PII: S0003-4878(00)00077-6 Ann. occup. Hyg., Vol. 45, No. 3, pp. 209–216, 2001 2001 British Occupational Hygiene Society Published by Elsevier Science Ltd. All rights reserved Printed in Great Britain. 0003–4878/01/$20.00 Cohort Mortality Study of North American Industrial Sand Workers. III. Estimation of Past and Present Exposures to Respirable Crystalline Silica R. J. RANDO†*, R. SHI‡, J. M. HUGHES‡, H. WEILL§, A. D. MCDONALD¶ and J. C. MCDONALD¶ †Department of Environmental Health, School of Public Health and Tropical Medicine, Tulane University Medical Center, 1430 Tulane Avenue, New Orleans, LA 70112 USA; ‡Department of Biostatistics, School of Public Health and Tropical Medicine, Tulane University Medical Center, 1430 Tulane Avenue, New Orleans, LA 70112 USA; §Department of Medicine, School of Medicine, Tulane University Medical Center, 1430 Tulane Avenue, New Orleans, LA 70112 USA; ¶Department of Occupational and Environmental Medicine, National Heart and Lung Institute, Imperial College School of Medicine, Dovehouse Street, London SW3 6LY, UK Background: Lung cancer and silicosis mortality were examined longitudinally and by a casereferent analysis in a cohort of workers selected from the North American industrial sand industry. Date of hire in the case-referent sub-cohort extended as far back as the second decade of the twentieth century. Objective: The aim of this study component was to develop estimates of average and cumulative exposure to respirable crystalline silica for the 342 selected cases and referents. Methods: Process and dust control histories were developed for each plant, and quantitative exposure data obtained from each of them and from a trade organization. An algorithm was developed to convert historical exposures reported in particle count concentrations to modern measures of mass concentration of respirable crystalline silica. Personal exposures were adjusted for use of protective equipment based on frequency of use and type of protection. Findings: Between 1974 and 1998, a total of 14 249 exposure measurements had been taken using a cyclone and membrane filter and gave an overall geometric mean of 42 mg/m3. The only exposure data identified earlier were based on approximately 500 samples collected across the industry between 1947 and 1955 using the Greenburg–Smith impinger, with analysis by microscopy. These data were converted to modern measures using a factor of 1 mppcf = 276 mg/m3 respirable dust and then adjusting for percentage silica. In general, the highest exposures occurred in bagging and bulk-loading operations and the lowest in wet processing of sand. Conclusions: There has been a substantial decline in exposure levels in this industry over time. The decline was rapid between the 1940s and 1970s and current exposures are, on average, less than 50 mg/m3. The use of personal protective equipment was judged to have had little impact on exposure before the 1970s. 2001 British Occupational Hygiene Society. Published by Elsevier Science Ltd. All rights reserved Keywords: silica; sand; mass-number conversion; exposure estimation INTRODUCTION Received 27 July 2000; in final form 28 September 2000. *Author to whom correspondence should be addressed The industrial sand industry provides high-purity silica sand and flour for glass manufacture, foundries, pigment production, and oil drilling. This entails the extraction of natural deposits of quartz mineral and 209 210 R. J. Rando et al. processing to remove contaminants and grade the product. Raw sand is extracted in three ways: hard sandstone is quarried by drilling and blasting, friable sandstone is hydraulically mined using high-pressure water cannon, and loose sand deposits are dredged from ponds. The first step is typically wet reduction using rod mills (chaser mills in the past). The material is then sent to flotation tanks to remove clays and other contaminants. These steps are collectively known as “wet processing”, and are followed by a drying operation. Steam coil dryers, common in the past, have been replaced by rotary kiln dryers and, more recently, fluidized bed dryers. Dried sand is segregated into size fractions by mechanical screening or air separation, and then stored in bins or directly bagged or loaded into bulk containers for transport by rail and truck. In some plants, dried sand is fed to a ball-milling operation to produce silica flour. The silicosis hazard from industrial sand and other crystalline silica-containing particulate has long been recognized. In 1997, the International Agency for Research on Cancer (IARC) concluded that crystalline silica was also carcinogenic to humans. As part of a cohort mortality study of North American industrial sand workers (McDonald et al., 2001), a nested case-referent study of deaths due to lung cancer and silicosis was conducted (Hughes et al., 2001). This report describes the reconstruction and estimation of exposure to respirable crystalline silica for 342 workers (123 cases and 219 controls), spanning the time period 1912 to 1994. METHODS Individual average levels of