-crystalline polymers during compounding in a batch mixer using on-line visualization. Recently, Gogos and Kim (2, 3, 4) identified similar steps in the melting sequence in the T/S extruder using carcass analysis from samples extracted from the screws. These key steps, from an energy input perspective are: 1. conductive heating in a partially-filled screw channel, 2. compaction and frictional heating in a fully-filled zone, 3. bulk plastic deformation (PED) and lubrication by the first formation of the melt phase 4. viscous energy dissipation (VED) in the liquid phase in the presence of un-melted solids with heat transfer into the solid phase, and 5. energy dissipation in the melt after the completion of the phase transformation (viscous heating).

Curry (5) examined the role of heat transfer from the barrel during melting in the compaction, PED and VED steps. Other researchers, including Potente (6) and Vergnes (7), have modeled melting using the VED and heat transfer mechanisms. In the current work, an experimental study was conducted in a T/S extruder running Low Density Polyethylene (LDPE) to quantify the axial melting profile and relative contributions of each step in the sequence.

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Experiment

McCullough (8) and Christiano (9) used a sliding barrel mechanism to generate dynamic axial and radial pressure scans in the filled liquid m ixing zone of a T/S extruder. Geng and Zhu (10) used a set of barrels fitted with glass windows contoured to the apex region to visualize solid transport and melting of HDPE in a T/S extruder. In this study, a Coperion W & P ZSK-40m m T/S extruder was fitted with a barrel slide device to enable axial movementof the barrels over the screws during a polymer compounding operation. The entire melting zone was examined with an on-line scanning method using four pressure transducers, a flush-wall infrared melt temperature probe (IR-TC) and one glass window as shown in Fig. 1. Pressure probes and the IR-TC were mounted in a spacer plate upstream of the barrel containing the glass window. Probes were located at several radial locations with tips mounted perpendicular and flush to the barrel surface. Two pressure probes were located near the apex region on the up-turning and down-turning screws. The glass window was contoured to the barrel shape in the apex region, with a slightincrease in clearance to preventthe screws from contacting the surface. The window provided a 30m m axial direction by 40m m wide view port into the extruder. A standard m elting zone screw configuration wasused as shown in Fig 1. A solid conveying region used 60m m followed by 40m m lead forward pum ping elem ents. Tw o forward 45o-stagger kneading blocks backed by a 40m m lead reverse pum ping elem ent constituted the working section. A short melt conveying zone was placed near the end of the screw. The system was set up to run in an opendischarge m ode. For each operating state, the slide was started in the retracted (X=0mm) position. A setofsteady state and dynam ic m easurem ents w ere recorded along with video images. Probe signals were recorded at 200 sam - ples/sec (though an elliptic anti-aliasing filter with 80hz cutoff frequency) for a 60 second duration. Allpressure probe signals were averaged to produce a single value at each axial location. Video was recorded a 30 fram es per second using standard equipm ent. The barrel slidewasthen m oved 10 or20m m toward the discharge. The system was allowed to stabilize and data were recorded again. The m easurem ents were repeated until the probes were positioned beyond the reverse pum ping elem ent. The test cycle was run for the operating conditions listed in Table 1. Low throughput (Q) and screw speed (N) states were selected so that the video equipm ent could capture the m otion of the material in the window. The polym er used in the experiments was Low Density Polyethylene (LDPE) Petrothene NA from Quantum Chemical.The melting point is between 104 and 115oC, the M elt Index (M I) is 7.0 and the m eltdensityis0.918 gm /cc. Pelletswere half-spheres with a diam eter of approximately 4.0 to 4.5mm.

