The long-term safe condition of sealed radioactive sources in schools Ralph Whitcher ABSTRACT Sealed radioactive sources for school science became available during the 1950s from educational equipment suppliers and by the 1960s and early 1970s many UK secondary schools had purchased sets of them. These sources have been in use since then, which raises the question of their safe service life. A study was undertaken to examine the condition of a relatively large sample of school sources to see whether there are signs of source integrity beginning to fail and whether there are any patterns to failures, particularly those that may be age-related. The findings may be helpful to schools when undertaking reviews of the sources they hold and making judgements on keeping older sources in continued use. Sealed radioactive sources for school science became available during the 1950s from educational equipment suppliers and by the 1960s and early 1970s many secondary schools had purchased sets of them. UK suppliers of school radioactive sources at that time included Griffin & George (now Griffin Education), Philip Harris, Panax, Nicholson, and Labgear (of these, only Philip Harris supplies sealed sources today). The sources have been in use since then, which raises the question of their safe service life. Generally, any piece of equipment, even if used correctly and maintained properly, will eventually wear or degrade to the point that it should be taken out of service, and sealed radioactive sources are no different. A study was undertaken to examine the condition of a relatively large sample of school sealed sources to see whether there are signs of source integrity beginning to fail and whether there are any patterns to failures, particularly those that may be age-related. The findings of this study may be helpful to schools when undertaking reviews of the sources they hold and making judgements on keeping older sources in continued use (although schools must follow their employer’s guidance). The Approved Code of Practice (ACoP) to the Ionising Radiations Regulations 1999 states that where a sealed source reaches the end of its working life, a review of its condition is advised with a view to replacing the source or having it examined by the supplier or manufacturer. If the evidence is that the source is safe for continued use, the ACoP recommends that a time limit should be set on its continued use, after which a further review should be undertaken (HMSO, 2000). School source construction School sealed sources comprise an active component (the part that is radioactive) and a holder (the part that holds and protects the active component). Griffin & George, Philip Harris, Panax and Nicholson source holders were a cuptype design, while those from Labgear were a plate-type design. These designs were approved by the Department of Education and Science (now the Department for Children, Schools and Families) for school purchase. The most popular is the cuptype (see Figures 1 and 2). There were variations in the design, but generally the construction is a recessed plated-metal (commonly brass) cylindrical source holder, roughly 13 mm diameter and 8 mm long. The cup has a 4 mm diameter spigot so the source can be manipulated with a suitable tool. The active component (a radioactive foil) is held inside the cup by a circular spring clip and protected by a wire mesh. The spring clip is not located within a groove; it stays in place by friction. In some designs the foil is also secured by adhesive. In the Panax cup-type design, the foil is often secured just with adhesive; the spigot and cup are fastened together by a circlip and epoxy resin adhesive. In the cup-type sources, the strontium-90, americium-241, plutonium-239 and radium-226 active components are foils; the active component SSR March 2009, 90(332) 113 The long-term safe condition of sealed radioactive sources in schools of the cobalt-60 source is a small pellet of cobalt-60 metal secured with adhesive and screened by an aluminium filter to attenuate the beta emissions. The Panax cobalt-60 source (labelled S3) has a longer cylindrical holder with a small diameter recess and the pellet is embedded inside the cylinder. The Panax 333 kBq strontium-90 source (labelled S4) has an active component, a small foil, in a cylindrical housing with a collimating slit; the housing is pressed into a clear plastic block (Figure 3). The plate-type design from Labgear is a 50 mm square piece of plastic, recessed in the centre, with the active component secured with epoxy resin adhesive (Figures 4 and 5). The strontium-90, americium-241 and radium-226 active components are disc foils. The cobalt-60 active component is a cobalt-60 pellet of metal but without an aluminium disc filter, and the thorium-232 is a thorium Whitcher compound embedded in epoxy resin adhesive. Some Labgear plates have wire mesh over the front to protect the active component. Figure 3 Panax S4 source; an aluminium protective cap covers the collimating slit Figure 1 Diagram of a cup-type source construction; there were variations in