Document qmJXJzO5oX0Zjgj4eKkGDxzKx
AIHAJ 61:881894 (2000)
Ms. #158
AUTHORS Daniel J. Caldwell Thomas W. Armstrong Neil J. Barone Joseph A. Suder Malcolm J. Evans
ExxonMobil Biomedical Sciences, Inc., 1545 Route 22 East, P.O. Box 971, Annandale, NJ 088010971
Hydrocarbon Solvent Exposure Data: Compilation and Analysis of the Literature
An occupational exposure database for hydrocarbon solvent end-use applications was constructed from the published literature. The database provides exposure assessment information for such purposes as regulatory risk assessments, support of industry product stewardship initiatives, and identification of applications in which limited exposure data are available. It is quantitative, documented, and based on credible data. Approximately 350 articles containing quantitative hydrocarbon solvent exposure data were identified using a search of computer databases of published literature. Many articles did not report sufficient details of the exposure data for inclusion in the database (e.g., full-shift exposure or task-based exposure data). Others were excluded because only limited summary statistics were provided, which precluded statistical analysis of the data (e.g., arithmetic mean concentration presented, but no sample number). Following evaluation, 16,880 hydrocarbon solvent exposure measurements from 99 articles were entered into a database for analysis. Methods used to identify and evaluate published solvent exposure data are described along with more detailed analysis of worker exposure to hydrocarbon solvents in three major end-use applications: painting and coating, printing, and adhesives. Solvent exposures were evaluated against current ACGIH threshold limit values (TLVs) and trends were identified. Limited quantitative data are available prior to 1970. In general, reported hydrocarbon solvent exposures decreased fourfold from 1960 to 1998, were below the TLVs applicable to specific hydrocarbon solvents at the time, and on average have been below 40% of the TLV since 1980. The database already has proved valuable; however, the utility of published exposure data could be further improved if authors consistently reported essential data elements and supporting information. Keywords: exposure assessment, exposure database, hydrocarbon solvent, occupational exposure, organo-psycho syndrome (OPS), TLV
APPLIED STUDIES
Funding for this project was provided by the Hydrocarbon Solvents Producers Association (HSPA) of the European Chemical Industry Council and by the Hydrocarbon Solvents Panel of the American Chemistry Council, formerly the Chemical Manufacturers Association (CMA).
Copyright 2000, AIHA
Numerous epidemiological studies have been conducted over the years to investigate the potential impact of solvents on the health of exposed workers. In many of these studies, there were difficulties in completing an adequate exposure assessment. This limits the usefulness of the studies because good exposure data are an essential part of quantitative risk evaluations. For example, organopsycho syndrome (OPS), also known as painter's syndrome, is characterized by neurobehavioral effects that include changes in psychomotor skills, attention, learning, and memory. OPS can
occur in workers as a result of excessive longterm exposure to solvents. Epidemiology studies of OPS often contain assumptions regarding workplace exposure because the intensity and duration of exposure has been difficult to quantify. This is because historic exposure data are rare; a mixture of solvents often is used, making exposure assessment difficult; and both the solvents and the working conditions change over time. However, good exposure data are essential if the relationship between long-term exposure to solvents and health effects (e.g., OPS, reproductive or developmental effects) is to be adequately defined. A comprehensive database of
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FIGURE 1. Number of papers by decade
APPLIED STUDIES
solvent exposure data would improve exposure assessments and therefore contribute to the understanding of health risks.
A critical evaluation of the published exposure data will provide an important input to both the on-going public debate on the health effects of solvent exposure and to regulatory risk assessments. Furthermore, information about the potential exposure to solvents in user industries is important in determining whether occupational exposure limits are, in fact, adequately protective. Quantitative exposure information also will assist in the prioritization of product stewardship efforts by identifying the need for safe handling procedures. Lastly, the accuracy of predictions from exposure modeling can be validated using measured solvent exposure data collected from a range of exposure scenarios.
METHODS
Literature Search Strategy
A stepwise approach was developed to compile and critically review available published data on exposure to hydrocarbon solvents in user industries. Initially, a broad search of the computer databases was undertaken using key solvent and petroleum terms. That search showed approximately 1.7 million articles containing the key search terms, but many were obviously irrelevant (for example, ``Waxing Poetic on the Works of Shelly,'' or ``Varnished Tales: History and Artifice in the Novel, 17891830'').
