nl States
          Environmental Protection
          Agency
Toxic Substances
Washington DC 20460
EPA-560/13-80-006
February, 1980
          Toxic Substances
&EPA    Sampling and Analysis of Selected
          Toxic Substances
          Task 2:  Analysis for Semivolatile
                    Brominated  Organics in
                    Fish and Turtles

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                                                    EPA-560/13-80-006
             SAMPLING AND ANALYSIS OF SELECTED TOXIC SUBSTANCES
 TASK 2:  ANALYSIS FOR SEMIVOLATILE BROMINATED ORGANICS IN FISH AND TURTLES
                                     by

M. D. Erickson, K. B. Tomer, J. T. Bursey, M.  A.  Moseley and E.  D.  Pellizzari
                         Research Triangle Institute
                            Post Office Box 12194
                Research Triangle Park, North Carolina  27709
                           Contract No.  68-01-5020
                                   Task 2
                               Project Officer

                             Vincent J. DeCarlo
                               Thomas E. Kopp
                  Office of Pesticides and Toxic Substances
                    U. S. Environmental Protection Agency
                          Washington, D. C.  20460
                  OFFICE OF PESTICIDES AND TOXIC SUBSTANCES
                    U. S. ENVIRONMENTAL PROTECTION AGENCY
                          WASHINGTON, D. C.  20460

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                                   DISCLAIMER

     This report has been reviewed by the Office of Pesticides and Toxic
Substances, U. S. Environmental Protection Agency, and approved for pub-
lication.  Mention of trade names or commercial products does not constitute
endorsement or recommendation for use.
                                        11

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                                    ABSTRACT

     Fish and turtle (5 from Arkansas and 3 from Louisiana) caught downstream
of the brominated organic chemical industry near El Dorado, AR were extracted,
cleaned up, and analyzed by GC/MS for brominated organics using full scan and
single ion monitoring electron impact GC/MS, and negative ion chemical ioniza-
tion GC/MS.  PBBs (C  H.Br, and C  H Br ) were identified in one sample and
several other brominated compounds were tentatively identified in several
samples.  Due to the high levels of interferences and very low levels of the
compounds of interest,  further identifications were impossible.   The compounds
were not quantitated, but levels appear to be much less than 1 ppm.
                                     ill

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IV

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                                    CONTENTS

Abstract	iii
Figures 	    v
Tables	   vi
List of Abbreviations	vii
Acknowledgements	viii
     1.  Summary and Conclusions	    1
     2.  Introduction 	    2
     3.  Results	    3
References	   18
Appendices
     A.  Sample location map and field data sheets from Arkansas
         sampling	   19
     B.  Sample location map and field data sheets from Louisiana
         sampling	   36
     C.  Analytical protocol:  Sampling and analysis of extractable
         halogenated organics in tissue 	   47

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                                     FIGURES
Number                                                                Page
  1       Full scan GC/EIMS spectrum of AR2E021 illustrating very
          high background	8
  2       Single ion plots from  SIM GC/EIMS analysis of AR2E021. ...  9
  3       Single ion plots from  GC/NICIMS analysis of AR2E021	14
  4       Single ion plots from  GC/NICIMS analysis of LA01	15
  5       Single ion plots from  GC/NICIMS analysis of LA03	16
                                         vi

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                                    TABLES
Number                                                               Page
 1       Summary of samples received from Arkansas and Louisiana. . .  4
 2       Summary of organic sample extraction and cleanup 	  5
 3       SIM mass spectrometry conditions for selected brominated
         compounds	12
 4       Raw data from SIM GC/EIMS analysis of AR2E021	13
 5       Brominated compounds found in fish and turtle samples from
         Arkansas and Louisiana 	 17
Al       Recovery of extractable halogenated hydrocarbons from human
         tissue extracts	49
A2       Estimated limits of detection for extractable halogenated
         organics analysis	55
A3       RMRs for PCBs and pesticides of interest to this program . . 56
A4       RMR factors for standard PCB solutions, selected ion
         monitoring mode	57
A5       Semi-volatile halogenated hydrocarbons in methanol spiking
         solution	59
                                      vii

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                              LIST OF ABBREVIATIONS

GC/EIMS        gas chromatography/electron impact mass spectrometry/computer
GC/ECD         gas chromatography with electron capture detection
GC/MS          gas chromatography/mass spectrometry/computer
GC/NICIMS      gas chromatography/negative ion chemical ionization mass
               spectrometry/computer
m/z            mass to  charge ratio
SIM            Selected  ion monitoring
                                     viii

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                                ACKNOWLEDGEMENTS

     The authors wish to thank Frank Hall and David Parrish, USEPA, Region
VI, Dallas, Texas for arranging the sampling; John Geise of the Arkansas
Department for Pollution Control and Ecology and Lewis Johnson of the Louisiana
Department of Wildlife and Fisheries for conducting the sampling; Barbara
Bickford, Para Gentry, and Steve Burke for assistance with the GC/MS analysis,
and Lynna Oglesby for typing the report.  We also wish to acknowledge the
Project Officers, Drs. Vincent DeCarlo and Thomas Kopp of OPTS, EPA,
Washington, D.C. for their assistance.
                                    ix