this design Figure 4 Diagram of a plate source construction; there were variations in the design Figure 2 The front of a cup-type source Figure 5 A Labgear plate-style strontium-90 source 114 SSR March 2009, 90(332) Whitcher The long-term safe condition of sealed radioactive sources in schools The original manufacturer of the active components for school sources assembled in the UK was the United Kingdom Atomic Energy Authority Radiochemical Centre. (The Radiochemical Centre has changed ownership several times since, to become Amersham, then Nycomed-Amersham. Currently the sealed-source manufacturing is owned by nuclitec GmbH.) The cobalt-60 active component was made by irradiating cobalt-59 metal, the naturally occurring non-radioactive isotope of cobalt, in an intense neutron field. The other active components were laminated foils made by sintering a radioactive compound, e.g. plutonium oxide, radium sulphate, strontium carbonate or americium oxide, with silver or gold metal, into a briquette. This was backed with silver and faced with gold or gold–palladium, and then rolled into a sheet foil. Discs were stamped from the sheet foil (in Panax sources, squares were cut from the sheet foil). Note that since the late 1990s, the construction of the strontium-90 foil changed. In the current design, the radioactive material is evenly deposited onto an aluminium backing plate and the plate is anodised to seal the activity into a thin surface layer. The literature supplied with some sources gave the americium-241 and radium-226 foil sources a recommended working life (RWL) of ten years (Amersham, 1991). In the discussions between the Scottish Schools Equipment Research Centre (SSERC) and Amersham in 1990, Amersham gave a RWL of ten years for americium-241 and strontium-90 foils, but five years for the radium226 foil and the cobalt-60 pellet (SSERC, 2008). Information from former Amersham staff (personal communication, 2004) indicated that these figures were not based on any direct evidence of failure, but an expectation that the sources would retain integrity for at least the RWL. The author is aware of two earlier surveys of school radioactive sources. The first, in 1974, was carried out by the National Radiological Protection Board (now the Radiation Protection Division in the Health Protection Agency). It tested 15 plutonium239 school sealed sources following concerns about the radiotoxicity of plutonium (NRPB, 1974). Under quite brutal destructive tests, including heating one source in a butane flame for five minutes, the sources retained remarkable integrity. However, the survey did find evidence to suggest that the manufacturing process of plutonium-239 and radium-226 foil discs by the Radiochemical Centre did not completely seal the active material between the metal layers; tiny fragments may become dislodged from the edge during the process of stamping out the discs from the sheet foil, possibly causing minute traces of contamination. The NRPB report pointed out that this leakage was orders of magnitude smaller than the limits for members of the public. The NRPB concluded that demonstrations and experiments using the plutonium sources could be carried out with a very high degree of safety. The second survey was carried out by CLEAPSE (now the CLEAPSS School Science Service) in 1982 and involved testing and inspecting sources from ten educational establishments holding sealed sources that were at least ten years old. The survey concluded that, among other things, no evidence was found that mechanical or chemical damage to the source face was causing a leak of active material (CLEAPSE, 1982). The study and checks chosen to test source integrity The tests chosen for this study were a remote visual examination of the radioactive foil surface, and a wipe test for contamination. This study was carried out on a total of 250 sealed sources, detailed in Table 1. The sources were held by 41 establishments mostly around the West Sussex area: 34 local authority schools, two independent schools, three sixth-form colleges, one further education college and one school science support establishment. The Table 1 Number of sources tested, by supplier and radionuclide Supplier Griffin & George Panax Philip Harris Labgear Nicholson Totals Am-241 17 25 7 1 0 50 Co-60 12 16 8 1 1 38 Pu-239 13 0 8 0 1 22 Ra-226 25 6 23 3 2 59 Sr-90 23 37 16 2 2 80 Th-232 1 1 SSR March 2009, 90(332) 115 The long-term safe condition of sealed radioactive sources in schools leak test was based on the ISO 9978:1992 standard; the particular test chosen was the wet wipe test because it is suitable for recurrent tests and because the other methods, such as the immersion test, could cause damage to the source. The gaseous emanation test for radium-226 sources was inappropriate for this study because it would not reveal leakage of radium-226 material, whereas the wipe would pick up both radon-222 decay products and radium-226 contamination. In the wipe test, the accessible external surface (not the active component) of the source is wiped and if there is more than 200 Bq of