Discussion of Results Steady-State M easurem ents Five melting states were run atseveralthroughputsand screw speeds as show n in Table 1. Steady state energy input, feed tem perature and extrudate m elt tem peratures are listed. M elt tem peratures were obtained with a hand-held thermocoupleimmersed into the molten polym er and a noncontact infrared sensor. As throughput is increased atconstant screw speed (120RPM ), specific energy inputand m elt tem peratures are decreased as expected. At constant throughput and increasing screw speed,the specificenergy decreases at 90RPM before increasing at120RPM . M elt TC m easurem entsand IR surface tem peratures move in opposite directions. The steady-state data is not sufficient to quantify changes in melting perform ance with sm allchanges in operating conditions. Visualizing M elting Sequence Figs 2a and 2b show the m elting sequence observed through the glass window at 27kg/hr (60lb/hr) /60RPM . In the partially filled solid conveying zone, the predom inant flow m echanism w as axial displacem ent. Some pellets did move from screw to screw in the figure-8 channel path. A sm allam ountof liquid film was formed on the surface of the glass indicating that som e m elting occurred by conductive heating from the barrel walls. A t the X=20m m slide position (window location W =110m m ) the screw channelwas fully filled and solids flow shifted to the figure-8 channel direction. This state represented a highly filled m ode where the screw channel filled well upstream of the firstkneading block disk. A t X=40mm thefullyfilled solid agglom eration is underwent deformation. At X=60m m deformation continued and a m eltphase appeared in the m atrix, indicating the lubrication step. Islands ofun-melted solids in molten polym erappeared by X=100m m . The VED m elting m ode dom inated and continued for the rem aining m elting zone length. There was evidence of localized deformation and squeezing flow in the nip region as the kneading block volum e was com pressed, but pellets slipped axially to theadjacent channels in the downstream and upstream disks. O ver the reverse pum ping elem ent at X=160m m therewasasignificant am ount of un-melted solids. The downstream portion of the reverse elem ent was not filled atthe interface with the forward conveying bushing. Un-meltwasobserved at the screw tip.