The next stage used improved search terms to limit irrelevant results and limited the search to articles published between 1996 and 1998 and possibly containing data on exposure to hydrocarbon solvents in user industries. The search included terms for specific industries (e.g., automotive, printing), solvent products (e.g., paint thinner, mineral spirits), components (e.g., cyclohexane, benzene, toluene, xylene), and branched, cyclic, and straight chain
alkane solvents with carbon numbers between 5 and 15, using Chemical Abstract Service registry numbers and focused nomenclature. The search also included exposure terms to cover personal breathing zone and general area samples. The search identified 22,000 articles. Restricting the search to occupational exposure in selected industries reduced this to 6000 articles. After examination of the titles, abstracts were obtained for 250 (4%). Review of the abstracts suggested 50 (20%) were relevant and the full publications were obtained. A review of these 50 publications indicated approximately one-half of them contained useful data.
This appeared to be a reasonable methodology for identifying the relevant articles. Therefore, the refined search strategy was applied without time limits and resulted in the identification of additional relevant articles. After the computer search, further articles potentially containing useable data were identified from references cited in articles reviewed. This technique served two purposes: It targeted resources to journals that routinely published sampling data, and it enabled additional historic data to be obtained, as the computer databases contain little information prior to the 1970s.
Database Assembly
The relevant data from each article were entered into a Microsoft Access database for subsequent analysis. The database was designed so that the data collected could be analyzed in a flexible manner. The appendix shows the database structure and provides brief descriptions of the database fields. An examination of the database structure reveals numerous database fields (e.g., PPE). However, this report discusses the analysis of only the personal breathing zone sample results.
The focus of this project was on articles containing hydrocarbon solvent exposure data; however, if other (nonhydrocarbon solvent) data also were reported in the same article, these data
882 AIHAJ (61) November/December 2000
TABLE I. Summary of Personal Breathing Zone Sample Results for Hydrocarbon Exposure Indicators
Exposure Indicator
IBPA PapersB SingleC AMC
nC
Total ND
WAME MINF MAXF
PentaneA Rubber solvent naphthaA HexanesA HexaneA BenzeneA CyclohexaneA VM&P naphtha HeptaneA Toluene Octane Ethyl benzene Xylene White Spirit/Stoddard Solvent Nonane Propyl benzene C10C12 HC Trimethyl benzene Total volatile HC
Total
36 2 7 32 196 203 9.5 0 567
45 1 8
8 263.0 0 584
50 1 2
2 0.7 0
0.7
69 19 86 65 1223 1309 92.9 0 1426
80 9 18 44 719 737 8.4 0 765
81 4
5
301
301 159.8
0 1288
95 3
11
267
267 47.5
0 9640
98
9 25 36
370
395 36.6
0 1291
111
53 168 138
5097
5265
98.7
0 6236
126 3
2 28 28 0.02 0 0.2
136 11
4 26
781
785 14.1
0 104
138 38 95 91 3548 3643 32.8 0 2218
150 10 30 25
370
400 466.5
0 2231
151 3
2 28 28 0.2 0 2
152 2
6 178 178 0.2 0
1
174 4
5 96 96 1.8 0 10
176 4 1 1 70 71 4.1 0 15
N/A 21 84 53 1594 1678 66.7 0 1483
528 542 14866 15394
75.1
0 9640
AIBP is initial boiling point in C, which is an indicator of volatility. BNumber of citations containing data on particular exposure indicator (multiple exposure indicators may be reported in one article). CDiscrete sample data point, whereas AM & n indicate the arithmetic mean value and corresponding number of samples. DTotal number of sample data points represented by the weighted arithmetic mean (WAM) in mg/m3. EThe WAM exposure in mg/m3. FMIN & MAX indicate the range of values reported in the literature, in mg/m3. G1996 ACGIH 8-hr TWA, in mg/m3, rounded to the nearest whole number. H% TLV is the WAM divided by the 1996 TLV.
TLVG
1771 1590 1762
176 32
1033 1371 1639
188 1402
434 434 525 1049 246 N/A 123 N/A
% TLVH
0.5 17
0.1 53 26 15
3 2 52 0 3 8 89 0.02 0.1
3.3
APPLIED STUDIES
were entered into the database. Thus, summary data representing over 33,500 data points were entered into the exposure database. Articles covering 27,000 data points had enough information to permit statistical analysis; of these, 16,880 data points were for hydrocarbon solvents; and of these, 15,394 were personal breathing zone samples.