exposure to respirable crystalline silica for all workers in the study were estimated by linking job histories to a job-exposure matrix. A separate job-exposure matrix was developed for each plant by taking into account existing exposure monitoring databases from the modern era (post-1970) and from the distant past (1947– 1954). The historical data, reported in units of millions of particles per cubic foot (mppcf) were converted to modern units of respirable crystalline silica concentration using a calculation algorithm. The exposure estimates were also adjusted for use of respiratory protective devices since about the mid-1970s. Details of the exposure reconstruction process follow. Plant visits Numerical and qualitative data on worker exposures were first obtained from all possible sources, including company documents, consultant reports, publications and government databases. After analysis of the data, each participating plant was visited by the industrial hygienist (RJR), who met with plant health/safety personnel and, usually, a long-term employee or retiree. A tour of each facility was made with the aim of relating job titles and work areas to exposure information, with special attention to temporal trends or changes that might have influenced exposure. The history and current state of any respiratory protection program was also reviewed. These inquiries were confined to the period beginning when any of the cases or controls were first employed, which ranged from 1912 to 1955. Available data Recent exposure measurements had generally used a 10-mm nylon cyclone in series with a PVC membrane filter. After collection of the respirable dust fraction, samples were analyzed for crystalline silica content by quantitative x-ray diffraction spectroscopy and for total particulate mass gravimetrically. Many of the participating plants had moved from routine laboratory analysis of silica content of collected dust to estimates based on average percentage silica in dust samples from a given area/department/task. In each case, the modern exposure measurements were presented in µg respirable crystalline silica per m3 of workplace air. The application of the cyclone sampler/x-ray diffraction technique began in the early 1970s; previously, samples had been collected using Greenberg–Smith or midget impingers containing alcohol/water solution, and the dust particles (⬍5 µm) counted microscopically in units of mppcf. Conversion of sample results In order to utilize these data, conversion into modern measures was necessary. In other industries (e.g. Vermont granite sheds), a conversion factor was obtained from side-by-side samples collected by impinger and by cyclone. However, no comparable data of sufficient reliability could be identified for the industrial sand industry, so a computational approach using an existing sample database (Severns, 1979) was taken. This was based on 14 samples collected on membrane filters with a 10-mm nylon cyclone preseparator, in various processes in several industrial sand plants, and analyzed by oil-immersion microscopy, with particle counts reported in nine size categories. While limited in scope, this was the only information of this type that could be identified for use in development of the conversion algorithm. The computational algorithm entailed estimation of the “true” environmental concentration of particles of a given size by accounting for the sampling efficiency of the cyclone, eC. The estimated concentration was then converted to a mass concentration assuming spherical silica particles of specific gravity 2.65. The mass contribution of each size fraction was then totaled to derive the mass concentration of respirable particulate in the sample. The collection/analysis efficiency of the impinger/microscope, eI, was then applied to the estimated environmental concentration to determine the expected:observed concentration by Cohort mortality study of North American industrial sand workers. III impinger for the same sample. The number contributions in each size fraction were summed to determine the overall particle concentration expected from an impinger sample of the same atmosphere. The conversion factor, equating the gravimetric respirable concentration in units of µg/m3 to the impinger particle count in units of mppcf, was then: µg/m3 = mppcf 冢 p 6×0.0283 m3 ft3 冘 冣冘 nid3i ni eI,i eC,i In this equation, di is the geometric mean aerodynamic diameter and ni is the observed particle count for the ith particle size interval in the microscopic analysis of the sample. For this particular set of samples, the values for particle size and collection efficiencies used in the computational algorithm are presented in Table 1. Personal protection The use of respiratory protective devices by workers was a potential confounder in the job exposure matrix. Until recently, there was little evidence of properly standardized or adequate respiratory protection and, in the past, only quarter-face masks with resin-impregnated felt filters had been widely available in this industry. There are many reports