The visualization for a low-fill state, 27kg/hr (60lb/hr) at 90RPM show ed that a slight change in screw speed had a large effecton the filled length of the m elting zone. The degree of fill at X=0mm and 20m m wasdecreased from the 60RPM state as expected. M elt streaking was observed indicating surface m elting with heat conduction from the barrel. At X=60mm, the conveying channelfilled withpellets. D eformation and the onset of the melt phase wereobserved over the first kneading block at X=80m m . The transition to VED melting occurred between X=100 and 120m m . The VED m elting m echanism progressed through the entire m elting zone. Although a significantam ountof un-meltrem ained,there w as slightly less than the 60RPM state. The 55kg/hr (120lb/hr) at 120RPM represented a high degree of fill with the sam e Q/N ratio as the 27kg/hr/60RPM condition. Solid conveying at X=0mm and filled length observed at X=20mm are similar to the 27kg/hr/60RPM state. Less melt streaking on the glass surface occurred due to reduced residence time at the higher screw speed decreasing heat transfer from the barrel. Compaction and deformation were seen at X=40 and 60m m . Lubrication and VED m elting began in the first kneading block at X=80mm. The VED m ode continued withareduction in pellet size. The un-melted solid volum e wasgreater than that observed in the low rate/RPM state. Axial Pressure and Tem perature Profiles The m elting steps observed in the visualization were used to interpret the average axial pressure (PAVG) and IR tem perature (TIR) profiles. Fig 2c shows the high-fill 27kg/hr at 60RPM state with the melting steps indicated. A large 300Psig pressure peak was observed at X=140m m followed by a rapid reduction to 210Psig. This is interpreted as the high-stress deformation region, followed by the lubrication of the m elt phase. The rem ainder of the kneading block length and reverse pum ping elem ent follow a pressure profile consistent with liquid flow theory 7. The TIR profile had a rapid decrease to a m inimum at X=130m m ,the location where the com paction began. This indicated that the pellets filling the channel had intimate contact with the barrel and drew m ore heat. Asthe deformation, lubrication and VED melting steps occurred, the IR tem perature increased significantly. This transition is consistent with the heat flux phenom ena observed by Curry5, where there is a high heat transfer rate from the barrel to coldpelletsduring com paction and from the melt film to the barrel during VED melting. The low-fillstate, 27kg/hr at 120RPM , pressure profile is shown in Fig 3. The plot illustrates the reduced filled length and m ovem ent of the com paction region to the first kneading block interface. Although the m elting steps are the sam e as other states, the large pressure peak isgreatly reduced. This m ay indicate that lubrication occurs very early, significantly decreasing the energy input from the deformation m ode. The Root M ean Square (RM S) values of the m eancentered dynam ic pressure signals w ere com puted foreach state. This RM S calculation (PRM S) represents the dynam ic peak-to-peak pressureorstress as the screw rotates. Figs 4 and 6 show the PRM S profiles for all states. The large PRM S increase corresponds to the com paction region and the maximum value in the deformation zone. The changes occur over very short axial lengths. The subtle effects of changes in geometry are evident as well. For exam ple, a sm all peak is observed at the double-lengthdisk attheinterface between kneading blocks. Effects of Throughput and Screw Speed Figs 3 and 4 show the PAVG and PRM S at 120RPM for different throughputs. The deformation PAVG peak is nearly absent in the low Q/N state. It increases and m oves upstream with increasing rate reflecting the filled length change. The initial PRM S rise and peaks moveupstream with throughput. For all rates, thePRM S values overlap starting at the second kneading block. This indicates that lubrication and VED melting dom inate and that flow is in the liquid regime.The screw speed effects are illustrated in Figs 5 and 6. As screw speed is increased, peak PAVG decreases and m oves downstream . The PRM S initial rise and peak also move downstream . Thus, the transition from low filltohigh fill states is captured. Conclusions An on-line m ethod to quantify melting during extrusion using visualization and axial dynam ic pressure and tem perature m easurem ents has been dem onstrated. Thekey m elting steps observed for the LDPE system through the glass windows included solid transport with conductive heating, com paction,deformation,lubrication and VED in the m elt with heat transfer to the un-melted solids. Average axial pressure, RM S pressure and tem perature profiles showed two distinct melting m odes. For large a Q/N ratio,com paction and deformation are initiated in the conveying region. A large, narrow pressure peak is observed in the high-stress deformation region that increases at higher throughputs. The RM S pressure increases prior to the pressure peak. For low Q/N states, the pressure peak is absent, indicating the onset of lubrication in the first kneading block. Infrared probe scans show a significant drop in tem perature in the com paction region due to efficient heatconduction from the barrel to the cold pellets in full contact with the metal surface. This is followed by a tem peraturerise w ith pellet-tobarrel and pellet-to-pellet friction and as the m elt phase is formed by VED heating. Visualization and axial scan data are usefulforcharacterizing melting performance as a function of materialproperties, screw geom etry and operating conditions. By linking the visualization with the axialpressureandtem peratureand profiles in a m odel system , quantitative data for melting zone evaluation is possible for operating states or materials where glass windows cannot be used. Nom enclature N = Screw Speed Q = Flow Rate P = Pressure RM S = Root m ean square T = Tem perature References 1) C. K. Shih, D. G. Tynan, D. A. Denelsbeck, “Rheological Properties of M ulticom ponent Polym er System s Undergoing M elting or Softening During Com pounding”, Polym er Engineering and Science, M id- D ecem ber, 1991, Vol. 31, No. 23, pp. 1670-1673. 2) C. G. Gogos, M . H. Kim, “M elting Phenom ena and M echanism in Polym er Processing Equipm ent”, SPE ANTEC 2000. 3) M . H. Kim, C. G. Gogos, “The Heating/M elting M echanism of Plastic Energy Dissipation”, SPE ANTEC 2000. 4) C. G. Gogos, Z. Tadm or, M . H. Kim, “M elting Phenom ena and M echanism s in Polym er Processing Equipm ent”, Adv. Polym . Tech., 17, 1998, pp. 285- 305. 5) J. Curry, “M elting M echanism s in ZSK Extruders”, SPE ANTEC 95, pp. 92-97. 6) H. Potente, U. M elisch, “Theoretical and Experimental Investigations of the M elting of Pellets in Co-Rotating Twin-Screw Extruders”, International Polym er Processing XI, 1996, pp. 101-108. 7) B. Vergnes, M . L. Delacour, G. Souveton, J. M . Bouvier, “A Study of Polym er M elting in a Co-Rotating Twin Screw Extruder”, PPS 15, June 1999. 8) T. M cCullough, B. Hilton, SPE ANTEC,1993, 3372- 3379. 9) J. P. Christiano, M . Lindenflezer. “Investigation of M ixing Patterns in Co-Rotating Fully Intermeshing Twin Screw Extruders M ixing Elem ents using Dynamic Pressure Distributions”, SPE ANTEC ’97, 501. 10) L. Zhu, X. Geng, “Physical M odel of Polym er Pellets M elting In Co-Rotating Twin-Screw Extrusion”, SPE ANTEC 2000. K eyw ords Extrusion M elting Visualization

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