INHALATION AND RETENTION OF THORIUM DUSTS BY MINERAL SANDS WORKERS
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Ann. occup. Hyg., Vol. 41, Supplement 1, pp. 92-98, 1997 © 1997 British Occupational Hygiene Society Published by Elsevier Science Ltd. All rights reserved Printed in Great Britain 0003-4878/97 $17.00 + 0.00 Inhaled Particles VIII PII: S0003-^878(96)00134-2 INHALATION AND RETENTION OF THORIUM DUSTS BY MINERAL SANDS WORKERS G. S. Hewson Department of Minerals and Energy, 100 Plain Street, East Perth, WA 6004, Australia INTRODUCTION Heavy mineral sands consisting of ilmenite, rutile, zircon and monazite, have been mined and processed in Western Australia since 1956. The industry is a significant one; in 1995 it mined 37.4 million tonnes of sand and processed 2.6 million tonnes of heavy mineral concentrate to produce 2.1 million tonnes of the individual mineral sands, at a value of $550 million. A specific occupational health concern associated with this industry is radiation exposure arising out of the presence of thorium and, to a lesser extent, uranium with all the heavy minerals. Monazite, a rare earth phosphate, is radiologically the most significant mineral, containing typically between 5 and 7% thorium and 0.1 and 0.3% uranium. Although monazite is a low volume product, comprising only about 0.5% of total mineral sand production, it tends to preferentially concentrate in airborne dust because it is softer than the titanium and zirconium bearing minerals. This is of particular concern during the processing of mineral sands because the minerals are subjected to a variety of vigorous physical treatment processes, such as screening and magnetic, electrostatic and gravity separation. Without the application of appropri- ate dust control technology, considerable airborne dust (and consequently radio- activity) concentrations may be experienced by workers who operate and maintain the separation plant. While the presence of radioactivity in this industry has been long appreciated, early protective and regulatory measures were focussed on control of external radiation exposure in circuits where monazite was being concentrated and bagged. Intake of radioactive dust was only recognised as a potentially significant source of exposure in the early 1980s, following national review and acceptance of ICRP Publication 30 (ICRP, 1979). This resulted in derived air concentration (DAC) values for thorium an order of magnitude lower than those previously applied to the industry (Hewson and Terry, 1995). The issue of intake of radioactive dust prior to the mid 1980s is important because there are many long-term workers in the industry and it is well recognised that each of the five dry separation plants were very dusty. In addition, early work practices, such as use of compressed air to blow down equipment, and sweeping, banging and brushing of floors and plant equipment, coupled with limited use of respiratory protective equipment, exacerbated the potential for dust inhalation by workers operating and maintaining the separation plants. Industry management 92
Inhalation and retention of thorium dusts 93 and employees, through a concern about the likely long-term health implications of exposure to radioactive dust, have both been anxious to ascertain the extent of past exposure and have supported a range of bioassay research endeavours. This paper examines the inhalation exposure estimates obtained from bioassay studies and compares them with estimates from personal air sampling and a retrospective assessment of intake of radioactivity. One objective of such a comparison is to assess the veracity of recommended biokinetic models. Another is to investigate the feasibility of using an alternative, cost-effective exposure assessment technique, such as exhaled thoron, as a routine monitoring tool. METHODS As thorium oxides have a very long half-time of clearance from the lung, bioassay measurements, apart from analyses of faeces, will reflect long-term chronic inhalation. To relate the results from bioassay to air sampling requires knowledge of annual average daily intake over the exposure period. For each year since 1977 an estimate of the average airborne alpha activity concentration across the industry was made as follows: X = (6).(20).(0.06).Dg.SATh.MHMc where X is the average alpha activity, Bq m~3 6 is the number of alpha particles emitted per decay of 232Th in ore dust 20 is the concentration factor for monazite in airborne dust (Hewson and Terry, 1995) 0.06 is the average thorium content of monazite Dg is the arithmetic mean gravimetric dust concentration, mg m~3 SATh is the specific activity of 232Th, 4.1 Bq mg""1 M H MC is the average monazite content of heavy mineral concentrate. The mean gravimetric dust concentration for separation plant workers was obtained from the Department's atmospheric contaminant exposure database, known as CONTAM. The number of personal air samples has varied from 165 in 1977 to in excess of 2581 in 1989 and the number of samples per "designated" radiation worker is now typically in the range of 6-10 per year. Details of the dust sampling measurements are summarised in Hewson and Terry (1995). The monazite content of heavy mineral concentrate feedstock (M HMC) to the dry separation plant was determined by reviewing historical mineral sands production data reported to the Department of Minerals and Energy by the mineral sands companies. For the years 1975, 1976 and the period prior to 1975, it was assumed that the mean personal dust concentration was 15 mg m~3, based on measurements in the late 1970s. This assumption maybe overly conservative as the two new plants which commenced operations in the mid to late 1970s were larger than the three existing plants and were considered very dusty by the inspectorate. An average M H MC content prior to 1975 of 0.40% was calculated by examining total production figures to that time. The estimates derived from this analysis were used to assign pre-1986 values for