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                                    SECTION 1
                             SUMMARY AND CONCLUSIONS

     Hexabromobiphenyl and heptabromobiphenyl were identified in one sample
(AR2 D010).  Decabromobiphenyl ether was tentatively identified in four
samples; decabromobiphenyl was tentatively identified in one sample; and one
sample contained three unidentified brominated compounds.  By comparison to
the response of standards, all brominated compounds were present at much less
than 1 ppm.
     The analysis required the use of both positive ion and negative ion
GC/MS.  Analysis by GC/EIMS alone would have incorrectly identified several
brominated compounds.   Further development of the use of GC/NICIMS will
facilitate better use  of this technique in future analyses of this type.
     The high background of these samples interfered significantly with the
analysis, and forced the use of extra cleanup steps.  Future analysis of this
type should employ better cleanup techniques, possibly gel permeation chromato-
graphy.

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                                    SECTION 2
                                  INTRODUCTION

     Previous studies have shown the presence of brominated organics in the
air, water, soil and other environmental media near the brominated organic
                                                         (1-3)
manufacturing industries near El Dorado and Magnolia, AR.      It is of
interest to determine if these chemicals are concentrating in and possibly
migrating with aquatic organisms.  The objective of this study was to analyze
several fish and turtle samples collected "downstream" from the alleged
sources near El Dorado, AR to see if brominated organics were present.

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                                    SECTION 3
                                     RESULTS

SAMPLE RECEIPT
     On July 13, 1979, five samples were received from Arkansas.  On October 9, 1979
three samples were received from L.R.C. Johnson, Monroe, LA.  The samples
were collected from streams and rivers near brominated chemical manufacturing
plants in the El Dorado, AR area.  The samples consisted of turtles and fish
and were composited by sampling personnel.  The samples were received frozen
in dry ice and were immediately transferred to a freezer awaiting analysis.
The samples received are summarized in Table 1.  Copies of the sample location
map and "Field Data Sheets" are attached in Appendices A and B.
PREPARATION OF SAMPLES FOR ANALYSIS
     The samples were allowed to thaw at room temperature for three hours,
then they were placed in a refrigerator overnight.   Approximately 100 g of
each sample was weighed out for analysis (see Table 2).  Fish samples AR2E021,
AR2E018 and AR2E016 utilized several whole fish.  Sample AR2D010 was a mixture
of turtle organs which were placed in a blender and homogenized.  Approximately
10% of the resulting macerate was used for analysis.  Sample LAOS consisted
of three large gars weighing more than 200 g each.   One fish was homogenized
in a blender and about one half of the macerate analyzed.
     The samples were worked up using the analytical protocol in Appendix C.
Specific details and deviations from the protocol are discussed below.  The
samples were extracted by placing them in a blender with 150 mL of redistilled
hexane.  The samples were broken up into small pieces using a slow blender
setting (mince) for approximately 30 sec.  Then, the mixture was blended at
the highest blender speed (liquefy) for 30 sec.  The macerate was scraped
down the sides of the blender, followed by another 30 sec of the high speed
blending.  The hexane solution was decanted, and the solids were reextracted
with 2 x 100 mL portions of fresh, redistilled hexane using the above extrac-

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                   Table 1.  SUMMARY OF SAMPLES RECEIVED FROM ARKANSAS AND LOUISIANA
Sample Code
AR2D008
AR2D010
Source
Bayou
Bayou
de
de
of
Sample
Loutre
Loutre
Sampling
Date
July
July
12,
11,
1979
1979
Time
0940
0900
Sample
Weight
(lb)
a
a
Description
common snapping turtle
alligator and snapper turtles


and
AR2E016      Cornie Bayou at
             Junction City

AR2E018      Bayou Cornie

AR2E021      Tributary of Cornie
             Bayou
LA01         Bayou de Loutr"

LA02         Bayou de Loutre

LAO3         Corney Lake
                             (1) red ear slider

July 10, 1979  1000   2.1    fish:  bullheads, sunfish and  sucker
July 11, 1979  1100   1.3

July 10, 1979  1400     H



Aug. 10, 1979  0800   2.0

Aug. 10, 1979  1015   2.2

Aug. 10, 1979  1200   2.3
                             fish:  bass, sunfish and crappie

                             fish:  pickerel, sunfish, bluegill,
                             blackspotted top minnows, redfin
                             shiners

                             large mouth bass (3)

                             gar (2)

                             gar (3)
  Not listed on Field Data Sheet

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     Table 2.  SUMMARY OF ORGANIC SAMPLE EXTRACTION AND CLEANUP








