EPA-600/1-77-004
                                            January 1977
  AN ASSESSMENT OF THE CHESS SULFATE AND NITRATE DATA

during the period RETA performed the chemical analysis
                          by

                 Leo T. Heiderscheit
        Statistics and Data Management Office

                         and

                   Marvin B. Hertz
              Population Studies Division
          Health Effects Research Laboratory
          Research Triangle Park, N.C. 27711
         U.S. ENVIRONMENTAL PROTECTION AGENCY
          OFFICE OF RESEARCH AND DEVELOPMENT
          HEALTH EFFECTS RESEARCH LABORATORY
          RESEARCH TRIANGLE PARK, N.C. 27711

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                               DISCLAIMER

      This report has been reviewed by the Health Effects Research Laboratory,
U.S. Environmental  Protection Agency, and approved for publication.   Mention
of trade names or commercial  products does not constitute endorsement or
recommendation for use.

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                                  FOREWORD
     The many benefits of our modern, developing, industrial  society are
accompanied by certain hazards.   Careful  assessment of the relative risk
of existing and new man-made environmental  hazards is necessary for the
establishment of sound regulatory policy.   These regulations  serve to
enhance the quality of our environment in  order to promote the public
health and welfare and the productive capacity of our Nation's population.

     The Health Effects Research Laboratory, Research Triangle Park
conducts a coordinated environmental  health research program  in toxicology,
epidemiology, and clinical studies using  human volunteer subjects.  These
studies address problems in air pollution,  non-ionizing radiation,
environmental carcinogenesis and the  toxicology of pesticides as well as
other chemical pollutants.  The Laboratory develops and revises air quality
criteria documents on pollutants for  which  national ambient air quality
standards exist or are proposed, provides  the data for registration of new
pesticides or proposed suspension of  those  already in use, conducts research
on hazardous and toxic materials, and is  preparing the health basis for
non-ionizing radiation standards.  Direct  support to the regulatory function
of the Agency is provided in the form of  expert testimony and preparation of
affidavits as well as expert advice to the  Administrator to assure the
adequacy of health care and surveillance  of persons having suffered imminent
and substantial endangerment of their health.

     This study addresses a concern regarding some of the air pollution
measurements collected in the CHESS air monitoring system.  Severe manpower
limitations forced the Health Effects Research Laboratory to contract for
the ctremical analysis of high-volume  filter strips.  Some measurement
effects resulted, and this paper investigates the nature of the differences
and recommends an appropriate procedure.
                                                H.  Knelson,  M.D.
                                               >Director,
                                     Health  Effects  Research Laboratory

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                                  ABSTRACT

     In the early 1970s certain filters from the CHESS network were collected
and sent to the Human Studies Laboratory Bioenvironmental Laboratory Branch
(BELB) for sulfate and nitrate analyses.  These analyses were interrupted on
October 1, 1972 and subsequently continued under contract signed March 1973
with Rickman, Edgerley, Tomlinson, and Associates (RETA).  Many of the filters
were not analyzed until RETA became fully operational in May 1973, whereupon
their measurements began to be inexplicably and consistently low.

     The disparity between HSL results and RETA's findings engendered an
investigation involving reanalyses to verify the apparent disparity, and then
to determine a statistical adjustment factor to correct for anomalies.  In
November 1974 Rockwell International undertook the reanalyses of these CHESS
filters.

     In Rockwell's reanalyses, the difference in RETA's sulfate data showed
a mean ratio of 51%, but the.results on nitrates were inconclusive.  The
effects of time and handling were not conclusively determined, altlrotit)ti"tfef't -
was an indication that nitrates decompose with timelaps-e more significantly
than sulfates.  Based on the results in this report^ it was recommended that
CHESS measurements for sulfates be increased by 51% for all sites for -the
entire period RETA performed these analyses.
                                      IV

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                         CONTENTS



                                                        Page





Foreword	       i i i



Abstract	        iv



Figures	        vi



Tables   	       vii



    1.  Introduction	  .  .  .         1



    2.  Other Studies Related to the Problem  ...         3



    3.  Rockwell's Reanalysis of CHESS Filters  .  .         4



    4.  Conclusions    	         8



    5.  Appendix       	        27

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                                 FIGURES
Number                                                            Page

