Original Article Industrial Health 2003, 41, 273–278 Thorium-232 Exposure during Tungsten Inert Gas Arc Welding and Electrode Sharpening Hiroyuki SAITO1*, Naomi HISANAGA1, Yukiko OKADA2, Shoji HIRAI2 and Heihachiro ARITO1 1 2 National Institute of Industrial Health, 6-21-1, Nagao, Tama-ku, Kawasaki, 214-8585 Japan Department of Energy Science and Engineering, Faculty of Engineering, Musashi Institute of Technology, 1-28-1, Tamazutsumi, Setagaya-ku, Tokyo, 158-8557 Japan Received July 26, 2001 and accepted May 28, 2003 Abstract: To assess the exposure of welders to thorium-232 (232Th) during tungsten inert gas arc (TIG) welding, airborne concentrations of 232Th in the breathing zone of the welder and background levels were measured. The radioactive concentrations were 1.11 × 10–2 Bq/m3 during TIG welding of aluminum (TIG/Al), 1.78 × 10–4 Bq/m3 during TIG welding of stainless steel (TIG/SS), and 1.93 × 10– 1 Bq/m3 during electrode sharpening, with 5.82 × 10–5 Bq/m3 background concentration. Although the annual intake of 232Th estimated using these values did not exceed the annual limit intake (ALI, 1.6 × 102 Bq), we recommend reducing 232Th exposure by substituting thoriated electrodes with a thorium-free electrodes, setting up local ventilation systems, and by using respiratory protective equipment. It is also necessary to inform workers that thoriated tungsten electrodes contain radioactive material. Key words: TIG welding, Tungsten inert gas arc welding, Thorium, sharpening, Tungsten electrode, Neutron activation analysis Introduction Thoriated tungsten electrodes have been used in tungsten inert gas arc (TIG) welding since around 19511). Thoriated tungsten electrodes are widely used because of certain advantages over pure tungsten electrodes, such as easier arc starting, greater arc stability and less weld metal contamination in direct current welding1). As thoriated tungsten electrodes are gradually consumed during welding, welders need to sharpen the tip of the electrodes at regular time-intervals on a grinder. There is a possible health risk for the welders who are exposed to thorium-containing dust during TIG welding and electrode sharpening operations. Thorium-232 (232Th) is a major isotope of Th (abundance ratio: approximately 100%, and is an alpha emitter with a decay half-life of 1.4 × 1010 years2). Its specific radioactivity is 4.07 × 103 Bq/g (1.1 × 10–1 µCi/g). In Japan, the derived air concentration (DAC) and the annual limit intake (ALI) *To whom correspondence should be addressed. for inhalation exposure to 232Th are 3 × 10–2 Bq/m3 and 1.6 × 102 Bq, respectively3). As 232Th is an alpha emitter, its effect on tissue by internal exposure is greater than betaand gamma-emitters4). In the past, liver cancer and leukemia developed in a number of patients examined by angiography with thorium oxide as an X-ray contrast medium5). Despite the wide spread use of TIG welding, until recently there have been only a small number of researchers who have paid attention to the health risks of thorium exposure associated with TIG welding. Breslin and Harris reported that the radioactivity released from welding fumes during TIG welding was less than 0.9 distegrations/min/m 3 (equivalent to 1.5 × 10–2 Bq/m3), which was lower than the maximum allowable concentration in the 1950’s (70 disintegrations/min/m3 = 1.17 Bq/m3)6). Saito and Ishida measured the radioactivity of thoriated tungsten electrodes by gamma-ray spectrometry in terms of both dose equivalent and surface pollution concentration 7). Although the radioactivity of welding electrodes was lower than that stipulated for radioactive materials in Japanese regulations8), 274 they pointed out the necessity of measuring airborne Th concentrations during welding. In previous reports, airborne 232 Th concentration during electrode sharpening were reported by Vinzents9), Crim10) and Jankovic11), which were < 0.3 to 53.3 times the DAC provided for in the Code of Federal Regulations12). Airborne 232Th concentration during welding were reported by Jankovic11) and Ludwig13) as 0.001 to 0.87 times the DAC. Thus, the documented levels of 232 Th during these operations are not consistent. The aim of the present study was to measure the airborne 232 Th radioactivity concentrations in the breathing zone of TIG welders during welding and electrode sharpening, as well as in the workplace air of the welding operations. The annual 232Th intake was estimated in order to assess 232Th exposure to workers during TIG welding. Methods TIG welding and