Other solvent exposures captured in the database but not evaluated or discussed in this report include acetone (3200), styrene (2900), various alcohols (1600), acetates (1500), and other ketones (1300). Limited data on other solvents and chlorinated hydrocarbons are also included in the database.
TABLE II. Change in ACGIH TLVs by Year for Selected Constituents
TLV
Solvent
Year mg/m3 ppm
Benzene
1948 1957 1974 1997
112 80 32 1.6
35 25 10
0.5
Ethyl benzene
1948 1967
868 434
200 100
n-Hexane
1948 1976 1982
1762 352 176
500 100
50
Propyl benzene (cumene)
1967
246
50
Toluene
1948 1973 1992
754 377 188
200 100
50
Trimethyl benzene
1970
123
25
Xylene
1948 1967
868 434
200 100
Approximately 20% of the articles presented limited summary statistics (i.e., the authors presented the arithmetic mean [AM] but no sample number, or presented the geometric mean [GM] but no geometric standard deviation [GSD], or presented the GM and GSD, but no ``n''), thus precluding statistical analysis of the data.
Quality Assurance on Data Entry
An industrial hygienist who was not involved in the primary data entry verified the integrity of the entries. This was accomplished during preliminary analysis of the data by checking the summary statistics, such as GM, AM, and number of samples from the original articles. During further work to combine specific process categories into broader industrywide categories, the number and type of samples, sample duration, and sample results were comprehensively verified. The project sponsors also verified the final analyses of the database contents.
RESULTS
During this project, 99 articles published between 19611998 were critically reviewed and exposure data entered into the database. Full citations are contained in the bibliography.
Hydrocarbon solvents can consist of individual chemicals (e.g., xylene or toluene), but often contain a large number of individual chemical species. To account for different ways exposure data were reported by the various authors, the concept of an exposure indicator was developed. For the purpose of this study, the term ``exposure indicators'' is defined as measured analytes that are constituents of, or surrogates for, the constituents of the solvent. This project identified a total of 77 solvent exposure indicators. However, even this approach presents problems when the exposure was to a mixture of solvents, or to a complex hydrocarbon solvent for
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APPLIED STUDIES
FIGURE 2. Average concentration and average %TLV of PBZ results by decade
FIGURE 3. Average concentration of PBZ results as percentage of 1996 TLV by industry 884 AIHAJ (61) November/December 2000
APPLIED STUDIES
FIGURE 4. Average concentration of PBZ results by process
FIGURE 5. Average concentration as percentage of 1996 TLV by exposure indicator AIHAJ (61) November/December 2000 885
FIGURE 6. Average concentration by exposure indicator
APPLIED STUDIES
which each exposure indicator result represented only part of the overall (total hydrocarbon) exposure. The remainder of this report is concerned only with the analyses conducted on the hydrocarbon solvent exposure indicators, which represented 35 of the 77 exposure indicators.
Age and Origin of Articles
Figure 1 shows the number of articles by decade of publication. Most of the articles in the database (80%) were published within the past 20 years. All 6 articles published during the 1960s were by American authors, whereas 9 of 12 articles published in the 1970s were by European authors. The increase in the total number of articles published probably reflects an increased interest and concern regarding occupational exposure to solvents throughout Europe and North America and the parallel development of the science of occupational hygiene.
Overall Analysis of Hydrocarbon Solvent Data
Table I presents a summary of the personal breathing zone (PBZ) hydrocarbon solvent data, by exposure indicator. Certain exposure indicators were grouped together, such as White Spirit with Stoddard Solvent, C10-C12 hydrocarbons, and hexanes (other than nhexane) to facilitate analysis.
The majority of solvent exposures were below the relevant occupational exposure limit (OEL) for each exposure indicator. The 1996 American Conference of Governmental Industrial Hygienists (ACGIH) threshold limit values (TLVs) were selected as the referent OELs for this analysis for several reasons: The vast majority of the authors compared their results with the ACGIH TLV,
changes in the value of the TLV over time are well documented and readily available, and the benzene TLV significantly changed in 1997 (i.e., a 20-fold decrease).