 1.   November 1974 - Rockwell  Reanalyzed Latter 1973 Filters
     for S04	   24

 2.   November 1974 - Rockwell  Reanalyzed Nine Bad Months
     for S04	   25

 3.   November 1974 - Rockwell  Reanalyzed Early 1974 Filters
     for SO4	   26

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                                   TABLES
Number                                                              Page
  1.   Ratio of Sulfate Quarterly Arithmetic Mean to 1973
       Quarterly Arithmetic Mean — First and Second Quarters	    9
  2.   Ratio of Quarterly Arithmetic Mean to 1973 Quarterly
       Arithmetic Mean -- Third and Fourth Quarters	   11
  3.   Ratio of Nitrate Quarterly Arithmetic Mean to 1973
       Quarterly Arithmetic Mean -- First and Second Quarters	   13
  4.   Ratio of Nitrate Quarterly Arithmetic Mean to 1973
       Arithmetic Mean -- Third and Fourth Quarters	   15
  5.   Analysis of Variance for Rockwell's Reanalysis	   17
  6.   November 1974 - Rockwell Reanalyzed 200 RETA Filters	   18
  7.   November 1974 - Rockwell Reanalyzed "Glassine" Filters	   19
  8.   November 1974 - Rockwell Reanalyzed HSL's Filters	   20
  9.   November 1974 - Rockwell Reanalyzed Nine Bad Months	   21
 10.   November 1974 - Rockwell Reanalyzed Latter 1973 Filters	   22
 11.   November 1974 - Rockwell Reanalyzed Early 1974 Filters	   23
A-l.   April 1973 - RETA Reanalyzed HSL's September 1972 Filters..   32
A-2.   June 1974 - RETA Reanalyzed RETA's October 1972 filters	   33
A-3.   June 1974 - RETA Reanalyzed HSL's September 1972 Filters...   34
A-4.   April-May 1974 - Laboratory Comparison	   35
A-5.   June 1974 - Laboratory Comparison	   36
A-6.   July 1974 - Lab Comparison for Side-by-Side CHESS Sites	   37
A-7.   May 1973 - Quality Control Spiked Solutions for Sulfates
       Mean Response and 95% Confidence Interval per
       Laboratory per Level	   38
A-8.   December 1973 - RETA Analysis of Spiked Solutions	   39
A-9.   NYCDAR-CHES5 N03 Discrepancy Study - RETA and QAEML
       Analysis for N03 in Solutions	   40
A-10.  July 1974 - Analysis of Unexposed Spiked Filters Mean
       Responses and 95% Confidence Intervals at Each Level	   41
                                     VI 1

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                                SECTION 1



                              INTRODUCTION





     The sulfate and nitrate fractions of  total  suspended participate Community



Health Environmental Surveilance Systems (CHESS) data showed a dramatic and



sustained decrease beginning in September  and October of 1972.  A review of



the data in Tables 1 through 4 indicates that the sudden decrease was not an



isolated incident, but that a peculiarity  existed across CHESS sites and the



drop could not be attributed solely to seasonal  variation.



     Tables 1  and 2 show the sulfate ratios of the quarterly arithmetic means



to the respective 1973 quarterly arithmetic means by site.   The sulfate ratios



for the first three quarters are generally similar through  1972, but drop in



1973.   However, the fourth quarter ratios  show the decrease dn 1972, and it



is sustained in 1973.



     The nitrate ratios displayed in Tables 3 and 4 show similar decreases,



although they also show a difference between 1970 and 1971  that has  never



been explained.



     It is unlikely that this across-the-board decrease could have been



caused by a decrease in actual pollutant levels.  An investigation by



Environmental  Monitoring and Support Laboratory  (EMSL)  could uncover no



significant Federal or State sulfur regulations  that were implemented for



the first time during  the period in question.



     The most obvious  source of error was  a change in the laboratories



responsible for the sulfate and nitrate analyses.  On October 1, 1972 the

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Bioenvironmental Laboratory Branch (BELB) of the Human Studies Laboratory
(HSL), now Health Effects Research Laboratory (HERL), ceased analysis of
sulfates and nitrates, and exposed filters received after that date were
stored for future analysis.  A contract was signed in March 1973, turning
over the sulfate and nitrate analyses to Ryckman, Edgerley, Tomlinson, and
Associates (RETA).  The same analytical methods used by HSL, BELB, were
also used by RETA.  RETA was not fully operational until  May 1973 and had
the difficult responsibility of overcoming the backlog of filters — which
were not stored and shipped under the most desirable conditions.   Therefore,
many of the filters were not actually analyzed until May and June of 1973.
     The effects of this excessive handling and delays in analyzing the
filters cannot be determined.  However, it was felt that the decrease in
pollutant levels was so large, and was sustained for so long, that the
problem entailed more than excessive handling and delays in analyzing the
filters.  Therefore, the purpose of this report is to show whether or not
RETA's laboratory procedures produced erroneous results, and if so, how the
existing data base can be adjusted to account for the errors.
     Quality control efforts were minimal during the period in which RETA
was performing the analysis.  However, our investigation did turn up several
sets of data which were related to the problem.
     The Human Studies Laboratory conducted an experiment in November 1974
in which Rockwell International (the current contracted laboratory) reanalyzed
some 219 filters which had been analyzed initially by RETA and HSL.  This
experiment provides the most direct approach to the problem, and our con-
clusions and recommendations are based primarily on it.

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                                SECTION 2



                  OTHER STUDIES RELATED TO THE PROBLEM





     Scattered attempts were made by various groups to check the quality of



RETA's output during the period in question.  However, a unified approach



to the problem was sorely lacking.



     In these experiments (see Appendix), the problem was approached in four



ways:  1) a second laboratory "reanalyzed" exposed filters which had been



analyzed some time earlier, 2) two laboratories analyzed the "same" exposed



filters simultaneously, 3) one or more laboratories analyzed the "same"



solutions of known concentrations, and 4) two laboratories analyzed the



"same" spiked filters of known concentrations.