Sample Code    Type of Sample    Wt. of Sample Extracted  (g)    % Fat





AR2 E021       Fish                      102.37                  2.2




AR2 D008       Turtle Liver              103.49                  2.2




AR2 D010       Turtle Organs             101.04                 29.9




AR2 E018       Fish                       97.06                  5.1




AR2 E016       Fish                      116.09                  3.4




LA 01          Fish                       98.56                  4.6




LA 02          Fish                       92.10                  6.1




LA 03          Fish                      119.80                  1.5

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tion procedure.  The extracts were combined, filtered through fluted filter
paper, and dried using cleaned sodium sulfate.  The volumes of the extracts
were adjusted to 200 ml, and a 5.0 ml portion of each sample was placed in a
weighed Reactivial  and blown down under nitrogen to determine the percent
fat (or percent extractables) gravimetrically.  The blown-down samples were
redissolved in hexane and recombined with  the appropriate extracts.
     All samples were partitioned into  acetonitrile, and the halogenated
hydrocarbons were back-partitioned into hexane, according to the procedure in
the analytical protocol  (Appendix C).   All of the samples were processed
through the Florisil cleanup procedure.  The 6% ether/hexane and the  15%
ether/hexane fractions resulting from the  Florisil  cleanup were combined, and
the volumes were reduced to 1.0 mL.  Due to the very high background  in the
GC/MS  analysis  (discussed below), all of the samples were chromatographed on
Florisil repeatedly until no yellow  coloration was  observed  in the  concentrated
extract.  For  the Arkansas  samples  (AR2xxxx) this required a total  of  three
cleanup cycles  on the Florisil chromatography column.
ANALYSIS
    „  The samples were analyzed by gas chromatography/mass spectrometry (GC/MS).
Initial attempts at analysis were impeded  by interference from high levels of
lipids and  other background.  Even after a total of three cleanup  cycles on
the Florisil  chromatographic column, the electron impact GC/MS (GC/EIMS)
spectra and selected  ion plots indicated potential  non-halogenated  interferences
even at m/z >  800.  To  confirm the GC/EIMS data, samples were submitted to
GC/negative ion chemical ionization  mass spectrometry  (GC/NICIMS).  This
 technique  detects  only  the  negative  ions  (vs. the positive ions detected in
 "normal"  electron  impact MS) and  can take  advantage of  the electron capturing
properties  (like  GC/ECD)  of certain  chemical classes.   Thus, it is  highly
 selective  for halogenated  organ.  The full scan GC/EIMS analyses of the
Arkansas  samples  found  no  brominated compounds.  A  typical spectrum is presen-
 ted in Figure 1.   The Arkansas  samples  (AR2xxxx) were  also analyzed by GC/EIMS
 in the selected ion monitoring  (SIM) mode  which is  more selective  and  sensitive
 than the  full scan mode.   Table  3 lists the SIM GC/EIMS conditions  for several
 brominated compounds.   A typical  listing of the peak intensities is shown in
 Table 4.   Representative single  ion  plots  are shown in Figure 2.   It  is clear

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that there is very high background from non-brominated compounds, giving
peaks with proper retention times and apparently correct ion intensity ratios
for many brominated compounds.
     To confirm the presence of the brominated compounds, the samples were
submitted to GC/NICIMS.  Typical ion plots are shown in Figures 3-5.  This
technique is far more sensitive than SIM GC/EIMS, so any brominated compounds
should be easily observed by the proper ratio of the m/z 79 and 81 ion plots
(100/98.7).  It should be noted that GC/NICIMS is a new analytical technique
and is subject to the following caveats:  1) relative sensitivities of differ-
ent compounds are not known; 2) all operational parameters have not been
optimized; and 3) the effects of sample matrix have not been thoroughly
investigated.  Thus, GC/NICIMS  data must be interpreted conservatively at
this point.  The tentative findings from SIM GC/EIMS and GC/NICIMS were then
correlated.  Identification of  compounds required that the SIM GC/EIMS peak
be confirmed by GC/NICIMS.  Some peaks observed by GC/NICIMS and not by SIM
GC/EIMS were labeled as "tentative" identifications due to the greater sensi-
tivity of the former technique.  The findings are presented in Table 5.  It
should be noted that TRIS, Tetrabrom, C-.-H.Br,, C,0H0Br.., C, _H,Br,0, C^H.Br^O
                                       L2. 4  O   LZ j  /   Iz 4  O    L2. 6  I
and C,Br OH were tentatively identified by SIM GC/EIMS but not confirmed by
GC/NICIMS.  Thus, analysis by GC/EIMS alone would have yielded several false
positive identifications.
     No effort was made at quantitation.  The high background "noise" levels
in the GC/EIMS data preclude any accurate or even "rough" calculation of the
response values such as those listed in Table 4.   The background interference
in GC/NICIMS is insignificant and quantitation should be feasible.  However,
the technique has not yet been  validated for quantitation.   Based upon the
relative response of the standards and samples, it is safe to extrapolate
that the brominated compounds found were at levels much less than 1 ppm.

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CO
                  4 0
>-.
4J



C
OJ  96-
4J

H  ee-


   78-


   68-


   M-


   48-


   38-


   28-


   10-


   ee-
                                        508
                700


      MOSS SPECTPUM HO.