Use of the new benzene TLV would inflate the %TLV calculation and would not accurately portray the level of compliance with the TLV in effect at the time of the study.
Table II presents the values of the ACGIH TLVs as they changed over time for selected hydrocarbon solvents/components. Figure 2 summarizes the weighted arithmetic mean (WAM) solvent exposure concentration by decade and the total number of solvent samples by decade:
WAM
n1 AM1
n2 AM2
n
nn AMn
n
1
where WAM weighted arithmetic mean; n number for measurements for the AM in a particular report; and AM the arithmetic mean of the data for a particular report.
The %TLV for Figure 2 was calculated in a multistep process. First, the %TLV for each sample result was determined by dividing the sample concentration by the TLV for the exposure indicator in effect during the year of publication. Next, the average %TLV for all samples in a given year was calculated. Finally, the weighted average of the %TLV for all years in a given decade was calculated.
A review of Figure 2 indicates that, in general, data prior to 1980 are limited. Further, where available, the reported hydrocarbon solvent exposures were considerably higher in the 1970s compared with subsequent decades in terms of both average concentration and average %TLV.
886 AIHAJ (61) November/December 2000
TABLE III. Reported Exposures Greater Than the TLV, Sorted by Year of Publication
Year Industry
Process
1978 1978 1980 1980 1985 1986 1986 1987 1987 1987 1991 1991 1991 1991 1992 1992 1993 1994 1994 1994 1994 1994 1995 1995 1995 1996 1996 1997
printing shoe auto auto printing flooring printing printing rubber rubber auto auto auto leather auto shoe auto printing printing printing printing printing paint/coating printing shoe furniture printing fiberglass
gravure nonspecific paint/coating application paint/coating application nonspecific adhesive application gravure nonspecific nonspecific rubber mixing paint/coating application paint/coating application paint/coating application tanning paint/coating application adhesive application nonspecific ink mixing nonspecific nonspecific solvent cleaning solvent cleaning paint mixing nonspecific adhesive application paint/coating application nonspecific fiberglass molding
Note: AEI is exposure indicator. B% TLV calculated based on ACGIH TLV at date of publication. CN is number of samples for specific EI reported in publication on which calculation is based.
EI NameA
toluene hexane toluene xylene hexane benzene toluene toluene toluene toluene benzene toluene xylene hexane toluene toluene toluene toluene toluene xylene toluene xylene hexane toluene toluene toluene toluene toluene
% TLVB
149 155 205 158 169 497 125 751 130 127 530 172 231 119 148 384 266 172 424 135 1409 135 130 498 169 382 199 130
NC
53 65 61
9 12 10 53
2 83
5 9 61 9 23 9 7 21 13 282 6 5 5 119 110 7 5 64 23
APPLIED STUDIES
Figure 2 indicates that the published hydrocarbon solvent exposure concentrations have decreased more than fourfold from the 1970s to the 1980s and 1990s--from an average of approximately 300 mg/m3 to less than approximately 70 mg/m3. The number of samples collected in the 1980s and 1990s increased by an order of magnitude compared with the 1970s. Over the same time period, the average %TLV decreased--from 93% in the 1970s, to 16% in the 1980s, to 37% in the 1990s. These findings suggest that exposures have been reduced in response to new information regarding health effects of solvents as reflected by reductions in the TLV for key hydrocarbon solvent components. The trend of adopting lower TLVs is also apparent by the increase of the average %TLV from the 1980s to the 1990s; the average %TLV in the 1990s was double that of the 1980s even though the average exposure concentrations were the same.
Analysis of Solvent Exposures by Industry and Process
The data were analyzed by both industry and process. The results are summarized in Figures 3 and 4, which present the average solvent concentration as a percentage of the 1996 TLV along with the number of samples.
Figure 3 suggests that the highest exposures occurred in the flooring industry. There were also significant exposures (average 50% of the 1996 TLV) in the fiberglass, paint/coating, construction, shoe, petroleum, marine, leather, and shoe industries, although the number of samples was low for some of these. Industries with the highest number of samples tended to have lower reported solvent exposures; all six industries with over 500 data points each had average concentrations below 50% of the TLV.
The fiberglass industry had high styrene exposures that are not discussed further in this report. However, there also were significant toluene exposures in the fiberglass industry; these toluene exposure data were used in the analyses that follow.