     RETA showed good reproducibility of HSL analyses in April  1973, just



before RETA became operational.   However, in June 1974, RETA's  reanalysis



of filters was different from earlier analyses by both RETA and HSL.



     When RETA and QAEML analyzed the "same" filters simultaneously in



April through June 1974, RETA's measurements were significantly lower.



     In July 1974, RETA consistently understated concentrations of spiked



filters.

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                                SECTION 3
                 ROCKWELL'S REANALYSIS OF CHESS FILTERS

GENERAL PROCEDURES
     In November 1974, 219 filters from the CHESS network were retrieved,
and new strips were cut from them and shipped to Rockwell  for reanalysis
for sulfates and nitrates.  The original  design called for one filter per
month per 12 stations from July 1972 through June 1974, but almost one-
third of the filters could not be reanalyzed, either because they were
in poor condition or they could not be located.
     Twenty-two of these filters had been initially analyzed by HSL and the
other 197 by RETA.  They were selected at random from high-exposure and low-
exposure sites in Charlotte, Birmingham,  Chattanooga, New York, Utah, and
California.
     In addition to these 219 filters, 62 other filters were sent to
Rockwell for reanalysis.  These filters were originally analyzed by RETA,
then set aside for quality control purposes in June 1973 and never
utilized.  Since these filters were stored in glassine envelopes, it
was felt that they were better preserved than the others.
Statistical Analysis
     An analysis of variance was performed on the 219 filter results to test
for possible effects of sites, days between exposure and reanalysis, and the
laboratory which did the first analysis.   The first concentration was
considered one of the independent variables and the second concentration
was analyzed as the dependent variable.

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     The concentrations, unless otherwise stated, are in micrograms
per cubic meter (yg/m3).
     The results in Table 5 show no effects of time or sites, but show
strong influences from the first concentration and from the laboratory
which did the first analysis.
     To make a valid comparison between the laboratories we must have them
both operating on the same experimental material.  Thus, we must make three
assumptions:
     •  First, since a second strip was cut from the filter for the reanalysis,
we must assume the pollutant concentration is uniform across the filter.
However, we are not aware of any documentation on this point.
     •  Second, we assume no change in pollutant amount between analyses  due
to the handling of the filters.
     •  Third, the natural pollutant decomposition over time was assumed  to
be negligible.  It was generally felt that this is a valid assumption for
sulfates, but some scientists feel  that nitrates decompose by a significant
amount.
     Subject to the above three assumptions, the data set can be thought  of
as n pairs of realizations of the log-normally distributed random variables,
x and y.  Since the filters were pulled from a population at random, we can
assume that the random variables X  = In x and Y = In y have a bivariate
normal distribution with means y2. ancj y2  variances a2 and a2 and correlation
                                x      y             x      y
coefficent p.
     Then the random variable Z = X - Y is normally distributed with mean
yz = yx " yy and variance °z = CTx + °y " 2pCTxay'  The fact tnat exP(z) =  X/Y
enables us to make inferences about the ratio of the random variables x and y.
     It was felt that gross violations of the first two assumptions would be

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manifest as outliers.  Therefore, the criterion for labeling an observation
as an outlier and excluding it from the analysis was based on the ratio.
     If we represent the sample arithmetic mean by I and the sample variance
by S2, we know that the statistic t=(Z"-yJ/(S//rvT) is distributed as  Student's
t with n-1 degrees of freedom.  Then t is used to test the hypothesis  that
y =0, or equivalently that x=y.  Confidence intervals are constructed  for
y , which is the geometric mean of the ratio x/y.
     The computer printouts show the descriptive statistics for x and  y (the
numerator in the ratio is listed first, then the denominator in the second
column) along with the value of t and the 95% confidence interval  for  y .
The value of t is significant at the 0.05 level if and only if the confidence
interval includes one.
     Table 6 shows the results of Rockwell's reanalysis of the 197 filters
originally analyzed by RETA.  RETA is 43-60% low on sulfates, with a mean
ratio of 51%, but there is no significant difference on nitrates.
     The data from the 62 filters which were stored in glassine envelopes
are analyzed in Table 7.  RETA comes up 22-35% low on sulfates, but 31-55%
high on nitrates.
     The 22 filters which were first analyzed by HSL are analyzed in Table 8.
There is no significant difference on sulfates, but HSL is 18-66% high on
nitrates.
     The filters initially analyzed by RETA were divided into three groups
to see if this breakdown would show an effect that the analysis of variance
did not show.  The first group, filters exposed between September 1972, and
June 1973, were the backlogged filters which were more physically abused.
The second group, filters exposed between July 1973, and December 1973, were

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analyzed on a more timely basis.   The other group of filters exposed in 1974
were analyzed on RETA's regular schedule -- within three weeks of exposure.
     A comparison of the results  in Tables 9-11  with Table 6 shows no group
effect.  The sulfate intervals are 36-60%, 32-70%, and 48-72% respectively,
all of which contain 51%.  None of the three groups show a significant
difference for nitrates.
     The ratio of Rockwell  to RETA is plotted against the RETA measurement
for each time group in Figures 1-3.  The plots indicate that the ratio does
not depend on pollutant level.