      UNIT   14 MEMBER
                                                                 ra/z
      T50      /
              m/z
6.63 MJHUTES	I Tf
                                                                         SCO
                                                                                             U|II,I.


                                                                                               850
                                                                                           "l""'""l	I"
                                     198
                                                                          IU, 2.6-9.FS200-200,- I2*0VI01 , 9- 12
         Figure  1.  Full scan GC/E1MS  spectrum  of AR2E021  illustrating very high background.

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  20.0 -


  16.0
1  8-0
   4.0


     0

722* 3


706* 2

800* 1
688* 1
                                      Time (min.)


   Figure 2.   Single ion plots from SIM GC/EIMS analysis  of AR2E021 (see Table 4 for ion intensity
              listings).  Conditions were 45 x 0.2 cm glass column packed with 2% OV-101;  column
              temperature was programmed from 200  - 280°  at 12°/min.;  carrier was helium at 30 mL/min.

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  20.0



  16.0-J
01
a

2  8.0
   4.0



     0
      0
                                                                                                                   502* 1
- 472* 1




  706* 2


  628* 1
                                                      Time  (min.)
                                                  Figure 2. (continued)

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50.0-
40.0
^30.0
*J
•H
m
8 20.0
4J
,3
10.0
A i-


,;.
'^•^^^.''•^^.^•^ 	 , ,--' '~----w-^.~^-.-.-.— .-«— ^"^•"•-'-T*-'
A
" "*"----":'- •-•••••• -"•- 	 •'""' " •"..•
•'
•
                                                                -529* 1

                                                                -502* 1
                                                                 417* 1
                                                                 488* 1
     Time (ntin.)
Figure 2. (continued)

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   Table  3.   SIM MASS  SPECTROMETRY  CONDITIONS FOR
             SELECTED BROMINATED  COMPOUNDS
Compound
C12H6Br4
C12H5Br5
C12H4Br6
C12H3Br7
H Br
12 2 8
C, _HBrn
12 9
C12Br10
C12H6Br4°
C12H5Br5°
C12H4Br6°
C12H3Br7°
C12H2Br8°
r HBr 0
12 9
C12Br10°
Trisd
Firemaster 680e
Tetrabrom
Pentabromophenol
C10C110 (std)
M3
466
544
622
700
778

856

934
482
560
638
716
794
872

950
692
682
540
484
494
SIM Ionsb
470,472
548,550
628,630
706,708
784,788

866

942
486,488,490
564,566
644,646
722,724
800,804
882

958
417,419
688,690
529,531
488,490
502
Intensity Ratio
100/65
100/98
100/73
100/98
100/96




100/65/16
100/98
100/73
100/98
100/96



90/100
100/73
100/25
100/98

a                          79
  Molecular weight, based on   Br.
  Selected ion monitoring ions; generally most
  base clusters.
c Ratio of SIM ion intensities calculated from
  ratios.  Acceptable experimental ratios were
  Tris(2,3-dibromopropyl)phosphate
e 1,2-Bis (2,4,6-tribromophenoxy)ethane
  2,2-Bis(dibromo-A-hydroxyphenyl)propane
intense ions  in parent or

natural isotopic abundance
±50% of stated ratio.
                               12