94 G. S. Hewson the annual intake of radioactive dust (and hence internal radiation dose) for those workers who had participated in bioassay studies. This required knowledge of the employment history of the individual and average annual working hours; informa- tion which was readily available from company records. The intakes were subsequently converted to committed (over 50 years) effective doses using conver- sion factors derived from the new ICRP 66 lung model (ICRP, 1994). Procedural details are described by Hewson and Terry (1995) and Terry and Hewson (1994). Results of recent bioassay studies were reviewed, including: (1) the concentra- tion of thorium in blood serum and urine (Hewson and Fardy, 1993); (2) the concentration of thorium in faeces (Terry et al., 1995); (3) the concentration of thoron exhaled in breath; and (4) the amount of thorium decay chain radionuclides deposited in lungs and other organs (Terry and Hewson, 1994, 1995). The predicted concentration of thorium in urine, blood serum and lungs was calculated using the ICRP 66 lung model (ICRP, 1994) and ICRP 30 biokinetic model for thorium (ICRP, 1979) and assuming workers were chronically exposed to relatively insoluble thorium ore dust with a median particle size (or activity median aerodynamic diameter—AMAD) of 10 urn. RESULTS At the five individual separation plant sites the average monazite content was found to vary between less than 0.1% and about 2.0%. The average monazite content across the industry has varied from 0.11% in 1994 to 1.13% in 1983, with the latter figure corresponding to annual monazite production of 15 606 tonnes. The value for 1994 is biased low as the industry substantially curtailed monazite production in 1994 as a result of a drastic fall off in demand. Thus, the above retrospective analysis cannot be applied to the 1994 and 1995 dust data. CONTAM records show that mean dust concentrations in the dry separation plants have progressively declined from 16.8 mg m~3 in 1977 to 1.4 mg m~3 in 1991, although a substantial level of non-compliance with the general dust standard of 10 mg m~3 was evident up to the mid 1980s. The average alpha activity derived from the retrospective assessment procedure for the period < 1975-1993 is shown in Fig. 1, together with the average monazite content and the actual average alpha activity, routinely determined by the mineral sands industry since 1986. It can be seen that there is reasonably good correlation between the actual and estimated alpha activities since 1986, which provides confidence in the reasonableness of the estimates in the period before 1986. The increased measured alpha activity in 1989 corresponds to a period when large scale engineering control work was being undertaken in some of the plants and it is assumed that the additional maintenance activity was resulting in increased resuspension of settled dust. Depending on the site (or monazite content of feed material), pre-1986 doses to separation plant workers were estimated to vary between 9 and 90 mSv per annum (cf. current ICRP recommended dose limit of average 20 mSv per annum). For other workers, annual doses of one-tenth or one-third these values were chosen, depending on nature of task and extent of dust exposure (Hewson and Terry, 1995). It is emphasised that the estimates relate to a "typical" plant producing about 2000-3000 tonnes monazite per annum or with about 0.5-0.7% monazite in
Inhalation and retention of thorium dusts 95 •*- Estimated Alpha Activity —% Monazite • Actual Alpha Activity 9 CD 1 Q. ' • N, • • \ II 0 ! 1 i 1 1 1 1 1 1 1 1 ! 1 1 1 1 1'
96 G. S. Hewson Urine - n=34, 1-20y Blood - n=25,1-20 y Lung - n = 19, 6-35 y TIB - n =62,4.5-35 y TIB - n =47, 7-35 y Faeces - n=2 PAS - 0.5 1 1.5 2.5 -1 Thorium Intake (Bq d 232 Fig. 2. Estimated intake of Th by mineral sands workers using various bioassay techniques, normalised against personal air sampling measurements. The longer thoron in breath (TIB) bar refers to 62 workers with employment between 4.5 and 35 years, and the shorter to a subset of 47 workers with employment longer than 7 years. from the start of intake (and is in equilibrium with daily inhalation rate) and reaches negligible amounts in about 7 days from the cessation of intake. The thoron in breath results show that, for those employees above the minimum detection limit (MDL), the thorium lung burdens are significantly higher than predicted on the basis of applying intake data (from personal air sampling data) to the new ICRP 66 lung model (ICRP, 1994). However, the results are biased by the large number of workers (81 out of 145 workers tested) below the MDL of the technique. Of interest is that 75% of short-term (employment duration < 7 years) workers are below the MDL and that the average intake of short-term and long-term workers is 0.15 and 0.54 Bq d"1 232Th, respectively. Thus, it is evident that there has been improvement in the exposure status of mineral sands workers over the last 7-10 years. The breath measurements revealed that 25 workers (17%), including three short term workers were estimated as receiving an average annual dose of 20 mSv or more over their total employment period. One of the highest lung burdens was measured on a retiree, who had been out of the industry for 10 years and other substantial burdens were measured on long-term workers who had not been working in dusty jobs for about 10 years. These results underline: (1) that considerable intakes of radioactive dust were incurred by some workers in the 1960s and 1970s; and (2) that once thorium ore dust lodges in the lungs it is avidly retained. The elevated lung burdens recorded against the three short-term workers are of concern, as their predicted intake is significantly above their work category colleagues. Differences in an individual's results arise through personal factors such as work habits, use or non-use of a respirator, mode (i.e. mouth or nose) and rate