in the literature concerning the inadequacy of such respirators, both in terms of the penetration of dusts through the filter media and of the propensity for “face-seal” leakage. Furthermore, the use of these devices in the study plants appeared to be sporadic and there were few plant regulations requiring their use and little, if any, enforcement. Because of these factors, it was decided to ignore the earlier use of respirators in estimating exposures. Information regarding dates of well-designed and enforced respiratory protection programs was obtained during site visits and through discussions 211 with plant personnel. The National Industrial Sand Association’s (NISA) Occupational Health Program for Exposure to Crystalline Silica in the Industrial Sand Industry (OHP) includes provisions for establishing and maintaining respiratory protection programs, instituted by some plants as early as the mid-1970s. For most of these, the exposure database included information on respirator use during sampling periods. Thus it was usually possible to estimate frequency of use for a given job directly from the recorded data. Where no information was available, estimates of usage frequency were obtained from discussions with plant personnel and personal observation. Thus for a given job, the exposure estimate was adjusted as follows: C⬘ = C(1⫺f) + C 冉 冊 f , WPF where C⬘ is the exposure concentration corrected for respirator use, C is the estimated environmental exposure concentration, f is the frequency of respirator use (0ⱕfⱕ1), and WPF is the workplace protection factor of the respirator. A WPF of 5 was used in this calculation based on a literature survey of reported protection factors for particulate hazards (Harris et al., 1974; Smith et al., 1980; Toney and Barnhart, 1976). For those facilities where the exposure database included information on respirator use, personal exposures were adjusted for protection and frequency, and exposure averages (C⬘) were computed from the adjusted data. Where this information was not directly available, an estimate was made for each job, based on local inquiry. Development and application of the exposure matrix Job history profiles for cases and controls were collapsed into 244 unique job groupings distributed across the participating plants. The exposure matrix for a given job grouping was developed only for those Table 1. Values used in development of the exposure concentration conversion factor Microscopy particle size categories (µm) ⬍0.3 0.31–0.42 0.43–0.6 0.61–0.85 0.86–1.2 1.21–1.70 1.71–2.4 2.41–3.4 3.4–4.8 a Geometric mean of range (µm) Aerodynamic equivalent diameter, di (µm) Cyclone penetration efficiency,a eC,i Impinger/microscope sampling efficiency,b eI,i 0.21 0.36 0.51 0.72 1.02 1.43 2.03 2.86 4.05 0.34 0.59 0.83 1.17 1.66 2.33 3.30 4.66 6.59 1 1 1 1 1 0.99 0.77 0.24 0.015 0 0 0 0 1 0.85 0.8 0.74 0.72 Taken from Caplan et al. (1977). Taken from Drinker and Hatch (1936); adjusted for microscopic limit of resolution (苲1 µm). b 212 R. J. Rando et al. years where it appeared in job histories. In recent times, exposures were corrected for respiratory protection. These exposure estimates were taken as the arithmetic mean exposure calculated from the post1970 exposure monitoring database for an appropriate time segment in which the exposures were judged to be stable. This was determined by examination of the timing of changes in process, work practices, and controls and correlating their impact on exposure as indicated from temporal trends in the exposure monitoring data. In some cases, no changes or trends were identified and the mean of the entire database for that job was used as the exposure estimate. Exposures prior to the 1970s were handled in a similar way, except that the converted historical data were integrated into the estimates. The history of a given job and facility served to identify probable dates for any likely changes in exposure level. After that time, the oldest exposure estimates from the current exposure database were taken as representative; that is, exposure estimates derived from the data of the 1970s and beyond were extrapolated back to the point of the change. For periods before any recorded change, plant- and job-specific historical dust exposure data were used, after first being transformed into modern exposure units using the conversion algorithm. This specific approach was possible in three plants. For the others, plant-specific historical data were not available and geometric mean exposures, averaged across all plants in an industrywide historical database and broken down by various production areas, were calculated and assumed to be representative of exposure. Both the plant-specific and industry-wide estimates were then adjusted individually for the percentage silica prevalent in the dusts from particular production areas. Likewise for those time periods preceding the historical database (pre-1947), the exposure estimates derived from the historical data were assumed to be representative. For reported jobs in which no specific sampling was done