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Table 4.  RAW DATA FROM SIM GC/EIMS ANALYSIS OF AR2E021
Mass
417
419
470
472
488
490
502
529
531
688
690
529
531
417
419
688
690
630
628
472
470
419
417
488
490
502
529
531
688
690
470
472
502
628
630
706
708
722
724
724
722
690
688
531
529
502
490
488
419
417
630
628
708
706
502
470
472
417
419
628
630
706
708
Peak
Intensity
00
01.
01.
01.
01.
03.
01.
03.
03.
00.
00.
01.
01.
66.
35.
00.
00.
02.
03.
01.
03.
15.
12.
04.
11.
07.
12.
11.
01.
00.
03.
02.
04.
01.
01.
00
00.
00.
00.
00.
00.
00.
00.
10.
13.
05.
09.
04.
11.
08.
01.
02.
00.
00.
05.
03.
03.
10.
05.
01.
00.
00.
00.
96
16
82
48
84
58
92
32
44
44
36
62
14
50
10
56
02
86
90
06
54
16
52
90
22
20
90
34
16
94
60
86
78
82
54
62
40
72
90
58
58
78
66
50
30
84
52
74
88
70
98
02
52
62
28
82
02
36
30
06
66
62
62
Retention Number of
Time Peak Data
(min.) Area Points
2.
1.
2.
2.
2.
2.
2.
2.
2.
2.
2.
3.
3.
4.
4.
4.
4.
4.
4.
4.
'4.
4.
4.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
5.
6.
6.
6.
6.
6.
6.
083
949
066
066
099
066
000
016
000
000
049
416
449
083
233
299
199
499
433
499
516
932
932
033
033
016
033
033
066
033
049
049
049
066
066
116
049
116
099
682
766
666
716.
749
749
766
766
766
782
732
732
749
749
732
799
849
832
266
199
682
799
749
849
09.
56
12.12
30.
29.
29.
53.
28.
54.
44.
03.
03.
23.
14.
2188.
1042.
04.
00.
66.
90.
19.
72.
293.
222.
77.
170.
108.
193.
166.
16.
11.
44.
32.
53.
19.
18.
09.
05.
08.
09.
07.
07.
08.
07.
158.
196.
88.
146.
70.
193.
138.
36.
36.
08.
08.
95.
68.
50.
180.
94.
25.
15.
17.
16.
88
02
88
46
28
10
34
66
42
80
90
26
16
14
02
94
00
68
34
22
04
40
24
64
74
24
76
66
34
88
98
50
78
02
18
54
56
70
30
50
26
14
80
38
56
12
56
76
38
16
38
08
26
22
54
40
30
04
62
40
84
23
23
39
39
33
33
33
33
33
26
26
29
29
65
65
15
15
43
43
38
38
39
35
35
35
35
35
35
35
34
27
27
22
25
25
31
31
28
28
25
25
24
22
30
29
29
29
29
29
29
36
36
33
33
35
35
35
37
37
51
51
53
53
Background
Intensity Comment
12.90
30.22
10.36
07.42
11.04 A
22.22 J
14.58
26.10 ^
22.08/
03.78
03.78
26.42 >
22.12 J
33.54 >
45.92 J
03.74-V
03.787
05.84 A
05.94 J
08.94
14.24
31.74 ^
38.00
08.96
16.84
11.66
20.70
17.00
03.54
03.66
11.44
07.84
11.62 ^
06.34-\
05.86J
03.16
03.00
03.38
03.54
03.64
03.64
03.78 >
04.00
19.40
23.62
14.78
20.18
11.10
25.56
17.50
04.14
04.30
03.22
03.48
12.52
10.24
08.32 J
27.28
38.80
05.10
04.90
03.70
03.48




Possibly C6Br5OH

Too early for Fire-
master 680


Possibly Tetrabrom

Ions do not maximize
at save tine
No real peak

Possibly Cj-H.Br,



Probably non-bromi-
nated background




1





Possibly C12H4Br6






Most likely non-
brooinated back-
ground peak




\
/













                          13

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          80
          60
        to
        c
        01
        >
        u
        m
           40
           20
                                                                ! n/z
                                                                 3 5
                                                                 3 7
                                                                 79
                                                                -3 1
                                                                '156
                                                                - 1 6 0
                                                                 1 6 2
                          100         200
                             Eile Position
300
Figure 3.  Single ion plots from GC/NICIMS analysis of AR2E021.  Conditions
           were 46 x 0.2 cm 2% OV101 column with a helium flow of 13 mL/min.
           Column temperature was at 200° for 2 min. then programmed to
           280° at 12°/min.  Separator temperature was 275°, multiplier
           voltage 2330, trap current 500A, electron energy 50V, and ion
           source temperature 250°.  Brominated compound at file position
           158 is 10 ng C.. -,Br   added during previous analyses as a
           standard.  Brominated compound at file position 182 was
           tentatively identified as C12Br  0.
                                14

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  80
  60
4-1
•H
co

0)
 '40
            \
          n
  20
                                                                              m'z
                                                                              ~3T
                                                                               S 1
                 100
200         300
File Position
400
500
     Figure 4.   Single ion plots from GC/NICIMS analysis of LA01.  Conditions
                were as in Figure 3, except the flow rate was 18 mL/min, the
                final column temperature was 290°C and the ion source tempera-
                ture was 275°C.  Note:  no trace of brominated organics was
                observed.
                                     15

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 80
  60
CD
C
0)
4-1
C
  40
01
PS
  20
                                                                               m/z_

                                                                               35
                                                                               37
                                                                               79
                                                                               81
                 100
200         300

 File Position
400
500
  Figure 5.  Single ion plots from GC/NICIMS  analysis  of LAOS.   Conditions
             were as in Figure 4.  Three brominated  organic peaks are
             clearly observed.
                                   16

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             Table 5.  BROMINATED  COMPOUNDS  FOUND IN FISH AND TURTLE
                       SAMPLES FROM ARKANSAS AND LOUISIANA
Sample Code
    Compounds Found
AR2D008

AR2D010
C12H4Br6
AR2E016

AR2E018

AR2E021

LA01

LAO 2

LA03
E GC/NICIMS data only
C12BrlO° (tent-);

C10BrnnO (tent.)'
C12BrlO°

C12BrlO°
C12BrlO
Three brominated compounds
eluting in the range of a
pentabromo-heptabromo compounds
(—• J.- ' Firemaster 680, C, ~H, Br,. ,etc. )'
                                      17

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                              REFERENCES