contamination removed by the wipe, the source is failed. The wipe in this study was a small disc of cellulose filter paper barely dampened with ethanol (this method is effective in removing surface contamination without damaging the source). A sample of wipes was also taken from the lead pots in which the sources were stored. The Labgear sources were wiped with a dry disc to avoid the slight risk of damage to the plastic mount. A Rackbeta 1217 liquid scintillation counter (LSC) was used for detecting any contamination on the wipes. This is a device using photodetectors for detecting and counting scintillations produced by particulate ionising radiations in a scintillating fluid. The advantage of an LSC is the high detection efficiency, approaching 100% for alpha and higher energy beta emissions, and low background, giving a low minimum detectable activity. Where significant contamination was found, a second measurement was taken using the LSC to give information on the energy spectrum from the alpha and beta emissions. The LSC spectrum is not adequate to identify a radionuclide uniquely, but it can be used comparatively to rule out radionuclides or to compare samples. The gamma spectrum on selected wipes was also investigated using a liquid-nitrogen-cooled hyper-pure germanium (HPGe) detector gamma spectrometer with multi-channel analyser. This gave a high resolution of gamma emission energy that would enable any contamination that emitted significant gamma radiation to be identified. The surfaces of the sources were examined using an Olympus Iplex remote inspection videocamera. The 3.5 mm optical adapter at the end of the remote optical cable and illumination enabled it to be placed very close to the protective mesh of the cup source to give a magnified view of the interior of the source holder and the foil surface on 116 SSR March 2009, 90(332) Whitcher a remote screen. Photographs of selected sources were also taken remotely using a Nikon 8700 digital camera. This has an 8 megapixel CCD and a 30 mm macro lens facility. Owing to sourceholder designs, there were limitations to the visual inspection. In the cobalt-60 cup-type source, the active component is obscured by an aluminium disc filter so the visual examination was limited to examining the filter. The Panax cobalt-60 source was also limited to examining the visible surface because the cobalt-60 pellet is embedded inside the cylinder. The other Panax cup-type sources have a close mesh weave which obscures the foil surface to the extent that a thorough examination is not feasible. The Panax S4 strontium-90 foil is also largely obscured and only part of the foil can be viewed through the collimating slit. The local authority records dating back to the 1960s gave the dates that local authority schools had received authorisation to purchase the sources. This date was used as a measure of the age of the sources in looking for any trends in degradation. Some caution is needed with these data; the accuracy could not be verified as they were not part of a quality assurance process. Results of the visual examination Most of the active component surfaces in the cuptype sources from Griffin & George, Philip Harris and Nicholson showed no obvious evidence of damage or degradation. As far as they were able to be examined, the Panax foils appeared to be in satisfactory condition too. On some foils there were faint marks, likely to be from the manufacturing process rather from any subsequent abuse; the marks were light and would have been difficult to achieve by scratching the foil with the mesh in place. Some foils had small areas of light blemishes. Three cup-type sources from establishment L showed significant corrosion on the front mesh and blemishes on the surfaces of the foils. The sources had been stored close to a defective protactinium generator and this had almost certainly caused the damage. There were five sources where the foil had moved off-centre so that the edge of the circular foil was revealed. This did not show in any Panax source, but other than that there was no pattern to the supplier, date of approval or radionuclide type of these sources. There were another two sources where the spring clip had moved forward leaving the foil loose, possibly from them being dropped Whitcher The long-term safe condition of sealed radioactive sources in schools and the spring clip dislodged (Figure 6). One of these two sources showed clear signs of being dropped or struck on the edges. The foils in the S4 strontium-90 sources could be seen partially, and from what was observed there was no evidence of surface degradation. All six Labgear sources (from three establishments) with foil discs had large patches of dark discolouration on the surface of the foils, easily visible. This was mainly where the foils were in contact with the epoxy resin adhesive, but not wholly. The epoxy resin adhesive was discoloured in most of the sources. There was a suspect fissure on an americium-241 foil (Figure 7). The suspect fissure was under the epoxy resin adhesive and could not be investigated further. Many