Figure 4 shows the specific processes associated with solvent exposure. Rubber spreading had the greatest reported exposure concentrations but may not reflect typical exposures, given the small number of samples reported.
Figures 3 and 4 show that hydrocarbon solvents are used in a very wide range of industries and processes. Average exposures and the number of data points vary considerably between industry and process. In many applications exposure would appear to be well controlled, whereas in others exposure potential is clearly higher.
Analysis by Solvent/Exposure Indicator
Figure 5 summarizes the hydrocarbon solvent personal breathing zone exposure data contained in the database by presenting the average percentage of the 1996 TLV and number of samples for the hydrocarbon solvent exposure indicators of interest. With the exception of Stoddard Solvent/White Spirit, toluene, and n-hexane, all of the average %TLV numbers are below 50% of the respective TLV (also shown in Table I). Note that the solvent exposure indicators are listed by increasing initial boiling point, which is indicative of relative volatility.
The airborne exposure concentration would be expected to decrease as the boiling point increases. Figure 6 confirms that the measured average concentrations generally are inversely related to initial boiling point. The notable exception is Stoddard Solvent/ White Spirits. The reason in unclear, but perhaps is related to its
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TABLE IV. Reported Exposures Greater Than One-Half the TLV, Sorted by Year of Publication
Year Industry
Process
EI NameA
1978 1980 1980 1985 1985 1985 1986 1986 1987 1987 1987 1991 1991 1991 1992 1992 1992 1993 1993 1994 1994 1994 1995 1995 1995 1996 1996
printing auto rubber printing printing printing flooring printing printing rubber rubber auto auto nonspecific auto nonspecific paint/coating auto printing aeronautic printing rubber auto nonspecific printing printing printing
gravure paint/coating application rubber curing nonspecific nonspecific nonspecific adhesive application gravure nonspecific nonspecific rubber spreading paint/coating application paint/coating application paint/coating application paint/coating application nonspecific nonspecific nonspecific gravure paint/coating application nonspecific paint/coating application paint/coating application paint/coating application nonspecific gravure nonspecific
toluene xylene hexane hexane toluene xylene toluene toluene toluene toluene toluene benzene xylene xylene toluene hexane toluene xylene toluene toluene toluene toluene toluene xylene toluene toluene toluene
Note: AEI is exposure indicator. B% TLV calculated based on ACGIH TLV at date of publication. CN is number of samples for specific EI reported in publication on which calculation is based.
% TLVB
82 62 58 78 78 87 54 69 58 53 54 68 80 69 58 80 62 79 67 80 65 83 82 81 80 77 92
NC
48 23 19 26
2 6 8 48 26 202 30 70 52 29 23 49 396 21 53 23 1368 5 9 29 172 53 46
APPLIED STUDIES
widespread use in open applications (e.g., painting/coating and parts cleaning).
Tables III and IV present data for specific industries and processes in which the average solvent concentrations were greater than the TLV (Table III), or between one-half of the TLV and the TLV (Table IV) in effect at the time of publication. These data are sorted by year of publication.
It is clear from Tables III and IV that many of the higher exposures reported in the literature occur to n-hexane, toluene, and xylene in the auto industry (during paint/coating applications) and in the printing industry. High concentrations of benzene also were reported in several older articles; however, solvents currently marketed in Europe and the United States contain less than 0.1% benzene.
Analysis of Exposure in Adhesive, Paint/Coating, and Printing Applications
Of the 15,394 hydrocarbon solvent PBZ sample data points, a subset representing sample results for the adhesive, printing, and paint/coating applications (three major current uses of hydrocarbon solvents) was selected for detailed analysis.(1) This analysis is summarized in the following paragraphs.
The main hydrocarbon solvent exposure indicators reported for three applications were: adhesive--toluene, xylene, hexane, cyclohexane, and naphtha; paint/coating--toluene, xylene, ethyl benzene, benzene, hexane; and printing--benzene, ethyl benzene, xylene, and toluene.
The average solvent concentration in the printing application
appears to indicate a steady downward trend over time. Similar marked trends are not evident for adhesives and paint/coating applications. For the latter, more recent articles seem to indicate lower exposures. This could be due to improved exposure controls or the introduction of modern paint formulations containing less solvent (e.g., ``high-solids'' and ``water-based'' paints).