electrode sharpening operations, simulating regular work and environments, were performed at the welding shop of a factory manufacturing chemical plant in Kawasaki-city in Japan. The operations were carried out under windless conditions without local exhaust ventilation in a capacious building (90 m × 140 m × height 15 m). The welder was outfitted with protective clothing, including a hood, gloves, dust respirator, and welding helmet. Welding Airborne samples were collected in the breathing zone during two kinds of welding: TIG welding of aluminum (TIG/ Al) using a 2% thoriated tungsten electrode (φ 3.2 mm) under conditions of 15 L/min flow rate of shielding argon gas and a welding current of 110 amperes AC; and TIG welding of stainless steel (TIG/SS) under the same conditions, except for a welding current of 115 amperes DC. Both operations were performed continuously for one hour. Electrode sharpening The welder manually sharpened the 2% thoriated tungsten electrode (φ 3.2 mm) on a wheel bench grinder (G13, Hitachi Co., Ltd., Japan), without local exhaust ventilation. The sharpening operation was performed continuously for 10 min, at a point 5 m from the welding area. Sampling Respirable particles (smaller than 7.07 µm) and nonrespirable particles (larger than 7.07 µm) near the breathing zone were separately collected using the “Roken T.RSampler” (Sibata Scientific Technology, Japan)14). Non- H SAITO et al. respirable particles were collected on an impact plate coated with silicone grease by inertial impact, and respirable particles were collected on a Teflon-binding glass fiber filter (T60A20, Palflex Co., Ltd., USA, φ 35 mm). The sampling points during TIG welding and electrode sharpening operations were less than 20 cm from the operator’s nose. The massconcentration of total particles was calculated from the massconcentrations of respirable and non-respirable particles. A background air sample was collected in the same factory using a Teflon-binding glass fiber filter (T60A20, φ 110 mm) attached to a high-volume aerosol-sampling device (HVC500, Sibata Scientific Technology, Japan) with a flow rate of 500 L/min. Background sampling was performed continuously for two hours at two points over 10 m from the welding and electrode sharpening areas. The dust generated during the electrode sharpening operation was collected as sediment on a paper laid on a desk to the right of the grinder. Neutron activation analysis The 232Th in the airborne dust samples collected on the filters and in the sediment dust collected on the paper were analyzed by neutron activation analysis. The samples were placed in a double polyethylene bag and inserted into an irradiation capsule, then irradiated in a nuclear reactor (TRIGA-II, Rikkyo University, Japan). 232Th in the irradiated samples absorbed neutrons to become 233Th, and 233Th decayed to 233Pa. After six hours of irradiation and nine days of cooling, the gamma activity of 233Pa (312 keV) was measured by gamma-ray spectrometry using a germanium detector at the Musashi Institute of Technology. The weight of 232Th (µg) was converted to the radioactivity of 232Th (Bq) using the specific radioactivity (4.07 × 10–3 Bq/µg). The radioactivity of total dust samples collected in the breathing zone was calculated from the radioactivity of the filter sample collected by the TR-sampler and the percentage of respirable dust in total dust measured by the same sampler. The airborne radioactive concentration (Bq/m3) was calculated with the radioactivity of 232Th (Bq) and sampling volume (m3). Time spent in welding work The length of time that operators spend in TIG/Al and TIG/SS welding and electrode sharpening, amongst other kinds of work in a regular workday, was investigated via a questionnaire on welders’ daily work assignments in the same factory. Industrial Health 2003, 41, 273–278 275 THORIUM-232 EXPOSURE DURING TIG WELDING Table 1. Airborne mass-concentrations of dust during TIG welding and electrode sharpening, and workshop background Measurement number Respirable dust (mg/m3) Total dust (mg/m3) Ratio of respirable dust to total dust (%) 1 1 1 2 0.725 0.358 0.600 – 0.992 0.483 2.85 0.175–0.210 73.1 74.1 21.1 – TIG/Al welding a) TIG/SS welding a) Electrode sharpening a) Background b) a) Respirable dust and non-respirable dust were collected using a TR-sampler (Roken type) near the breathing zone of workers. Concentration of total dust was calculated from concentrations of respirable dust and non-respirable dust. b) Total dust was collected using a