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                                SECTION 4



                               CONCLUSIONS





     We recommend that sulfates be increased by 51% for all  CHESS sites



for the entire time period RETA performed the analyses.



     We believe there is a decomposition effect with nitrates, as evidenced



by the Tables 7 and 8.  Since we could not detect a difference between RETA



and Rockwell on the 197 filters, we cannot recommend a nitrate adjustment.



However, if decomposition prevented a valid comparison, an independent



study to quantify that effect could enable us to formulate a nitrate adjust-



ment factor.
                                       8

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TABLE 1.  RATIO OF SULFATE QUARTERLY ARITHMETIC MEAN TO
          1973 QUARTERLY ARITHMETIC MEAN - - FIRST
          AND SECOND QUARTERS
Site

0211
0221
0232
0312
0323
0331
0411
0421
0431
0511
0521
0531
0541
0621
0622
0631
0632
0633
0634
0635
0641
0642
1st Quarter
70 71
2.36 1.62
1.61 1.24
2.74 1.95
1.33
2.26
1.78 1.50
2.54
2.25
2.03
0.32
0.62
0.61
0.80
1.19
1.43
1.53
1.50
1.55
1.11
1.74
1.27
1.29
72
1.76
1.34
2.10
1.80
2.89
1.86
2.80
2.31
1.92
1.16
0.87
0.70
0.84
1.60
2.10
1.85
1.56
2.14
1.48
1.98
1.54
1.88
73
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00-
1.00
1.00
1.00
1.00
1.00
1.00
1.00
2nd Quarter
70 71
1.90 1.51
1.83 1.58
2.09 1.54
1.63
1.31
2.27 1.75
1.10
1.26
1.38
1.57
1.79
l.BtJ
1.51
1.40
1.38
0.81
1.61
1.41
1.37
1.43
1.32
1.28
72
1.41
1.41
1.65
1.89
1 .33
1.67
1.51
1.41
1.49
2.23
2.54
1.69
•1.49
1.56
1.47
0.89
1.51
1.47
1.48
1.35
1.34
1.50
73
1.00
1.00
1 .00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1 .00
1.00
1.00
1 .00
1.00
1.00
1.00
1.00
                                                     (continued)

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TABLE 1  (continued)
Site
          70
1st Quarter
 71      72
 73
70
  2nd Quarter
71       72
73
0711
0721
0722
0732
        2.27    1.00
        1.82    1.00
        1.79    1.00
        1.90    1.00
                     0.87     1.72     1.00
                     0.76     1.58     1.00
                     0.72     1.48     1.00
                             1.71     1.00
0811
0821
0822
0831
0832
0841
0842
        3.97
        5.61
        5.80
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.79
1.15
1.18
1.26
1.17
1.23
1.23
1.00
1.00
1 .00
1.00
1.00
1.00
1.00
                                      10

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Site
        TABLE 2.  RATIO OF SULFATE QUARTERLY ARITHMETIC MEAN TO
                  1973 QUARTERLY ARITHMETIC MEAN - - THIRD AND
                  FOURTH QUARTERS
3rd Quarter
4th Quarter

0211
0221
0232
0312
0322
0331
0411
0421
0431
0511
0521
053T
0541
0621
0622
0631
0632
0633
0634
0635
0641
0642
70
1.16
1.09
1.47


1.52







1.41
1.59
1.45
1.52
1.64
1.69
1.45
1.52
1.23
71
0.95
1.03
1.22
1.41
1.16
1.30
1.28
1.23
1.28
1.52
1.43
1.35
1.10
1.10
1.21
1.19
1.29
1.43
1.27
1.17
1.10
1.00
72
1.14
1.09
1.24
1.61
1.45
1.40
1.35
1.16
1.18
1.12
1.37
1.18
. 1.01
1.35
1.43
1.39
1.26
1.80
1.64
1.35
1.47
1.30
73
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
70
1.82
1.49
1.96
1.64
1.79
2.22
3.13
2.27
2.33




1.67
1,67
1.72
1.47
1.89
1.75
1.92
1.82
1.75
71
1.98
1.90
2.08
1.57
1.63
2.07
2.91
2.11
2.44
3.45
2.86
2.44
1.49
1.73
1.60
1.60
1.53
1.91
1.82
1.92
1.89
1.75
72
1.20
0.67
1.06
1.05
1.14
1.44
0.94
0.86
1.00
1.72
1.71
1.68
1.07
1.15
0.97
1.21
1.01
1.23
1.39
1.15
1.13
1.18
73
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
                                                              (continued)
                                      11

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TABLE 2 (continued)
Site


0711*
0721*
0722*
0732*

0811
0821
0822
0831
0832
0841
0842
       3rd Quarter
         4th Quarter
70
71
1.18
1.08
1.11