Review of Semiquantitative Articles
In addition to the quantitative data assembled in the database, approximately 20 publications detailed exposures in adhesives, painting, or printing industries usefully, but in insufficient detail, or in units difficult to abstract for inclusion in the database. Several of the publications in the database also contained additional qualitative information useful for evaluating historical trends. These publications provide some additional information about total solvent (rather than just exposure indicator compound) exposures. Conclusions that can be drawn from these articles follow.
Adhesives
Limited data were provided in two articles. Ekberg et al.(2) found for floor layers that the mixture (additive effects) formula showed exposures of 1.8 versus the mixture limit of 1.0. Mutti et al.(3) showed an exposure for shoe gluing of 1.5 for the solvents as a mixture, versus the mixture limit of 1.0. These semiquantitative articles are in agreement with the quantitative data discussed earlier in this article. Ekberg et al.(2) further commented that exposures ``were higher'' (p. 105) in the 1950s and 1960s when more solvent-based glues were used. The longer-term data (243 to 317 min) presented as fraction of the TLV showed water-based glue
888 AIHAJ (61) November/December 2000
TABLE V. Summary of Semiquantitative Papers for the Paint Industry
Operation
Total Solvent Exposure, as Fraction of TLV
Hanninen 1976 Elofsson 1980A Elofsson 1980A Riala 1984A
Maizlish 1987
Triebig 1988
car spray paint industrial spray painting car spray painting house type painting, interior,
poor ventilation spray painting and spray
gluing house painters
0.32 0.24 0.3 0.91
0.09
0.53
Triebig 1992A
spray painters
0.92
ADenotes article in the database.
Comments
mainly aromatics and white spirit mainly aromatics, ketones, trichloroethylene mainly aromatics, white spirits, ketones solvent naphtha (calculated with 300 ppm
TLV) mainly aromatics, aliphatics, ketones
as given by Triebig; mainly aromatics, acetates, ketones
calculated from Triebig's data; mainly aromatics, aliphatics
APPLIED STUDIES
exposures (additive mixture calculations) of 0.02 and 0.03, but for work including solvent-based adhesives the results were 0.2 to 0.5. The authors further comment that water-based glues were introduced in the 1970s.(2)
Painting
Of the 13 additional articles reviewed on painting operations, six provided insights on total solvent exposure.(49) Range or other variance measures generally were not given with the summary statistics. Key results are presented in Table V as a fraction of the TLV (additive effects, mixture calculation).
Nelson et al.(10) provide an assessment of solvent exposures in an automotive assembly operation, including assessments by decade from the 1950s to the 1980s. Unfortunately, the assessment is aggregated, and not available by operation; degreasing, painting, and other solvent uses are grouped together. Recognizing that these data are of uncertain applicability, the trends are presented in Table VI.
Note that Nelson et al.(10) reported data for aliphatic hydrocarbons; gasoline; heptane; kerosene; VM&P naphtha (a total of 81 data points); and petroleum distillates, not further defined (a total of 286 data points). Presumably, the petroleum distillates are other fractions not reported individually.
Printing
Five articles provided useful information about exposures in printing operations. Of particular note, two articles(11,12) assessed toluene exposures over time. Orbaek's and Nise's earliest data were from 1969, although estimates are provided back to the 1950s.(12) The time trends from these articles indicate toluene exposure decreased from 300450 ppm in the 1960s to 5070 ppm by the mid- to late 1980s. These trends are in agreement with the quantitative data in the database as already discussed.
Several additional studies derived from the epidemiology literature were identified. These provided estimates of exposure to
house painters; however, since they lacked any quantitative information they were not included in the semiquantitative articles review.
Summary of Review of Semiquantitative Articles
These articles contain data that would have been a valuable addition to the quantitative database if adequate details had been reported. A limited number of articles were published prior to 1970; the data they contain are inadequately characterized. However, review of qualitative data reported in the 1960s revealed potentially high exposures. Thus, these articles are informative and give likely ranges of past exposure. However, they are not necessarily indicative of typical worker exposures.