high-volume dust sampler. Table 2. Radioactivity concentrations of 232Th and percentages in airborne dust during TIG welding and electrode sharpening, and workshop background Sampling period TIG/Al welding TIG/SS welding Electrode sharpening Background 1 hour 1 hour 10 min 2 hour Measuremen number 1 1 1 2 Radioactivity concentration of 232Th (Bq/m3) 232 Total Respirable Non-respirable Th percentage in airborne dust (w/w %) 1.11 × 10–2 1.78 × 10–4 1.93 × 10–1 4.97 × 10–5 6.67 × 10–5 8.14 × 10–3 1.32 × 10–4 4.07 × 10–2 – – 2.96 × 10–3 4.60 × 10–5 1.52 × 10–1 – – 2.8 × 10–1 1.6 × 10–2 1.7 5.81 × 10–3 9.37 × 10–3 Results Table 1 shows the airborne concentrations of total dust and its respirable components during TIG/Al and TIG/SS welding and electrode sharpening operations as well as the background levels. The level of respirable dust was highest for TIG/Al welding (0.725 mg/m3), followed by electrode sharpening (0.600 mg/m3) and TIG/SS welding (0.358 mg/ m3). The levels of total dust during electrode sharpening (2.85 mg/m3) were higher than during TIG/Al welding (0.992 mg/m3) and TIG/SS welding (0.483 mg/m3). The ratio of respirable dust to total dust for both TIG welding operations was relatively high (73.1–74.1%) compared to electrode sharpening (21.1%). This indicates that less respirable dust is contained in the dust produced during electrode sharpening. The background concentrations of total dust were found to vary from 0.175 to 0.210 mg/m3, with an arithmetic mean of 0.193 mg/m3. Table 2 shows the radioactivity concentrations of 232Th and mass concentration of 232Th in airborne dust during TIG/ Al and TIG/SS welding and electrode sharpening, as well as the background levels. The level of respirable 232Th was highest for electrode sharpening (4.07 × 10–2 Bq/m3), followed by TIG/Al welding (8.14 × 10–3 Bq/m3) and TIG/SS welding (1.78 × 10–4 Bq/m3). The level of total 232Th, calculated from the radioactive concentration of 232Th in the respirable dust and the percentage of the respirable dust in the total dust, was highest for electrode sharpening (1.93 × 10–1 Bq/ m3), followed by TIG/Al welding (1.11 × 10–2 Bq/m3) and TIG/SS welding (1.78 × 10–4 Bq/m3). The background 232Th radioactivity concentrations were found to vary from 4.97 × 10–5 to 6.67 × 10–5 Bq/m3, with an arithmetic mean of 5.82 × 10–5 Bq/m3. The mass concentration of 232Th in airborne dust varied from the highest in electrode sharpening (1.7%) to much lower values during TIG/Al welding (0.28%), TIG/SS welding (0.016%) and in the background (an arithmetic mean of 0.0076%). The mass-concentration of 232Th in the sediments collected from the electrode sharpening workplace was 1.4%. Discussion The nominal percentage of ThO2 in the electrode is 1.7– 2.2% according to JIS Z 3233, equivalent to 1.5–1.9% Th15). The observed percentage of 232Th in the sediment (1.4%) approximates to the nominal value by JIS. Similarly, the percentage of 232Th in the airborne dust collected on the filter during electrode sharpening (1.7%) was almost equal to the nominal content of Th in the electrode. These two points of 276 H SAITO et al. Table 3. Summary of past reports of airborne radioactivity concentration of 232Th during electrode sharpening Author Kind of grinder Vinzents 9) Crim Jankovic 11) Radioactivity concentration (Bq/m3) Measurement number Total Breathing zone a) Respirable Non-respirable 4.5 × 10–1 d) 1.15 d) 2 1.6 d) Bench Belt a) Breathing zone Breathing zone a) 1 1 7.0 × 10 < 1 × 10–2 c) < 1 × 10 < 1 × 10–2 c) – – Bench, belt Breathing zone b) 4 8.1 × 10–2 d) – – Belt 10) Measurement position –2 –2 c) a) No description of detailed position. b) Near collar element of worker. c) Below detection limit. d) Arithmetic mean. –: Not determined. Table 4. Summary of past reports of airborne radioactivity concentration of 232Th during welding Author Jankovic Current 11) Ludwig 13) Local ventilation system Measurement position DC DC DC DC None None Installed Installed Outside helmet Inside helmet Outside helmet Inside helmet DC DC AC None Installed None Inside helmet Inside helmet Inside helmet Measurement number Radioactivity concentration (Bq/m3) Total Respirable Non-respirable 4 2 4 5 1.5 × 10 2.2 × 10–4 3.7 × 10–5 1.1 × 10–4 – – – – – – – – 14 2 8 4.6 × 10–4 1.8 × 10–4 2.6 × 10–2 – – – – – – –3 –: Not determined. evidence indicate that the airborne 232Th originated from the electrode. The radioactivity concentration of 232Th in the total dust during electrode sharpening was 1.93 × 10–1 Bq/m3; higher than that during both welding