Pellizzari, E. D.,  R. A. Zweidinger, and M.  D.  Erickson, "Environmental
Monitoring Near Industrial Sites:   Brominated Chemicals" EPA-
560/6-78-002, June  1978.
Zweidinger, R. A. and E. D. Pellizzari, Development of Sampling and
Analysis Methodology for-Tris(2,3-dibromopropyl)phosphate,  Final
Report on EPA Contract No. 68-01-1978, Task III, May 1978.
Zweidinger, R. A.,  S. D. Cooper, M. D. Erickson, L. C. Michael, and
E. D. Pellizzari, Sampling and Analysis for Semi-Volatile Brominated
Organics in Ambient Air, in Monitoring Toxic Substances, D.  Schuetzle,
ed., ACS Symposium Series 94, 1979, p. 217-231.
                               18

-------
                  APPENDIX A
SAMPLE LOCATION MAP AND FIELD DATA SHEETS FROM
               ARKANSAS SAMPLING
                     19

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20

-------
           Brominated  Compounds Study-Fish Tissue Analysis
                         Field Data Sheet
Station *H2D CO
Secondary #(s) State Atf K USGS
Location Description - £ti^/> ^ p/£» Lo i'-J-v
V
XV A. .-.-.An ^7~P ^ / rt*-? / ^ ' Lo e
Other
t 3-S" 4eSon'
IxhiJ STfi#3.
TlS s ; ^ ^ vi/ ; 5 55
Station Located on Map?
Field Investigators  60h  ^vt»>v»er>^
     Scientific  Name(s) 	
     Habitat
                   V
     Tropic Level    ^Vaia cub I*   -ftrf   v£
Sampl e #      ^.f>v^"	B
     Fish Weight
     No. of Fish
     Length
     Species Common Name(s)
     Scientific  Name(s) 	
     Habitat 	
     Tropic Level 	
                               21

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  Field Observations
  Fish
  Odor
  Color
  Turbidity
   Vegetation
   Scum	
   Flow
   Other
   Comments
   Dischargers
  Field Measurements -   .'St^ox      * -  vvt
                                                    <£, /Ac
  Parameter                Value          Units          Comments
  Dissolved Oxygen         I              *ttW f
  Temperature              3 7*£          ^
  PH
  Conductivity
  Flow                      /^
  Turbidity                < ^?5"         TCU
77 #ro-m,vi g.
                                      22

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Other
                                 23

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           Brominated Compounds Study-Fish Tissue Analysis
                         Field Data Sheet
Station
Secondary #(s)   State  fttfk    USGS          Other
Location Description -   C^LM pv/   ete,  Lc^^rc.    af-   t
       •foTJ>^Q   Si "fa T) Or')
       PS  ;   rf/^M/  ?  5
Station Located  on Map?
Field Investigators   ^nh  Si no fe. Ton   a^-iJ  .ToKh
Date "7- //~7?    Time
Sample I  /^if^DOJO     em I j  6)
                                                            --   So
     Tropic Level   Pro^f     -ft    *f*
Sample #
     Fish Weight
     No. of Fish
     Length
     Species Common  Name(s)
     Scientific Name(s) 	
     Habitat         	
     Tropic Level 	
                               24
                  K/./  r/^<^   -fitf/r  -tits**-  wl  //v€**   (/}
                                  ^~^^r  1^ "^^^^^^^^^^^   -* •     ^
     Scientific  Name(s) _^ _ •
     Habitat    <         '

-------
Field Measurements
Parameter
Dissolved Oxygen
Temperature
PH
Conductivity
Flow
Turbidity
Field Observations
Fish	
Odor
Color
Turbidity
Vegetation
Scum	
Flow
Other
Value
£.c?
/9.«v*
 7.Q
Units
                                                      Comments
                                       TTfrc
Comments
Dischargers    All
                                25

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Other
                               26

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               Brominated Compounds Study-Fish Tissue Analysis
                              Field Data Sheet
>
     Station
     Secondary #(s)   State Atfk     USGS	Other
     Location Description -   Cornie.   Be** on   /.
         Taps     & /5"w
     Station Located on Map? (fepNo
     Field  Investigators
     Date  7-yO-7f     Time yo/cc
     Sample f   ft £ 2 E.O l'^
          Fish Weight
         No. of Fish    A'*/"
         Length
         Species Common Name(s)
         Scientific Name(s) _^	
         Habitat
         Tropic Level
    Sample #	Hc-y^«—	B
         Fish Weight _/	
         No. of
         Length
                        *
         Species Common Name(s)
         Scientific Name(s)
         Habitat
         Tropic Level	
                                   27

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Field Measurements -
 • :<•  £>-* oa
Parameter
Dissolved Oxygen
Temperature
PH
Conductivity
Flow
Turbidity
Field Observations
Fish	
Odor
Color
Turbidity
Vegetation
Scum	
Flow
Other
Comments
Dischargers
Value
                                       Units
Comments
                         -7.J
                                        JCuk
                                  28

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*  Other
                                   • /
                                    J,
                               29
                                                         //

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           Bronrinated Compounds Study-Fish Tissue Analysis
                          Field Data Sheet