DISCUSSION
Articles published prior to the 1970s usually contained incomplete descriptions of the sampled operation and employed a plethora of reporting approaches. Even at present, there is a wide range in the details provided that restricts the ability to combine data sets for further analysis. Authors often reported ``average concentrations,'' without reporting the number of samples, duration of sample, and so forth. These practices limited any meaningful statistical analysis. More consistent and more detailed descriptions of the sampling survey rationale, operating conditions (routine and typical versus worst case or upset conditions), and other exposure descriptors would help improve the utility of published articles and occupational exposure databases. The essential data elements have been described by Rajan et al.(13) and the Joint ACGIH-American Industrial Hygiene Association Task Force.(14)
There is an upward trend in the number of reported exposure measurements from the 1970s to the present, with a corresponding downward trend in the reported hydrocarbon solvent exposures. Although the date of publication may not in all cases reflect
TABLE VI. Trends of Solvent Exposure in Automotive Assembly Operations
Units: ppm
1950s
1960s
Petroleum distillates VM&P naphtha
26 (n 12) range 21000 17 (n 25) range 3200
275 (n 62) range 04000 325 (n 7) range 125548
Source: Nelson et al., 1993.
1970s
5 (n 22) range 2290 92.5 (n 10) range 3380
1980s
15 (n 190) range 01890 5 (n 39) range 22110
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APPLIED STUDIES
the date of sampling, hydrocarbon solvent exposure indicator average concentrations were generally below the TLVs applicable at the time of publication. Furthermore, TLVs for some key hydrocarbon solvent exposure indicators have been reduced considerably since the 1960s.
As indicated in Figure 2, occupational exposures to individual exposure indicators are, on average, below 40% of the TLV for results reported since 1980. However, exposure to more than one exposure indicator (i.e., chemical substance) can occur at the same time. To calculate an OEL for such mixtures or blends of hydrocarbons, a reciprocal calculation procedure (RCP) that uses the OELs of constituent compounds is most appropriate.(15,16) ACGIH has described the use of the RCP to calculate exposure limits for mixtures for 60 years. Proposed OEL guidance values for hydrocarbon solvents, based on the RCP, recently were adopted by the European Hydrocarbon Solvents Producers Association.(17)
This database can be used as a ``reality check'' on the exposure estimates used in epidemiology studies that allege effects and report only subjective, qualitative estimates of solvent exposure by extracting data for specific industries, solvents, or time periods. Approximate RCP-based historic hydrocarbon solvent exposures can be estimated from the information in this database.
Evaluated overall, most exposure data are related to benzene, toluene, xylene, n-hexane, and ethyl benzene. This likely reflects concern over the unique toxicity exerted by some of these materials (i.e., benzene and blood effects, n-hexane and peripheral neuropathy). Industry and government regulations have responded to these concerns. The benzene concentration in solvents is now less than 0.1% and use of n-hexane in solvents is much reduced.
This exposure database can be used to validate existing exposure estimating models and future models that may be under development.
7. Maizlish, N.A., L.J. Fine, J.W. Albers, L. Whitehead, and G.D. Langolf: A neurological evaluation of workers exposed to mixtures of organic solvents. Bri. J. Ind. Med. 44:1425 (1987).
8. Triebig, G., D. Claus, I. Csuzda, K.-F. Druschky, et al.: Crosssection epidemiological study on neurotoxicity of solvents in paints and lacquers. Int. Arch. Occup. Environ. Health 60:233241 (1988).
9. Triebig, G.: Neurotoxicity of solvent mixtures in spray painters. Int. Arch. Occup. Environ. Health 64:353359 (1992).
10. Nelson, N.A.: Historical characterization of exposure to mixed solvents for an epidemiologic study of automotive assembly plant workers. Appl. Occup. Environ. Hyg. 8:693702 (1993).
11. Svensson, B.-G.: Hormone status in occupational toluene exposure. Am. J. Ind. Med. 22:99107 (1992).
12. Orbaek, P., and G. Nise: Neurasthenic complaints and psychometric function of toluene-exposed rotogravure printers. Am. J. Ind. Med. 16:6777 (1989).
13. Rajan, B., R. Alesbury, B. Carton, M. Gerin, et al.: European proposal for core information for the storage and exchange of workplace exposure measurements on chemical agents. Appl. Occup. Environ. Hyg. 12:3139 (1997).
14. Joint ACGIH-AIHA Task Group on Occupational Exposure Databases: Special report. Data elements for occupational exposure databases: Guidelines and recommendations for airborne hazards and noise. Appl. Occup. Environ. Hyg. 11:12941311 (1996).
