Radiation Physics and Chemistry 57 (2000) 641645

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New applications of 10 MeV electrons for reeled goods

C. Gu nthard*, D.W. Lee
Studer AG Werk Hard, CH-4658, Daniken, Switzerland

Abstract Because of their high penetration capability, electron beams produced by 10 MeV machines are increasingly used for the sterilization processing of medical devices. Worldwide there are already more than 20 such machines in action for this purpose. But compared with electron beam sterilization, the physical crosslinking of plastic products with 10 MeV has not been as much investigated as in the range of low and medium energy. So the products with high wall thickness or big dimensions are still chemically crosslinked as the penetration and power of the beam of existing accelerators was not sucient for those products. But now radiation crosslinking is possible also for higher dimensions of reeled goods due to higher beam power up to 150 kW, and one machine with dierent handling systems can be used for sterilization and modication of plastic products. The aim of our work is to examine the homogeneous crosslinking of industrial products by a 10 MeV/150 kW electron beam as for instance for XLPE-c pipes and heat shrinkable tubes. Furthermore the uniformity of crosslinking especially along the roundness is measured, which is one of the essential quality characteristics. 7 2000 Elsevier Science Ltd. All rights reserved.
Keywords: 10 MeV/150 kW electron beams; Crosslinking; Homogeneity; Warm water pipes; Heat shrinkable tubes

1. Introduction Since the beginning of the 1970s the electron beam technology has found a wide industrial acceptance for sterilization of medical devices and polymer modication. The main reasons are economical and ecological advantages, so nowadays there are more than 1000 electron beam machines operating worldwide (Scharf, 1998) in dierent application elds. Most of those machines are using beam energies in the range of 0.15 MeV with 40100 kW of power, which is ample to treat technical products. The highenergy machines up to 10 MeV are increasingly used in the sterilization of single-use medical devices. Those

* Corresponding author.

machines mostly have a relatively low beam power of about 1040 kW, which is suciently cost eective for low doses of sterilization (25 kGy), but not for crosslinking of plastic products, which need relatively high doses of 150300 kGy. Therefore products with big wall thickness or complicated geometry are still chemically crosslinked. By means of big dimensioned polyethylene pipes and heat-shrinkable tubes, this paper presents the application of electron beams with high beam energy and a power of 10 MeV/150 kW. Studer Company bought the rst Rhodotron-type 10 MeV accelerator from IBA company (IBA (Ion Beam Applications), 1995) for his Swiss based contract irradiation center and has now well over 2 years of processing experience with this installation, based on a 3 4 shift continuous operation.

0969-806X/00/$ - see front matter 7 2000 Elsevier Science Ltd. All rights reserved. PII: S 0 9 6 9 - 8 0 6 X ( 9 9 ) 0 0 4 8 5 - 5

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Fig. 1. Penetration of 10 MeV electrons in LDPE plates (density: 0.92 g/cm3)

2. The 10 MeV electron beams If the charged electrons with almost light speed are moving through a material, they lose their energy by interaction with the electron structure of that material. The distance passed by those charged electrons, so called the penetration, depends on the energy of the accelerator and on the density of the irradiated material. In their energy range between 1 and 10 MeV, the relation of beam energy and electron penetration can be estimated with the following formula (Becker et al., 1979): E 2X2 Z50 0X3 where E is the incident electron energy (MeV) and Z50 is the eective product thickness (g/cm2) by single side treatment. The eective product thickness is dened with an exit dose of 50% of maximum dose. The factor 2.2 is appropriate for polymers such as polystyrene, polymethylmethacrylate, and cellulose. For compounds like polyethylene this factor should be about 5% larger, because the high hydrogen content increases the stopping power and reducing the range of the energetic electrons (Becker et al., 1979). According to this formula the beam energy of 4.5 MeV has the eective product thickness for polyethylene 1.8 cm, and 10 MeV has 4.2 cm. If the products are irradiated on both sides by turning, the useful range can be about doubled. Fig. 1 shows a measurement of depth/dose distribution of polyethylene plates (density 0.92 g/cm3) being irradiated by electron beams of 10 MeV perpendicular to the surface of products. The homogeneous crosslinking is up to 4.5 cm, where the exit dose is

about 50% of the surface dose. This value is very close to the obvious theoretical value of 4.2 cm. The beam power utility can be theoretically calculated by the following equation (Becker et al., 1978): P Doa3600 Mat 1aFp where P (beam power kW), Do (average absorbed dose kGy), M/t (mass throughput rate, kg/h) and Fp power utilization eciency. In the praxis some loss of power is unavoidable due to the scattering, failure of some selectrons to hit the products, etc. So the power utility very much depends on the design of the beam geometry, under beam handling system, specication of product, procuts dimension, etc.

3. Crosslinking of reeled products More than 60% of the installed electron beam accelerators are used for the treatment of reeled products e.g. cable, wire, tubes, pipes, etc. The reasons are the advantages in processing, compared to chemical crosslinking, as well as in economical and ecological points of view. One of the important requirements for those products is the homogeneous crosslinking around the whole cross section. The ionizing radiation must suciently penetrate all positions of the roundness. As with reeled products the conguration of beam penetration becomes more complex than with at sheets, as shown in Fig. 1, it deserves special concern. The reeled products are strung by an under-beam handling consisting of two sets of drums and moved back and forth repeatedly for 2-sided irradiation,

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(A ) must be specially considered, which is dened as follows: A OD2 ID2 1a2 where OD is the outer and ID is the inner diameter. The beam should have power high enough to penetrate this worst case, especially for plastic pipes or heat shrinkable tubes, which are hollow, otherwise some of the retarded electrons are accumulated inside the pipe and may puncture the pipe wall.