operations. Although this is a spot measurement, this value is six times the DAC (3 × 10–2 Bq/m3), stipulated in the pertinent ministerial ordinance3). Compared with previously published values (Table 3), the airborne radioactivity concentrations of 232Th obtained in the present study were one tenth of those reported by Vinzents9), and 2.4–2.8 times those reported values by Crim10) and Jankovic11). The airborne radioactivity concentration of 232Th in the total dust sampled during TIG/Al welding was 1.11 × 10–2 Bq/m3. Although this was a spot measurement, this level was one third of the DAC. The level obtained in the present study was half the highest airborne 232Th concentration reported by Ludwig13) (Table 4). The airborne 232Th during TIG/SS welding was 0.1–4.8 times that reported by Jankovic11) and 0.007–1.27 times the concentration of that reported by Ludwig13) (Table 4). In the present study, the airborne radioactivity concentration of 232Th during TIG/ Al welding was found to be 62–64 times that during TIG/ SS welding. The reason for this is that TIG/Al welding is done with an alternating current and that increases the consumption of the electrode compared to direct current welding6). It has also been reported that the airborne 232Th concentration during alternative current welding was higher than during direct current welding 13) . The airborne radioactivity concentration of 232Th during electrode sharpening reported by Vinzents et al. was 8 times that found in the present study, and 53 times the DAC (3 × 10–2 Bq/ m3)9). The 232Th radioactivity concentration during TIG welding with alternating current reported by Ludwig was 2.4 times that found in TIG/Al welding of the present study, and close to the DAC level12). The difference in the airborne 232 Th radioactivity concentrations between Vinzents 9), Ludweig13) and the present study would be derived from the differences in the work space, welding devices including the electrode-sharpening grinder, electric current and welding materials, as well as the installation of a local exhaust ventilation system. To assess the exposure to 232Th, the annual intake (AI) of 232 Th was estimated by the following equation: AI = CshpRwTshpDwP / PF + CalRwTalDwP / PF + CssRwTssDwP / PF + CweRwTweDwP + CenvRr P {(24-Tshp-Tal-Tss-Twe) Dw + 24(365-Dw)}. Here, C shp , C al , C ss , C we and C env are the observed Industrial Health 2003, 41, 273–278 277 THORIUM-232 EXPOSURE DURING TIG WELDING Table 5. Annual intake of 232Th for the operator estimated from the observed airborne radioactivity concentrations of 232Th and hours spent welding Case number 1 Dust respirator 2 3 4 Without (PF=1) 5 6 With (PF=10) Electrode Sharpening (hours/day) TIG/Al welding (hours/day) TIG/SS welding (hours/day) Other kind of work (hours/day) 0.17 7 0 0.83 0.17 0 7 0.83 0.17 3.5 3.5 0.83 0.17 7 0 0.83 0.17 0 7 0.83 0.17 3.5 3.5 0.83 Estimated Annual Intake (Bq) Ratio to Annual limit intake (160 Bq) 33.2 0.21 10.2 0.06 21.7 0.14 3.3 0.02 1.0 0.006 2.2 0.014 radioactivity concentrations of 232Th in total dust during electrode sharpening, TIG/Al and TIG/SS welding, other work and in the non-working time period, respectively. The airborne radioactive concentration of 232Th in the atmosphere of Kawasaki-city (Cenv) was 3.23 × 10–7 Bq/m3 16). Rw and Rr are the average hourly respiration volumes during light physical work (1.2 m3/hour) and in the non-working time period (1.0 m3/hour), respectively. Tshp, Tal, Tss and Twe are the working time periods (hours/day) spent in electrode sharpening, TIG/Al and TIG/SS welding, and other operations, respectively. The daily work period of an operator spent in each of the assigned jobs is shown in Table 5. These time periods were investigated via a questionnaire of daily work assignments in the subjects’ factory. P is the pulmonary absorption coefficient of 232Th and is assumed to be 100%. Dw is the annual number of workdays (days/year), and is assumed to be 250 days/year. The annual number of work hours was assumed to be 2000 hours/year (8 hours/day × 250 days/year). PF is the protection factor of the dust respirator 17) , defined as the ambient contaminant concentration divided by the contaminant concentration inside the face piece18). In the present study, we assumed two possible cases for TIG welding: with a dust respirator (PF=10) and without (PF=1). As shown in Table 5, the annual intake of 232Th was estimated on the basis of the assigned working hours that the welder spent in welding and electrode sharpening jobs, with and without