Station *  A R 3 £ O I & _
Secondary #(s)    State _  USGS _ Other _
Location Description -   C. Or n I p.   P, »** n L »    6  r>- ,'Jr
                                         ---
       "T/ffS '
          ,—
Station Located on Map?(Yes^No
Field Investigators  j^o^  J? ry f^-^s^w   (>A^   JTcK
Date  7"// • 7f   Time  V
Sample #  A if ^ £  0 / 5"
     Species Common Name(s)
     Scientific Name(s)
     Habitat
     Tropic Level
Sample I
     Fish Weight
     No. of Fish
     Length 	
   ,  Species Common Name(s)
     Scientific Name(s) 	
     Habitat m	
     Tropic Level 	
     Fish Weight
     No. of Fish    A'S^~  g>x.   &<*-<.(<
     Length
                             30

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Turbidity
Field Observations
Fish	
Odor
Color
Turbidity
Vegetation
Scum	
Flow
Other
Comments  •
Dischargers
 r-  -,-, n
 Field Measurements -
                  •
.Parameter                Value          Units          Comments
 Dissolved Oxygen         5^ j*3          »,./ /
 Temperature              ^?k *            C
 PH                       4.V0         _
 Conductivity             ^-6^          x* fl t

                                 31

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Other
                                      .  S
                                      .  y
                              32

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           Brominated Compounds Study-Fish Tissue Analysis
                          Field Data Sheet
Station I   Atf
Secondary #(s)   State A )? /C   USGS _ Other
Location Description -   T^f^,,*far}>  e •£
       My ^/^  /.c.    T/35 ;.
Station Located on Nap? (fep'No
Field Investigators
Date 7-IO-7?     Time   ? : Oo
Sample I   A 1?
     Fish Weight
     No. of Fish      /if  ow
     Length
     Species Common Name(s)
     Scientific Name(s)   .
     Habitat
     Tropic Level
Sample # 	
     Fish Weight 	
     No.  of Fish	
     Length 	
   \  Species Common  Name(s)
     Scientific Name(s)
     Habitat
     Tropic Level	•_ ._
                            33

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Field Measurements  — H1*~.
Parameter                Value           Units           Comments
                                                                       *
Dissolved Oxygen         	          	          	
Temperature              	          	          	
PH                       	          	          	
Conductivity             	          	          	
Flow                     	          	          	
Turbidity                	          	          	
Field Observations

Fish	
Odor
Color
Turbidity
Vegetation
Scum	
Flow
Other
Comments
Dischargers
                                 34

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Other
  /5
  7
                              35

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                  APPENDIX B
SAMPLE LOCATION MAP AND FIELD DATA SHEETS FROM
              LOUISIANA SAMPLING
                     36

-------

-------
          Brominated Compounds Study-Fish Tissue Analysis
                         Field Data Sheet
Station #    LAOI
Secondary #(s)   State _  USGS _ Other

Location Description -  Bavou  De Lutrp  at Hwy 9  R-r-i

 La Station # S08-0210-010

 Union  Parish, La.

Station  Located on Map? Yes/No

Field Investigators     Louis  R. C. Johnson

Date i n  ang-h      Time n« • nn _
Sample $ _ A

     Fish  Weight   2 ibs
     No. of Fish    3
     Length _ 2 (9 inches)  1(10  inches)
     Species Corrraon Name(s)  LM Bass
     Scientific Name(s)      MlcroFtQ'ruE Salmcidoc
     Habitat
     Tropic Level
 Sample # _ •>
      Fish Weight    1.5

      No. of Fish
      Length	3  inches to 6  inches
    \
Species  Common Name(s)    Bream
      Scientific Name(s) 	Lepomis  species

      Habitat                      	
      Tropic Level	JJO.D Preditory-food-iish.

                                ,  38

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Field Measurements
Parameter
Dissolved Oxygen
Temperature
PH
Conductivity
Fl ow
Turbidity
 Field Observations
Fish
Odor
        yes
        None
 Color   Dark
Turbidity
 Vegetation   Yes
 Scum	
 Flow
            None
                        Value
Units
Comments
                              NONE
             Average
 Other
 Comments
 Dischargers
                                  39

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Other
                                     40

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           Brominated Compounds Study-Fish  Tissue Analysis
                         Field Data Sheet
Station #    LAO2
Secondary #(s)   State _  USGS _ Other_
Location Description -   Bayou  DeLutre     Huey  33
          TTm'nn Pa-rich
Station Located  on  Map? Yes/No
Field Investigators  L.  R. C.  Johnson
Date 10 August     Time  10:15 hrs
Sair.pl e # _ A
     Fish  Weight  2 Ibs,  3 oz.
     No. of Fish2
     Length _ 15  inches
     Species Common Name(s)      Gar
     Scientific Name(s)   ;   Lepisoteus  species
     Habitat          Preditor
     Tropic Level
 Sample #	
     Fish Weight
     No. of Fish
     Length
     Species Common Name(s)
     Scientific Name(s) 	
     Habitat 	
     Tropic Level 	
                                41