15. European Centre for Ecotoxicology and Toxicology of Chemicals (ECETOC): Occupational Exposure Limits for Hydrocarbon Solvents (Special report no. 13). Brussels, Belgium: ECETOC, 1997.
16. Health and Safety Executive, United Kingdom (HSE): Occupational Exposure Limits (Report EH 40/96). London: HSE, 1996.
17. Daughtrey, W.C., A.M. Medeiros, C.S. Nessel, M.J. Evans, and D.E. Owen: ``Documentation for Proposed Group Guidance Values for OEL Setting for Hydrocarbon Solvents'' (Report prepared for CEFIC Hydrocarbon Solvents Producers Association). 1999. Exxon Biomedical Sciences, Inc., 1545 Route 22 East, P.O. Box 971, Annandale, NJ 08801-0971.
ACKNOWLEDGMENTS
The authors acknowledge the HSPA Occupational Health Task Force, particularly Dr. Tom Farmer and Mr. Doug Rhodes, and Ms. Janet Catanach of the ACC Hydrocarbon Solvents Panel, who reviewed a draft of this manuscript and provided helpful comments and guidance.
REFERENCES
1. Caldwell, D.J., T.W. Armstrong, N.J. Barone, and J.A. Suder: ``Hydrocarbon Solvent Exposure Assessment'' (Report prepared for CEFIC Hydrocarbon Solvents Producers Association). 1998. Exxon Biomedical Sciences, Inc. 1545 Route 22 East, P.O. Box 971, Annandale, NJ 088010971.
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APPLIED STUDIES
892 AIHAJ (61) November/December 2000
TABLE A1. Database Table-Field Descriptions
Table
Field
TblApplication TblAuthor tblCitation
ApplicationID Application CitationID CitationID AuthorLast AuthorInitial CitationID Title JournalName JournalVolume JournalPageStart JournalPageEnd JournalYear Language
Country StudyReason
tblControl tblExposureIndicators
tblPPE tblSampleResults
DataQuality Abstract ApplicationID Control ApplicationID ExpIndID NoSamples NoExposed RefVal Unit Source Type ApplicationID PPE SampleNo ApplicationID ExpIndID Strategy Type SampleMethod
tblSolventExpInd tblSolventsUsed
AnalyticalMethod Duration Single AM GM Unit NoSamples StdDev GSD Min Max ApplicationID SolventID SolventName ExpIndID ApplicationID SolventID SolventName NoSamples NoExposed
Description
unique application identification number end use application (e.g., spray painting) link to citation link to citation last name of author initials of author unique citation identification number title of journal article name of journal volume of journal first page of range of pages article found on last page of range of pages article found on date of journal issue language of reference text country where study was performed reason sampling was done (worker complaint, regulatory compliance,
exposure assessment, process change) study quality (1, 2, or 3) good, fair, poor journal abstract link to citation and end use application type of engineering control used to reduce exposure link to citation and end use application exposure indicator ID number of sample results provided for this solvent number of individuals exposed (not necessarily sampled) reference value used in study unit of measurement for RefVal (ppm or mg/m3) organization which established RefVal (e.g., ACGIH TLV or OSHA PEL) TWA, STEL, or CEILING link to citation and end use application type of personal protective equipment used by workers to reduce exposure unique identification for sample link to citation and end use application link to exposure indicator sample strategy (worse case, targeted, random) sample type (PBZ or Area) sample collection method (pump & tube, diffusive monitor, direct reading
instrument, etc.) reference to standard analytical method used (NIOSH, OSHA, etc.) sample collection period in minutes single sample result concentration arithmetic mean geometric mean unit of measure number of samples if result is mean standard deviation if result is mean geometric standard deviation minimum of range if result is mean maximum of range if result is mean link to citation and end use application link to solvent look-up table (tlkpSolvents) link to solvent name (tlkpSolvents) exposure indicator ID link to citation and end use application link to solvent look-up table (tlkpSolvents) category of solvent name of the solvent (product) used number of sample results provided for this solvent number of individuals exposed (not necessarily sampled)
APPLIED STUDIES
AIHAJ (61) November/December 2000 893
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FIGURE A1. Database structure 894 AIHAJ (61) November/December 2000