of the sources had what appeared to be stress cracks in the epoxy resin. The condition of the epoxy resin adhesive in six of the sources was such that it was decided not to test them any further but to take them out of service and place them in a sealed container; it was plausible that a wipe test could dislodge fragments of epoxy resin, possibly releasing fragments of the foils. This left just two Labgear sources, both radium-226, for leak-testing. Of the 244 sources that were leak-tested, wipes from 227 sources showed no detectable contamination. Of the 17 sources that showed contamination on the wipes, 16 were radium-226 sources and one was a plutonium-239 source held by establishment B. None of the wipes exceeded the 200 Bq fail threshold and all but one were a small fraction of it (Table 2). Note that the lower the estimated activity, the greater the uncertainty of the estimate. (When deciding whether contamination is present, there is the problem of the count from background radiation. If the background count, which is random in nature, fluctuates above average on a particular measurement, it may be wrongly interpreted as the presence of contamination – a false positive. To reduce the chance of this, a decision-level count is chosen high enough above the estimated average background count to be confident of avoiding false positives, but not so high that significant contamination is missed – a false negative. The decision level for this study was chosen at a 99% confidence level of avoiding false positives. This gave an estimated minimum detectable activity of contamination, using the LSC, of 0.34 Bq.) The contamination arising from radium-226 sources was expected because radium-226 decays to radon-222, and in some school radium-226 sources (the evidence suggests about 30% of them) radon is able to migrate through the thin foil surface and edge to cause marked contamination; Figure 6 The foil has moved out of place; the bottom edge of the foil has moved forward and over the spring clip Figure 7 Centre of a Labgear americium-241 source showing surface degradation and suspect fissure (bottom left); this is the reverse side of the plate source Results from the leak test SSR March 2009, 90(332) 117 The long-term safe condition of sealed radioactive sources in schools Whitcher Table 2 Activity measured on the wipes with detectable contamination Type Ra-226 Ra-226 Ra-226 Ra-226 Pu-239 Ra-226 Ra-226 Ra-226 Ra-226 Ra-226 Ra-226 Ra-226 Ra-226 Ra-226 Ra-226 Ra-226 Ra-226 Activity/kBq 185 185 185 185 3.7 185 185 185 185 185 185 185 185 185 185 185 185 Supplier Establishment* Panax Philip Harris Griffin & George Philip Harris Griffin & George Philip Harris Griffin & George Philip Harris Griffin & George Philip Harris Griffin & George Philip Harris Griffin & George Griffin & George Philip Harris Griffin & George Labgear A A B C B C D A E A F C G H I J K Approval date/year 1966 1966 1966 Not known 1966 Not known Not known 1966 Not known 1966 1970 Not known Not known 1960 1965 Not known Not known Estimated activity on wipe/Bq 124 6.6 6.0 6.0 5.5 2.9 1.6 1.4 1.3 1.2 0.80 0.76 0.73 0.52 0.47 0.35 0.33 * The codes A–L have been assigned to distinguish establishments of interest in this study. this is normal because the foil design was not a guaranteed encapsulation of the radon-222. The radon-222 decays and the radioactive daughter products gradually accumulate on the surfaces of the source and storage pot. Low levels of radon222 contamination are not a concern if the sources and pots are cleaned periodically – keep in mind that the average concentration of radon-222 in UK homes is about 20 Bq m–3 (Watson et al., 2005). The contamination of 124 Bq on the wipe of a Panax radium-226 source from establishment A Figure 8 Gamma spectrum of the radium-226 wipe 118 SSR March 2009, 90(332) was much higher than from any other source in the study. This was much higher than was expected from radon-222 contamination, although it was still within the ISO 9978 200 Bq limit and would not be a failure on this standard. A corresponding wipe from the storage pot of the source also showed well above average levels of contamination. The gamma spectrum of this radium-226 wipe, using the HPGe detector, was measured and compared to background (Figure 8). The characteristic energy line of 186.2 keV confirmed that radium-226 Whitcher The long-term safe condition of sealed radioactive sources in schools was present in the contamination, the other lines coming from the radium-226 decay products, bismuth-214 and lead-214. Educational establishment A had four radium226 sources; the other three showed contamination but at much lower levels. Cross-contamination could not be ruled out because the storage pots were not uniquely labelled and the sources could have been swapped into different storage pots after use. No radium-226 was detected on the wipes from the other three radium sources from establishment A. (The minimum detectable activity was estimated to be 1.8 Bq, the efficiency of the HPGe detector being much lower than the LSC.) Figure 9 shows a scatter diagram of