Inhalation and retention of thorium dusts 97 of breathing and smoking habit. Such factors may result in the actual exposure being either higher or lower than estimated from personal air sampling. The discrepancy may also be due to a combination of incorrect intake data, inappropri- ate metabolic data or incorrect assumptions about dust characteristics, such as particle size. As the metabolic data reflect the latest scientific knowledge it is more likely that the air sampling data is not providing representative coverage of high exposure tasks. However, the discrepancy could be explained if the AMAD was 5 urn (not 10 urn) or if the worker was a mouth breather. The range of ratios of predicted thorium lung burden (from air sampling) to estimated burden (from breath measurements) varied from 0.43 to 13.5, confirming that there is substantial inter-worker variability in intake, even for workers with similar employment periods in the same work category. It is interesting to note, however, that the average ratio of measured to predicted lung burdens for long term workers is within a factor of 2, which provides some confidence in the reasonableness of the retrospective assessment. Many health physicists might consider this as good agreement. The results indicate that thoron in breath measurements provide data that are complementary to air sampling data and are able to identify workers whose work habits require closer investigation. One disadvantage of the breath measurements is that the MDL is relatively high and therefore the technique is primarily restricted to long-term workers or short-term workers with significant intake. The Depart- ment of Minerals and Energy has recently developed and commissioned an alternative breath measurement device, utilising an electrostatic collection cham- ber and this has resulted in a 50% improvement in the MDL. The Department has provided this device to industry and it is currently being trialled on selected workers using a measurement strategy based on tests at the start, middle and end of the year. Preliminary results indicate that the technique is sufficiently sensitive and cost effective and could replace the comprehensive and expensive regime of personal air sampling that is currently used by the industry. The major advantage of the technique over air sampling is that it identifies individual workers at elevated risk and enables suitable investigation and intervention strategies to be implemented. While the air sampling regime is considered comprehensive, in comparison to sampling conducted in other industry sectors, it should be recognised that the number of air samples on an individual worker represents only about 5% of the worker's annual working shifts. CONCLUSIONS Reasonably good correlation between estimates of thorium intake derived from air sampling and retrospective assessment and estimates from bioassay measure- ments was found for long-term workers. Bioassay measurements on recent workers, although higher than expected, confirm the increasing improvement in industrial hygiene conditions and work practices since the early 1980s. Periodic thoron-in-breath measurements could replace the comprehensive regime of person- al air sampling which currently exists in the industry, thereby providing a relatively sensitive and cost effective diagnostic monitoring tool. Continued study of the mineral sands workforce could yield important informa-
98 G. S. Hewson tion about the inhalation and retention of insoluble dust particles. Mineral sands dust has the advantage of a "radioactive signature", which allows direct in vivo measurements of the dust in the lungs and other organs and the measurement of thoron exhaled in breath. Periodic measurements of workers who are no longer employed in dusty tasks will enable an assessment of the clearance of dust from the lungs. REFERENCES Hewson, G. S. and Fardy, J. J. (1993) Thorium metabolism and bioassay of mineral sands workers. Health Phys. 64, 147-156. Hewson, G. S. and Terry, K. W. (1995) Retrospective assessment of radioactivity inhaled by mineral sands workers. Radiat. Prot. Dosim. 59, 291-298. International Commission on Radiological Protection (1979) Annual limits on intake for workers. ICRP Publication 30, Pergamon Press, Oxford. International Commission on Radiological Protection (1994) Human respiratory tract model for radiological protection. ICRP Publication 66, Pergamon Press, Oxford. Terry, K. W., Hewson, G. S. and Meunier, G. M. (1995) Thorium excretion in faeces by mineral sands workers. Health Phys. 68, 105-109. Terry, K. W. and Hewson, G. S. (1995) Thorium lung burdens of mineral sands workers. Health Phvs. 69, 233-242. Terry, K. W. and Hewson, G. S. (1994) Thorium lung burdens of workers in the mineral sands industry. Report of research commissioned by the Titanium Minerals Committee of the Chamber of Mines and Energy. Department of Minerals and Energy, Perth Western Australia.
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