4. Warm-water polyethylene pipes Plastic pipes for carrying hot water under moderate pressure are mainly made of polypropylene (PP), polybutylene (PB), chlorinated polyvinylchloride (CPVC) and crosslinked polyethylene (XLPE). Their demand is drastically increasing due to the ecological advantages, as according to the analysis results (Ka ufer et al., 1994) plastic pipes are showing the lowest contaminating values in ground, water and air comparing to steel or copper pipes. Among them the crosslinked polyethylene (XLPE) pipe shows the greatest toughness, withstanding the stress of high pressure and temperature for a long term. So it is nowadays well established for these high performance corrosion-proof pipes with long-term resistance in the eld of oor heating, for sanitary use and drinking water supply. Nowadays in Europe the demand for polyethylene for the production of pipes is about 600,000 tons a

Fig. 2. Geometric consideration of Reeled product irradiation

whereby they are increasingly crosslinked all around the wall. Here the penetration must be considered especially in worst case of irradiation. Fig. 2 shows an example, the beam is vertically approaching the surface of the product. Although the electrons are optimally penetrating the wall thickness (B ) of the product, the side range (A ) is not suciently penetrated (Ba uerlein, 1981; High Voltage Engineering, 1979), as it is exceeding the wall thickness (B ). Therefore this worst case

Fig. 3. Distribution of gel contents around the cross section of pipes (50mm outer diameter 6mm wall thickness) iradiated by 10 MeV electrons

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Fig. 4. Minimum and Maximum Hot Set values of dierent dimensioned heat shrinkable tubes (wall thickness 23mm and 3 5mm) irradiated by 10 MeV and 4.5 MeV electron beams

year with a segment of 10% being crosslinked, which is a rapidly increasing segment. Besides, the conventional steel and copper pipes must be replaced in the near future, because they have more and more corrosion problems, incrustations or microbial risks. Additionally the water quality is getting worse and toxicity of copper (Scha fer and Schu mann, 1991) being dissolved by acid water is also serious. Fig. 3 shows the distribution of gel contents around the cross section of the pipe, whose dimension is 50 mm (outer diameter) 6 mm (wall thickness), crosslinked by 10 MeV/150 kW electron beams. The mean value of gel contents is 69% and its distribution is very dense, which causes a sucient and homogeneous crosslinking along the roundness.

5. Heat shrinkable tubes There are three categories of heat shrinkable tubes in use according to their long-term application tem-

peratures, namely made of PVC , of crosslinked polyolenes or uoropolymers as PVDF or PTFE. On the basis of price-performance advantages the crosslinked polyolenes are mostly used for temperatures up to 1308C. The materials are often made of polymer blends compounded with dierent additives to meet the properties of ame resistance and resistance against heat aging. Here the homogeneous crosslinking around the cross-section is an important characteristic of quality, which inuences the follow-up process of the expansion, the resulting wall thickness and the thermal shrinkage. Fig. 4 shows the comparison of Hot Set distributions of dierent dimensioned heat shrinkable tubes, which are crosslinked with the two dierent beam energies of 4.5 and 10 MeV. The Hot Set (elongation under heat (2008C/15 min) and load (20 N/mm2) measures according to DIN 57472 or IEC 540. This test is widely used by cable, wire or heat shrinkable products to check the crosslinking state, so the higher crosslinked material the lower the Hot Set value.

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Up to 20 mm outer diameter with 23 mm and 3 5 mm thickness the dierences of the maximum and minimum Hot Set values are not so noticeable. However, with big dimensioned tubes of 30, 40, 50 and 65 mm outer diameters this dierence is becoming very signicant. For example in case of 50 mm tube the Hot Set value is 190220% when crosslinked by 10 MeV, whereas it is 190330% treated by 4.5 MeV.

Pfa kon, Switzerland) and Mr. H. Mitschak (Cellpack GmbH in Waldshut-Tiengen, Germany) for technical assistance.

References
Ba uerlein, R., Siemens AG. 1981. Vernetzung von Kabel- und Leitungsisolierungen aus Polyolenen durch energiereiche Strahlung, Bundesministerium fu r Forschung and Technologie, Forschungsbericht, pp. 81123, July 1981. Becker, R.C., Bly, J.H., Cleland, M.R., Farrell, J.P. 1978. Accelerator requirements for electron beam processing. International meeting on Radiation Processing, Miami, Florida, October 1978. Becker, R.C., Bly, J.H., Cleland, M.R., Farrell, J.P., 1979. Accelerator requirements for electron beam processing. Radiat. Phys. Chem. 14, 353357. High Voltage Engineering, 1979. Estimating electron beam processing requirements for wire, cable and tubular products, Rev. 4. IBA (Ion Beam Applications) 1995. Practical advantages of the IBA Rhodotron, October 1995. Ka ufer, H., Weinlein, R., Jakel, C. 1994. The VENOB methode (consideration of comparing the results under standardized condition), Technische Universita t, Berlin, December 1994. Scha fer, S.G., Schu mann, K., 1991. Zur Toxikologie des Kupfers. Bundesgesundheitblatt 7, 323327. Scharf, W. 1998. Warsaw University of Technology, Poland, Electron accelerators for industrial processing a review, April 1998.

6. Conclusion The latest development of powerful 10 MeV accelerators not only enables the already established electron beam sterilization of medical devices but also the crosslinking of polymer products. The combination with crosslinking of big dimensioned products opens new elds of application, which could not be realized commercially, due to the limited range of penetration of beam and of machine power. Big dimensioned hot water polyethylene pipes (50 6 mm) and heat shrinkable tubes (up to 65 5 mm) are irradiated and the distribution of the crosslinking degree around the cross section were measured. The results conrm the successful treatment.

Acknowledgements We thank Mr. G. Gielenz (Huber+Suhner AG in