the LSC gross count rate of the wipes, in counts s–1, against the year that government approval was given to purchase the radium-226 sources. Unknown dates are plotted at the end of the scatter diagram. Note that the radium-226 cup-type source from UK suppliers was discontinued around 1997. The background count rate is marked with a dotted line. The correlation coefficient (using CORREL in Microsoft Excel) gave a value of –0.14 (ignoring the data from sources of unknown date of approval). This is a weak negative correlation and does not support a hypothesis that older radium-226 sources give higher levels of contamination. The contamination from the wipe of the plutonium-239 source was investigated by gamma-spectrum analysis, measured over a time of 250 000 seconds. This revealed no significant characteristic gamma energy above background; this is consistent with a plutonium- 239 contamination because there is negligible photon emission beyond the low-energy part of the spectrum. An energy spectrum plot of the particulate emissions from the wipe of the plutonium-239 source, measured over 256 logarithmically separated channels using the LSC, was significantly different compared to the spectra of the wipes from the radium-226 sources (see Figure 10 for examples). This eliminated crosscontamination by radon-222 progeny from the radium-226 source that the school also held. A spectrum plot of a small quantity of low-activity plutonium-239 agreed with that from the wipe from the plutonium-239 source. From this it can be concluded with reasonable confidence that the contamination on the plutonium-239 wipe was from a small quantity, 5.5 Bq, of plutonium-239. Discussion and actions Of the 244 sources that were leak-tested, only two results gave cause for further investigation to check source integrity: a 1966 Panax radium226 source from establishment A, and a 1966 Griffin & George plutonium-239 source from establishment B. The close weave of the mesh made it difficult to examine the Panax radium226 foil surface, but from what could be seen there was no obvious damage or degradation. The subsequent wipe re-test of the Panax radium226 source showed a repeated high level of contamination so it was taken out of service and disposed of. (Establishment A held sources taking it well beyond the standard holding of 1.1 MBq, so Figure 9 Wipe tests: gross count rate for Ra-226 SSR March 2009, 90(332) 119 The long-term safe condition of sealed radioactive sources in schools Whitcher Figure 10 Liquid scintillation counter spectrum plots it was decided to dispose of the other radium-226 sources it held too.) The other 11 radium-226 cuptype sources listed in Table 2 were kept in service, with advice to clean them and re-test periodically. The visual examination of the plutonium-239 source from establishment B revealed no evidence of damage or degradation, although the foil disc was located slightly to one side under the spring clip, revealing an edge of the foil disc. The source was taken out of service, and re-tested after three months. There was no detectable contamination from the source or storage pot on the re-test; consequently the source was reinstated for use. The contamination from the plutonium-239 source could have been from a tiny fragment that had become dislodged from the foil edge during the process of stamping out the disc from the sheet foil. This would be consistent with the findings of the 1974 NRPB report in which small traces of plutonium-239 contamination were found on some plutonium sources and storage pots, the largest amount being 3.3 Bq. This compares to the 5.5 Bq found in this survey. The three cup-type sources from establishment L that had corroded meshes were taken out of service and disposed of. Although the leak test revealed no contamination, there was clear evidence of surface degradation of the foils by the exposure to hydrochloric acid fumes from a leaking protactinium generator. The two cup-type sources that had loose foils were taken out of service. Although it might be tempting to try to relocate the foil and spring clip, there is a risk of damaging the foil. Generally, the Labgear sources were not in a satisfactory condition. The visual examination showed marked degradation. Consequently, all eight Labgear sources in this study were taken out of service and disposed of. 120 SSR March 2009, 90(332) Conclusions This study did not reveal any evidence of age-related failure modes in the cup-type americium-241, strontium-90, plutonium-239 and cobalt-60 sources and the Panax S4 strontium-90 sources (although the activity of old cobalt-60 sources has decayed to the extent that they are only useful to show the effect of half-life). A risk assessment based on this evidence would help support extending their service life for, say, another ten years, provided the sources continue to show no visual signs of damage or degradation, and no detectable contamination by a suitable leak test. The same conclusion can be reached for a cup-type radium-226 source, where the source is in satisfactory condition from a visual inspection and