72
1.00
1.00
1.00
1.00
0.84
0.79
0.82
0.75
0.81
0.85
0.77
73




1.00
1.00
1.00
1.00
1.00
1.00
1.00
70
 71
2.56
2.50
2.04
 72
1.00
1.00
1.00
1.00

0.72
0.73
0.63
0.57
0.57
0.55
0.71
73
                                                           1.00
                                                           1.00
                                                           1.00
                                                           1.00
                                                           1.00
                                                           1.00
                                                           1 .00
  NEW JERSEY DENOMINATORS ARE 1972  QUARTERLY  MEANS
                                     12

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TABLE 3.   RATIO OF NITRATE QUARTERLY ARITHMETIC MEAN
          TO 1973 QUARTERLY ARITHMETIC MEAN - - FIRST
          AND SECOND QUARTERS
Site

0211
0221
0232
0312
0323
0331
0411
0421
0431
0511
0521
0531
0541
0621
0622
0631
0632
0633
0634
0635
0641
0642
1st
70 71
1.50 1.00
1.00 0.69
2.00 1.22
1.23
1 .36
1.56 1.22
1.18
1.21
1.00
0.50
0.71
0.80
1.21
2.40
1.62
19.75
3.60
6.12
5.50
2.40
3.14
1.60
Quarter
72
2.17
1.23
2.00
1.30
1.29
1.28
2.36
2.86
1.95
1.00
1.58
2.40
4.86
3.00
2.46
11.00
3.40
5.62
5.67
2.70
2.71
1.90

73
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1 ;--00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
2nd
70 71
1.50 3.00
1 . 50 3.17
1.57 3.00
2.89
2.21
1.64 2.50
1.25
1.86
2.33
3.20
3.14
2.29
3.00
5.14
4.57
3.83
5.33
7.00
7.14
6.00
4.00
3.43
Quarter
72
1.50
1.67
1.57
1 .56
1.21
1.43
1.75
2.14
1.83
2.80
2.14
1.57
2.00
2.14
1.86
1.38
2.78
3.13
3.29
3.00
1 .57
1.71

73
1.00
1.00
1 .00
1.00
1.00
1.00
1 .00
1.00
1.00
1 .00
1.00
~1 .00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1 .00
1.00
1.00
                                                   (continued)
                          13

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 TABLE 3 (continued)
 Site
           70
1st Quarter
 71       72
 0711
 0721
 0722
 0732

 0811
 0821
 0822
 0831
 0832
 0841
0842
       4.36
       3.89
       7.79
                                   73
        2.23     1.00
        1.94     1.00
        2.00     1.00
        2.00     1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
                        2nd  Quarter
               70       71       72       73

                     9.00    3.00    1.00
                     5.63    2.63    1.00
                     3.20    1.50    1.00
                             2.25    1.00
2.17
1.41
2.08
1.95
1.71
3.27
2.60
1.00
1.00
1.00
1.00
1.00
1.00
1.00
                                    14

-------
Site
          TABLE 4.  RATIO OF NITRATE QUARTERLY ARITHMETIC MEAN
                    TO 1973 QUARTERLY ARITHMETIC MEAN -- THIRD
                    AND FOURTH QUARTERS
3rd Quarter
4th Quarter

0211
0221
0232
0312
032?
0331
0411
0421
0431
0511
0521
0531
0541
0621
0622
0631
0632
0633
0634
0635
0641
0642
70
1.00
2.50
2.00

1.45
1.49


1.00




3.57
2.63
4.00
2.78
2.38
5.56
2.00
1.49
1.00
71
4.50
8.50
9.50
3.85
2.23
2.07
3.45
4.55
4.00
3.23
3.23
2.33
3.45
4.96
7.89
6.08
6.94
5.76
18.67
7.26
4.73
4.00
72
2.00
2.00
2.50
2.23
1.57
1.24
1.48
1.88
2.00
1.61
1.32
1.33
1.83
2.00
2.32
7.40
3.97
3.57
9.60
3.76
1.49
1.50
73
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
70
0.71
0.70
0.80
0.85
0.67
0.65
1.27
1.00
0.94
3.70
1.67
1.16
1.16
1.89
2.22
4.00
1.69
2.33
3.85
2.27
1.41
1.56
71
2.86
2.50
2.80
2.08
1.67
1.65
2.80
2.89
3.01
2.81
3.00
3.57
2.57
3.87
4.67
3.76
3.54
4.42
9.39
3.20
2.32
2.67
72
0.86
0.80
0.80
1.00
0.80
1.00
0.81
0.61
0.59
1.00
1.17
0.83
0.50
1.09
1.00
1.48
1.00
0.77
0.85
0.68
0.66
0.67
73
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
1.00
OD
1.00
1,00
1 .00
1.00
1.00
1.00
1.00
1.00
1.00
                                                              (continued)
                                     15

-------
TABLE 4 (continued)
Site
0711*
0721*
0722*
0732*

0811
0821
0822
0831
0832
0841
0842
3rd Quarter
4th Quarter
          70
71
2.08
3.45
2.72








72
1.00
1.00
1.00
1.00
2.70
1.85
3.85
3.13
2.56
3.23
3.23
73




1.00
1.00
1.00
1.00
1.00
1.00
1.00
                                 70
 71
5.00
5.26
4.17
3.03
 72
1.00
1.00
1.00
1.00