a dust respirator. When the operator worked without the dust respirator (PF=1), the annual intakes of 232Th were estimated to accumulate to 10.2– 33.2 Bq (one twentieth – one fifth of the ALI), depending on the time spent in the assigned welding jobs. Wearing the respirator (PF=10) effectively reduced the annual intake of 232Th to 1.0 – 3.3 Bq (0.006–0.02 of the ALI). Although the number of measurements was small in the present study, the estimation of the AI can be taken to indicate that the annual intake resulting from occupational exposure of welders to 232Th during the regular combined operations of TIG/Al welding, TIG/SS welding and electrode sharpening does not exceed the ALI. It should be noted, however, that the present welding and electrode sharpening operations were carried out in a spacious compartment, which allowed hazardous fumes and dust to effectively dissipate, although no local exhaust ventilation system was installed. In many factories, TIG welding and electrode sharpening are carried out in a narrow space without the use of a dust respirator. Moreover workers may handle carelessly the sediment including 232Th after electrode sharpening operation. There would be a possibility that airborne 232Th concentrations in such workplaces elevate close to the DAC. In conclusion, though the 232Th level during welding and sharpening was lower than the DAC, we recommend that thoriated tungsten electrodes be replaced with thorium-free electrodes such as lanthanum-tungsten or cerium-tungsten electrodes for safety purposes. If a thoriated tungsten electrode is used, it is of the upmost importance to inform workers that the electrode contains radioactive material. Furthermore, it is necessary to reduce the risk of exposure, using a local exhaust ventilation system and a dust respirator, and ensure face and hand washing after work and the sanitary handling of clothes. References 1) American Welding Society (1951) Hi-Thoria tungsten reduces cost. Welding J 30, 264. 2) Holden NE (1977) Table of the isotopes (Revised 1995), CRC Handbook of Chemistry and Physics, 77th edition, 11-38-143, CRC Press. 3) Ministry of Labour (1972) Ordinance of prevention of ionizing radiation hazards, Ministry of Labour Ordinance No.41 of September 30, 1972, Industrial safety and health law and related legislation of Japan, 278 4) 5) 6) 7) 8) 9) 10) 11) H SAITO et al. 688–723, Japan Industrial Safety and Health Association, 1991. Bertell R (1986) Handbook for estimating health effects from exposure to ionizing radiation (2nd ed.). Institute of Concern for Public Health, Buffalo. Mays CW (1988) Alpha-particle-induced cancer in humans. Health Physics 55, 637–52. Breslin AJ and Harris WB (1952) Use of tthoriated tungsten electrodes in inert gas shielded arc welding. Ind Hyg Q 13, 191–5. Saito H, Ishida Y (1991) Radioactivity measurement of tungsten rods containing thorium. Keikinzoku Yousetsu 29, 20–6 (in Japanese). Science and Technology Agency (1988), Notification No. 15 of the Science and Technology Agency, May 18, 1988 (in Japanese). Vinzents P, Poilsen OM, Ligaard R, Simonsen H, Hansen EB, Hviid J, Svane O (1994) Cancer risk and thoriated welding electrodes. Occup Hyg 1, 27–33. Crim EM, Bradley TD (1995) Measurement of air concentrations of thorium during grinding and welding operations using thoriated tungsten electrodes. Health Physics 68, 719–22. Jankovic JT, Underwood WS, Goodwin GM (1999) 12) 13) 14) 15) 16) 17) 18) Exposures from thorium contained in thoriated tungsten welding electrodes. Am Ind Hyg Assoc J 60, 384–9. United States Nuclear Regulatory Commission (1992) Standards for protection against radiation, 10 CFR Part 20. Ludwig T, Schwaß D, Seitz G, Siekmann H (1999) Intakes of thorium while using thoriated tungsten electrodes for TIG welding. Health Physics 77, 462– 9. Kimura K (1978) On the T.R (total and respirable) dust sampler (Rep. 1). J Sci Labour 54, 11–8 (In Japanese). Japanese Standards Association (1990) Tungsten electrode for inert gas shielded arc welding, JIS Z 3233:1990, Japanese Standards Association. Japan Environmental Sanitation Center (1997) The Environment Agency commissioned business result report (1996), The analysis report on floating dust and suspended particulate matter at the National Atmosphere Survey Network (NASN). National Institute for Occupational Safety and Health (1997) Pocket guide to chemical hazards, xxv-xxx. DiBerardins LJ (1999) Handbook of occupational safety and health, 2nd ed, 655, John Wiley & Sons, Inc. Industrial Health 2003, 41, 273–278