there is no contamination detected by a leak test. The evidence from this study suggests that the contamination on radium-226 sources by radon222 is generally small. Nonetheless, this radon-222 contamination is a nuisance because it could mask low levels of contamination from radium-226, an indicator that the source integrity is starting to fail. It is not possible with school science equipment to tell if there is radium-226 contamination in the radon-222 contamination. Consequently, for a radium-226 cup-type source in which there is detectable contamination on the leak-test wipe, a cautious approach is needed in deciding whether to extend its service life. CLEAPSS recommends that where deposits of small quantities of radioactive decay products are found on the outside of the radium-226 source, the radium-226 source and its storage pot should be cleaned carefully and the source should then be re-tested before its next use. If the contamination persists, the employer’s Whitcher The long-term safe condition of sealed radioactive sources in schools Radiation Protection Adviser should be consulted for advice (CLEAPSS, 2008). If the source exhibits repeated contamination despite cleaning, it is difficult to justify keeping the source in service. A different approach has been taken by SSERC; for schools in Scotland, SSERC strongly advises that that all sources, including the radium-226 sources, should be disposed of by an authorised route after a time limit of three RWL periods (SSERC, 2008). For sources kept in service, considering that many of the sources are now over 40 years old, suitable leak tests and indirect visual examination of foil surfaces (for example by using a mirror) should be done at least yearly (the Approved Code of Practice to the Ionising Radiations Regulations 1999 specifies a period of no more than 24 months, and recommends more frequent testing when a sealed source is to be retained in use beyond its recommended working life). Schools should follow the guidance from CLEAPSS or SSERC on inspection and testing. The Labgear sources in this study were found to be at the end of their service life. This study provided no evidence to support extending the service life of Labgear sources, although the sample size of Labgear sources in this study was small. It is worth noting that the activities found on the contaminated wipes in this survey would not be a failure using the ISO 9978 standard. Except for one wipe, the estimated activities of contamination on the wipes were very low – less than 10 Bq. To put this into perspective, there is probably as much activity from radium-226 in a 300 g bag of Brazil nuts (Watson et al., 2005). The justification for detecting low activities in this study is the investigation into any early evidence of source integrity failure. Disposal of sources Sealed sources that are no longer in a safe condition should be disposed of by an authorised route. In England and Wales, the Environment Agency has produced a guidance document (available through CLEAPSS) that explains the available disposal routes. SSERC has produced guidance for schools in Scotland. Schools in Northern Ireland should contact DENI. In some cases it is possible to dispose of sealed sources with normal refuse but it is important to check the conditions that apply; these conditions vary in the different parts of the UK. Acknowledgements I am greatly indebted to Dr Alan Flowers and staff at the School of Life Sciences at Kingston University for their support and use of the university nuclear laboratory facilities. I also wish to thank Kieran Agnew for joint working in the planning stages during his MSc postgraduate study at the University of Surrey. Finally, I would like to thank the West Sussex schools and colleges and other establishments who participated in this study. References Amersham (1991) Amersham safety instructions for unpacking and use of alpha foil and sources. Ref HIO41 Issue 1. CLEAPSE (1982) Hazards from radioactive sources in schools and colleges. R. J. J. Orton. Unpublished. CLEAPSS (2008) Managing ionising radiations and radioactive substances in schools. etc. L93. Uxbridge: CLEAPSS School Science Service. HMSO (2000) Work with ionising radiation. Ionising Radiations Regulations 1999 Approved Code of Practice and Guidance. L121. Regulation 27, para 482 & 491. London: HMSO. NRPB (1974) The use of plutonium-239 in schools and other educational establishments. T. Williams. NRPBR28. National Radiological Protection Board. SSERC (2008) Protocol on the ageing and leak testing of sealed radioactive sources. Edinburgh: Scottish Schools Equipment Research Centre Watson, S. J. et al. (2005) Ionising radiation exposure of the UK population: 2005 review. HPA-RPD 001. Chilton: Health Protection Agency/Radiation Protection Division. Ralph Whitcher is Chair of the Association for Science Education’s Safeguards Committee. He is Radiation Protection Adviser for several local authorities including West Sussex County Council. He was formerly an advisory teacher for science. SSR March 2009, 90(332) 121
© Copyright 2026 Paperzz