1.03
0.91
0.67
0.42
0.85
0.81
0.62
73
                                                       1.00
                                                       1.00
                                                       1.00
                                                       1.00
                                                       1.00
                                                       1.00
                                                       1.00
 "NEW JERSEY DENOMINATORS ARE 1972 QUARTERLY  MEANS
                                      16

-------
        TABLE 5.  ANALYSIS OF VARIANCE FOR ROCKWELL'S REANALYSIS
              Factor
Initial Concentration
Days Between Exposure and Reanalysis
Sites
Laboratories
              Factor
Initial Concentration
Days Between Exposure and Reanalysis
Sites
Laboratories
Sulfates
  d.f.
   1
   1
   1
   1

Nitrates
  d.f.
   1
   1
   1
   1
Partial S.S,
  26280.2
     83.3
    124.0
    401.4
Partial  S.S
    868.9
     11.6
      5.8
     33.2
F value     p
644.85   0.000
  2.04   0.154
  3.04   0.083
  9.85   0.002
F value     p
248.40   0.000
  3.32   0.070
  1.66   0.199
  9.49   0.002
                                      17

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                                APPENDIX

EXPERIMENTS INVOLVING THE REANALYSIS OF EXPOSED FILTERS
     The same rationale that was used in the Statistical Analysis of the
Rockwell experiment in the text is used here.
1.A.  (Table A-l) In April 1973, several weeks before RETA was fully
operational, 10 filters from the CHESS network which had been analyzed
by HSL in September 1972 were flown to St. Louis to have RETA reanalyze
them for sulfates.
     The data are in milligrams per filter, so the values would have to be
approximately halved to convert to micrograms per cubic meter.  Table A-ll
contains conversion factors for the different units used in these studies.
     The analysis shows a laboratory difference, but it is only 3-15%.  In
the absence of any standards to go by, this was, and still is- considered
good agreement.
1.B.  (Tables A-2 and A-3) In June 1974, RETA was asked to reanalyze 30
filters exposed in the CHESS network in September and October 1972.
Eighteen of the filters were initially analyzed by RETA, and the remaining
12 were analyzed first by HSL.
     Table A-2 shows the results for the 18 filters first analyzed by RETA.
The 1974 analyses were 1-15% higher than 1972 for sulfates, but were 13-32%
higher than 1972 for nitrates.
     Table A-3 compares RETA 1974 vs. HSL 1972.  RETA's sulfate measurements
were 35~108% lower than HSL's.   The RETA nitrate values were also well below
HSL's, but the correlation between nitrate values was a low 0.478.
                                     27

-------
EXPERIMENTS COMPARING LABORATORIES ANALYZING THE SAME FILTERS SIMULTANEOUSLY
     In the experiments, two strips were cut from the filter and one given
to each laboratory for analysis.   Thus, we need to make the assumption of
uniformity of pollutant concentration across the filter.  However, the other
two assumptions are not necessary, as there is no timelag between analyses.
Statistical Analysis
     The same approach was used on these data sets that was used on the
experiments involving reanalysis  of exposed filters.
2.A.  (Table A-4) In April and May 1974, 13 filters were given to RETA and
QAEML for a laboratory comparison for both sulfates and nitrates.
     The measurements showed high correlations, but RETA was 23-41% low on
sulfates and 26-46% low on nitrates.
2.B.  (Table A-5) In June 1974, another laboratory comparison involving
RETA and QAEML was performed using 16 filters.  Only  nitrates were analyzed,
as this was part of the New York City DAR-CHESS "N03 Discrepancy Study.
     The data are in rr.icrograms per filter*"strip, so  the values-would have
to be divided by approximately 200 to convert to micrograms per cubic meter.
     RETA was 19-30% low on these nitrate measurements.
2.C.  (Table A-6) In July 1974, two CHESS hi-vol instruments were located
in Garden Grove, California, for 21 days and in Thousand Oaks, Calfornia,
for two days.  The filters from one instrument were analyzed by RETA and the
other by Rockwell.
     These data necessitate the further assumption that the pollutant
concentration is uniform across the CHESS sites.  The Garden Grove
instruments were located one mile apart.
                                     28

-------
      There was  no  significant  difference  between  the  RETA  and  Rockwell measure-
 ments of  sulfates.   RETA  was low on nitrates,  but  the  correlation coefficient
 on  nitrates was a  very  low 0.247.
 EXPERIMENTS COMPARING LABORATORIES ANALYZING SPIKED SOLUTIONS
      Spiked solutions containing known (unknown to the laboratory) pollutant
 concentrations were given to each laboratory for analysis.   Several levels
 of concentration were used.
     The only assumption needed is that the solutions are homogeneous.  If
 the solution was separated into bottles,  aliquots, or otherwise broken down
 into smaller containers, it needs to be assumed that the concentration would
 remain the same throughout.
     All the data are in micrograms per milliliter, so the  values would have
to be divided by approximately 3.4 to canvert to micrograms per cubic meter.
Statistical Analysis
     We assumed that all solutions were identical  except for pollutant content,
and that level  was  known without error.  The mean respefise  of each .laboratory
at each level  was tabulated,  and a 95% confidence interval  for that if?.ean-was
calculated when possible.   If the laboratory was functioning correctly, we
would expect the confidence interval  to include the known level of input.
3.A.  (Table A-7)  In May 1973,  RETA and OAEML were each given five sulfate
solutions at each of three levels to check RETA's quality.   Both laboratories
exhibited errors in measurement, but due  to ignorance concerning the method
 itself, no alarm was sounded.
 3.B.  (Table A-8) In December 1973, RETA analyzed 16 solutions at two
 pollutant levels for sulfates and nitrates.  Two solutions  at each level
were analyzed on both the morning and afternoon of each of  four days.
                                     29