and no specific information on the job’s tasks was available (for example, “labour” and “utility”), exposure was assumed to be equal to the overall mean of the exposure estimates for all production jobs in the facility. For each subject in the case-control study, average exposures to crystalline silica were then calculated by integrating the unique job histories with the jobexposure matrix, enabling cumulative exposures to be calculated using duration of employment/exposure. Thus, D= 冘 Ci⬘×ti and C̄⬘ = D 冘 ti where D is the cumulative exposure estimate, and C̄⬘ is the estimated average exposure, with Ci⬘ the exposure estimate over time period ti. RESULTS Historical descriptions of plants and processes from the industrial sand industry were identified in several trade reports (for example Rock Products, 1927; Sawyer, 1947; Mocine, 1948; Ayers and Crew, undated; further information about these can be obtained from the first author of the current paper). In the distant past, certain common process changes dramatically reduced exposure levels. In the modern era, controls generally resulted in lesser reductions in exposure. Table 2 is a listing of the more important and commonly-encountered process changes, broken down by general process area, especially important in bagging and bulk loading. For the years before 1970, the only quantitative exposure data discovered were those presented in four unpublished reports on studies undertaken by Professor Theodore Hatch on behalf of the Industrial Health Foundation of America, 1947 to 1955. These reports, details of which can be obtained from the first author, contained the results of approximately 400 samples from at least 19 sand-processing plants, three of which were in the present study. The other plants in the Hatch reports could not be identified, although probably some also are in the current study. The samples were collected with Greenburg–Smith impingers and were quantitated by microscopy. The industrial hygienist followed the workers around and placed the impinger samplers “within a few inches of the worker’s nose”; in areas where no specific dust source could be identified, such as in break rooms, area samples were collected. Table 3 presents a summary of the data reported by Hatch in his initial survey of 19 facilities in 1947. As a limit of 5 mppcf was proposed at that time, Table 3 suggests that there were excessive exposures throughout the industry. Most notable were drilling operations, screening, milling, and bagging and bulk loading in box cars of both sand and silica flour. It is also evident that there were large differences in dust levels for similar processes between plants. It is uncertain whether these were true differences or simply a reflection of the wide variability within plants and the relatively small number of samples examined. After about 1970, exposure databases were available for all plants in the study. For the most part, these represented reliable data collected by modern, state-of-the-art monitoring techniques. Most were the result of personal sampling in the breathing zone of workers, with the use of respiratory protection frequently recorded. Table 4 presents a summary of the exposure data obtained from the companies since 1973, showing that plant-wide geometric mean exposures to respirable crystalline silica ranged from 20 to 107 µg/m3 during this period. There were very Cohort mortality study of North American industrial sand workers. III 213 Table 2. Common process changes and controls that reduced historical exposure to crystalline silica in the American industrial sand industry Industrial sand process area/department Significant process changes Quarrying Change from dry-drilling to wet-drilling Replacement of secondary blasting/drilling with drop ball Air-conditioning and filtration of heavy equipment cabs Enclosure of primary crusher and construction of crusher operator control booth Replacement of chaser mills with rod mills (as exposure was low and the material wet, this common process change had little effect) Replacement of steam-coil with rotary kiln and fluid-bed dryers Enclosure and ventilation of screens Improved screens that require less brushing Installation of air filters and local exhaust hoods in operator booths Replacement of burlap bags with paper bags Replacement of bag-sewing with glueing Improvements in bagging machine design and ventilation Use of bagging station enclosures and air curtains Surface coating of filled bags with oil or water Use of automated palletizers and shrink wrappers Replacement of box cars with hopper cars and trucks Automation of loading process Local exhaust ventilation of loader chutes and mechanisms Paving and wetting of access roads and grounds Improved dust collection on local exhaust systems Upgrading of respiratory protection programs Crushing Wet processing Drying Screening Milling Bagging Bulk loading General Table 3. Historical exposure data for 19 industrial sand plants (taken from Hatch, 1947) Process area and operation Quarry Crushing Wet processing Drying Screening Milling