-------
     An analysis of variance was performed to test for possible time of day
and data effects.  Neither was significant for sulfates, but both were
significant at the 0.05 level for nitrates.  The ANOVA table appears with
RETA's estimates of the levels in Table A-8.
     RETA's accuracy is poor, but these are very low levels, especially
for nitrates.
3.C.  (Table A-9) In June 1974, as part of the New York City DAR-CHESS N03
Discrepancy Study,  RETA and QAEML analyzed solutions at six levels  of N03.
QAEML provided one measurement at each level,  while RETA analyzed three
solutions at each level.
     Confidence intervals were not calculated, as RETA's values contained
almost no variability.   Although RETA appears  to obtain lower measurements
at higher concentrations, we did not evaluate  these differences because of
the small  sample size and lack of knowledge concerning interlaboratory
variablity.
EXPERIMENT INVOLVING ANftfcYSM-"8F SPIKED FILTERS
     In July 1974,  Rockwell  and RETA analyzed  five filter strips of known
concentration at each of five levels for sulfates and at each of four levels
for nitrates.
     It has to be assumed that the pollutant concentration was distributed
uniformly across the filters.
     The data are in milligrams per filter, so the numbers would have to be
approximately halved to convert to micrograms  per cubic meter.
Statistical Analysis
     Mean responses and confidence intervals for the mean responses were
tabulated as in Section 3 above.
                                      30

-------
     Table A-10 contains the data showing that RETA is consistently low on



both sulfates and nitrates.   Rockwell  is also low at some levels,  but not to



the same extent as RETA.  A knowledge of interlaboratory variability would



enable further inferences to be made from this data set.



CONVERSION FACTORS FOR TABLES



Assuming:  Time = 1440 minutes, Flow = 50 cubic feet per minute



Micrograms per Cubic Meter = 2.95 x 10"1 Micrograms per Milliliter



                           = 5.89 x 10"3 Micrograms per Strip



                           = 4.91 x lO"4 Micrograms per Filter
                                      31

-------
TABLE A-l.  APRIL 1973 - RETA REANALYZED HSL'S SEPTEMBER 1972 FILTERS


                               Sulfates

     Geometric Mean Ratio                            0.906

     95% Confidence Interval
     for Geometric Mean Ratio                    (0.846, 0.970)

     Correlation Coefficient of Logs                 0.9818

     Number of Observations                             10

                                               HSL           RETA

     Arithmetic Mean                          33.680        36.360

     Geometric Mean                           31.424        34.676

     Maximum                                  58.200        57.600

     Minimum                                  20.000        23.400

     Standard Deviatton                       13.747        12.307

     Geometric Standard Deviation              1.472         1.375
                                      32

-------
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-------
       TABLE A-5.  JUNE 1974 - LABORATORY COMPARISON

                          Nitrates
Geometric Mean Ratio                          1.242
95% Confidence Interval
for Geometric Mean Ratio                  (1.189,  1.297)
Correlation Coefficient of Logs               0.9968
Number of Observations                           15
                                          EMSL         RETA
Arithmetic Mean                         558.800      519.120
Geometric Mean                          479.062      385.780
Maximum                                1762.000     1375.100
Minimum                                  94.000       79.200
Standard Deviation                      114.869       89.003
Geometric Standard Deviation              1.218        1.215
                               36

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-------
   TABLE A-7.   MAY 1973 - QUALITY  CONTROL SPIKED SOLUTIONS FOR SULFATES
               MEAN RESPONSE AND 95% CONFIDENCE  INTERVAL  PER LABORATORY
               PER LEVEL
Concentration Level
      (yg/ml)                RETA                  QAEML            # of Obs.

         0               0.0 --                2.4 (2.1, 2.6)            5

        30              24.8 (20.2,  29.4)      28.5 (27.6, 29.4)          5

        60              47.0 (41.7,  52.3)      61.1 (52.1, 70.1)          5
                                      38

-------
rABLE A-8.   DECEMBER  1973  -  RETA  ANALYSIS  OF  SPIKED  SOLUTIONS


Factor S.S.
Total 15977.9
Day 101.3
Level 15487.9
Time 26.2
Error 362.3
Level (pg/ml)
10
60


Factor S.S.
Total 34.98
Day 0.16
Level 34.27
Time 0.10
Error 0.44
Level (yg/ml)
1
10
Sul fates
ANOVA Table
d.f. M.S.
31
3 33.7
1 15487.9
1 26.2
26 13.9
Mean Responses
8,47 (7.41, 9.53)
52.47 (49.62, 55.32)
Nitrates
ANOVA Table
d.f. M.S.
31
3 0.05
1 34.27
1 0.10
26 0.01
Mean Responses
0.195 (0.178, 0.212)
2.265 (2.151, 2.379)


F P

2.42 0.087
1111.34 0.000
1.88 0.178

# of Obs.
16
16


F " P

3.23 0.037
2012.44 0.000
5.94 0.020

# of Obs.
16
16
                                39

-------
      TABLE A-9.   NYCDAR-CHESS  N03  DISCREPANCY  STUDY
                  RETA AND  QAEML  ANALYSIS  FOR N03  IN  SOLUTIONS
Concentration Level                                 RETA
      (yg/ml)                QAEML           (average  of  three)

         4                    3.75                  4.20

         6                    5.90                  5.90

         9                    9.00                  8.50

        11                   11.00                 10.60

        14                   14.10                 13.47

        16                   16.10                 14.20
                                 40

-------
        TABLE A-10.   JULY 1974 - ANALYSIS OF UNEXPOSED SPIKED  FILTERS
                     MEAN RESPONSES AND 95% CONFIDENCE INTERVALS  AT
                     EACH LEVEL
                                Sulfates

Concentration Level
      (yg/ml)               RETA                   Rockwell          #  of  Obs,

        3.00           1.84  (0.51,  3.17)       2.88  (2.55,  3.21)         5

       11.26           9.24  (8.08,  10.40)     11.16  (10.53,  11.79)       5

       15.18          12.64  (10.98,  14.30)    15.26  (13.71,  16.81)       5

       27.76          22.16  (21.24,  23.08)    25.78  (25.35,  26.21)       5

       36.00          24.90  (22.34,  27.46)    34.00  (32.96,  35.04)       5


                                Nitrates

        3.05           2.40  (2.15,  2.65)       2.64  (2.53,  2.75)         5

        6.04           4.80  (3.99,  5.61)       5.52  (5.38,  5.66)         5

        9.01           7.95  (7.09,  8.81)       8.88  (8.74,  9.02)         5

       12.00           8.94  (7.59,  10.29)     10.96  (10.82,  11.10)       5
                                      41

-------
                                  TECHNICAL REPORT DATA
                           (Please read Instructions on the reverse before completing)
1. REPORT NO.
  EPA-600/1-77-004
                             2.
                                                          3. RECIPIENT'S ACCESSI Of* NO.
4. TITLE AND SUBTITLE

  AN ASSESSMENT OF THE CHESS SULFATE AND NITRATE  DATA
  during  the  period RETA performed the chemical analysis
             5 REPORT DATE
               January 1977
             6. PERFORMING ORGANIZATION CODE
7. AUTHOR(S)

  Leo T. Heiderscheit and Marvin B. Hertz
                                                          8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
 Health Effects  Research Laboratory
 U.S. Environmental  Protection Agency
 Research  Triangle  Park, N.C. 27711
                                                          10. PROGRAM ELEMENT NO.
                1EA615
             11. CONTRACT/GRANT NO.
12. SPONSORING AGENCY NAME AND ADDRESS
 Health Effects  Research Laboratory
 Office of  Research and Development
 U.S. Environmental Protection Agency
 Research Triangle Park, N.C. 27711
             13. TYPE OF REPORT AND PERIOD COVERED
               In-house	
             14. SPONSORING AGENCY CODE

               EPA-ORD
15. SUPPLEMENTARY NOTES
16. ABSTRACT
       In  the  early 1970s certain filters from  the CHESS network were collected  and
 sent  to  the  Human Studies Laboratory  (HSL)  Bioenvironmental Laboratory  Branch  (BELB)
 for sulfate  and nitrate analyses,  These  analyses were interrupted on October  1,
 1972  and subsequently continued under contract signed March 1973 with Rickman,
 Edgerley,  Tomlinson, and Associates  (RETA).   Many of the filters were not  analyzed
 until  RETA became fully operational  in May  1973, whereupon their measurements  began
 to be  inexplicably and consistently  low.    The disparity between HSL results  and
 RETA's findings engendered an investigation involving reanalyses to verify the
 apparent disparity, and then to determine a statistical adjustment factor  to  correct
 for anomalies.   In November 1974 Rockwell International undertook the reanalyses  of
 these  CHESS  filters.

       In  Rockwell's reanalyses, the difference in RETA's sulfate data showed a  mean
 ratio  of 51%,  but the results on nitrates were inconclusive.  The effects  of  time
 and handling were not conclusively determined, although there was an indication that
 nitrates decompose with timelapse more significantly than sulfates.  Based on  the
 results  of this report, it was recommended  that CHESS measurements for  sulfates be
 increased by 51% for all sites for the entire period RETA performed these  analyses.
17.
                               KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
b.lDENTIFIERS/OPEN ENDED TERMS  C. COSATI Field/Group
  sulfates
  inorganic nitrates
  chemical  analysis
  CHESS
07 B
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