Bagging Bulk loading Drilling Shovel Primary Secondary Leaching and dewatering Moist sand handling and storage Sand washing Rotary kiln Steam coil Drier screens Grading screens Personnel rooms Grinding mill Storage bins and upper levels Personnel rooms Bagging machines Box cars (sand) Hopper cars (sand) Flat cars (sand) Box cars (silica flour) Mean of means— plants [mppcf] Range of means [mppcf] Number of samples/number of means—plants 7.8 1.0 4.6 2.8 1.0 1.3 1.5 3.5 4.6 84 (GM=39) 42 (GM=7.9) 1.6 7.8 19.7 1.4 20 67 (GM=20) 3.3 11 91 (GM=12) 0.5–16 0.3–1.7 1.5–15 1.4–4.8 0.4–1.8 0.3–3.3 0.3–4.7 0.7–12 0.4–14 2–>170 1.0–220 ⬍2–3.8 0.6–40 1.0–77 0.6–2.6 5.0–60 1.8–350 1.5–5.0 0.3–5.0 0.8–180 9/4 5/3 18/8 9/4 11/4 17/9 28/10 24/10 33/9 31/12 38/6 5/– 25/9 23/9 12/5 25/8 22/9 3/2 3/2 5/2 GM: geometric mean of means. wide variations across job groupings within a given plant, with the highest levels generally seen in bagging and bulk-loading operations and the lowest among administrative personnel. Historical to modern dust conversion factors, computed according to the algorithm, are presented in Table 5 for the various processes studied by Severns (1979), with values ranging from 206 in an air sizing operation to 364 around vibrators. A Kruskall–Wallis ANOVA of the conversion factors across different areas showed no important difference (P = 0.61). An overall mean conversion factor of 276 µg/m3 per mppcf was therefore applied to all historical dust samples as follows: 214 R. J. Rando et al. Table 4. Exposure data obtained from the plants since 1973 Location/plant µg/m3—Respirable crystalline silica Years Number of samples Illinois/1 Illinois/2 New Jersey/1 New Jersey/2aa New Jersey/2ba Ohio/1 Ohio/2 West Virginia and Pennsylvania/1 West Virginia and Pennsylvania/2 Quebec 1 1974–1996 1976–1994 1974–1996 1975–1996 1979–1991 1975–1997 1974–1997 1973–1996 1973–1996 1978–1998 1493 608 1420 1064 199 263 336 3478 5143 2565/444b Total 1973–1998 14 249 Geometric mean (geometric standard deviation) 24 107 20 59 68 56 57 42 45 86 (9.2) (7.5) (9.2) (6.2) (3.0) (6.2) (6.8) (7.1) (5.1) (4.0) 42 (6.5) a New Jersey Plant 2 is in two neighboring locations, requiring separate assessment. Dust samples/silica samples. b Table 5. Historical–modern dust concentration conversion factors derived from the computational algorithm Average count median diametera (µm) Plant/process area Conversion factorb (µg/m3 per mppcf) n mean s.d. Drying Screening Air sizing Vibrators Bin room Bulk loading Bagging 0.46 0.45 0.45 0.38 0.56 0.36 0.31 4 1 2 2 1 1 3 292 252 206 364 276 344 297 128 – 3 5 – – 103 Overall 0.42 14 276 59 a Geometric mean particle size of respirable dust fraction collected with cyclone pre-separator. Kruskall–Wallis ANOVA, P=0.61. b µg/m3 (respirable crystalline silica) = [276]×[mppcf]×[% silica] DISCUSSION The percentage silica in the latter equation was derived from the average sample assay reported in the modern database for a given plant/area/job. In fact, the silica assays reported by Hatch were often taken from settled dust and appear extraordinarily high and are possibly unreliable. On the other hand, silica assays in the modern database are likely to be negatively biased, since high loadings derive primarily from particles released from the sand as it is being processed. Nevertheless, the conversion factor of 276 used in this paper is high compared to others reported previously. For example, Ayer et al. (1973) used a conversion factor of 110 for dusts from the Vermont granite sheds, and the ACGIH (1981) recommended a conversion factor of 167 for dusts in which the density and mass median diameter are unknown; Tomb and Haney (1988) reported a range of 46 to 313 for various mineral dusts; and Seixas et al. (1997) suggested factors ranging from 90 to 180 for the diatomaceous earth industry. Although a conversion factor of 276 may be positively biased to some (unknown) extent, the use of this conversion factor, which we developed specifically for the industrial sand industry, was deemed preferable in our judgement to using data derived from other unrelated industries. In any case, any bias in conversion should be internally consistent and apply equally to cases and referents in the epidemiological analysis (Hughes et al., 2001). For each of the 342 workers in the case-referent study, annual exposure estimates were calculated by coupling their job history for a given year with the job-exposure matrix. Annual average exposure levels Cohort mortality study of North American industrial sand workers. III 215 Fig. 1. Mean exposure levels and numbers of workers in the case-referent study present for each year in the study period. ranged from approximately 400 to 500 µg/m3 in the 1930s and 1940s, falling to less than 50 µg/m3 in the late 1980s (see Fig. 1). It must be remembered that the data are representative only of job titles actually recorded in the work histories of cases and referents and, as such, are not necessarily representative of industry-wide exposures for any given year. 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