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Field Measurements
Parameter
     »
Dissolved. Oxygen
Temperature
PH
Conductivity
FT ow
Turbidity
                        Value
Units
Comments
                                 NONE
 Field Observations
Fish	
Odor     None
          Some  seen
 Color     Amber
 Turbidity Nn
 VegetationNone
 Scum     None
 Flow
 Other
          Moderate
 Comments
 Dischargers
                                    42

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Other
                                     43

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           Brominated Compounds Study-Fish Tissue Analysis
                         Field Data Sheet
Station #  LA03
Secondary #(s)    State	  USGS	Other	
Location Description  -   r^-n^-, T«va-.onrir r~nth bank rnrt  nf TT;
                        *-rt-f-L "".i  J-J«-*-~w*,_L Tjrii ^ £_XJ'W HI UiillJT* t/tLi-f L  LJ J. t *
 Forestry  service  Boat Launch  Claiborne  Parish,   Louisiana


Station Located on Map?  Yes/No
Field Investigators  L. R. C.  Johnson	
Date 10 August      Time 12:00 hrs
Sample ? 	 A
     Fish Weight     2  Ibs, 4  oz	
     No. of Fish	3	
     Length        15 inches	
     Species Common Name(s)   Gar	
     Scientific Name(s)      Lepisos-teus
     Habitat
     Tropic Level     Preditor
 Sample #	
      Fish Weight
      No. of Fish
      Length 	
      Species Common Name(s) 	
      Scientific Name(s) 	
      Habitat 	
      Tropic Level 	
                                  44

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.Field Measurements
Parameter
Dissolved Oxygen
Temperature
PH
Conductivity
Flow
Turbidity
 Field Observations
 Fish
Some
 Odor    None
 Color   Clear
 Turbidity  Clear
 Vegetation   Heavy
 Scum _
 Flow _
 Other
   None
                Value
Units
Comments
                         NONE
 Comments
 Dischargers
                                     45

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Other
                                     46

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                        APPENDIX C
ANALYTICAL PROTOCOL:  SAMPLING AND ANALYSIS OF EXTRACTABLE
              HALOGENATED ORGANICS IN TISSUE
                            47

-------
   ANALYTICAL PROTOCOL:   SAMPLING AND ANALYSIS OF EXTRACTABLE HALOGENATED
                             ORGANICS IN TISSUE

1.0  Principle of Method
     Semi-volatile halogenated hydrocarbons are extracted from tissue samples
with organic solvents, dried, and concentrated to an appropriate volume for
quantification using GC/ECD.  Identifications are confirmed by GC/ECD  using
a second column and, when sufficiently concentrated, by GC/MS/COMP.  Samples
are optionally subjected to liquid chromatographic cleanup on Florisil to
remove lipids if severe interferences are encountered.  This procedure was
adapted from that of Thompson (Al).
2.0  Range and Sensitivity
     The sensitivity of response to GC/ECD is a function of the instrument,
the compound, and the matrix from which it is extracted.  The detection
limit for GC/ECD analysis is 1-5 ng/g (ppb), depending on compound and
instrumental conditions.
3.0  Interferences
     Interferences in sample analysis and quantification using GC/ECD are
manifested in the electron capturing ability of the given contaminant.
Blood extracts which have not been cleaned up contain interferences which
can largely be removed by gradient liquid-liquid chromatography on 2% aqueous
deactivated Florisil and/or back partitioning with acetonitrile, as discussed
below.
4.0  Precision and Accuracy
     Preliminary recovery results, shown in Table A.-1 indicate that recoveries
are from 60-90% for several types of tissue.  Further recoveries will be
determined with individual samples as they are analyzed throughout the
program.
5.0  Apparatus
5.1  Sampling Apparatus
     Samples must be collected and stored with a minimum potential for con-
tamination or loss of more volatile components.  The primary cause of
contamination is from plasticizers (£•£•, phthalates) in plastic and rubber.
Therefore contact with these materials must be minimized or eliminated.
                                      48

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   Table A-l.  RECOVERY  OF EXTRACTABLE  HALOGENATED  HYDROCARBONS

                    FROM HUMAN  TISSUE EXTRACTS
Tissue
Adipose0
Brain
Liver
Kidney
Spleen
Lung
Percent
Extractable
Material3
84.3
4.4
1.1
1.1
1.3
0.4
Percent,
Recovery
76.6
69.7
85.1
64.5
91.2
87.5
  Also described as "percent fat" in some procedures.
  Recovery of 198 ng aldrin added to tissues after maceration and before
  extraction as an internal standard.  Percent recovery determined after
  all analytical manipulations.  Aldrin represents a suitable standard,
  since it is metabolized to endrin and has not been found in tissues.
  Mean recovery for adipose tissues « 79.1 + 10.6%.

C Analytical workup includes acetonitrile partitioning to reduce fat
  content.
                                 49

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Samples should be stored in glass jars with foil-lined or (preferably)
teflon-lined screw caps.  The bottles must be thoroughly cleaned and oven-
treated prior to use.
5.2  Extraction Apparatus
     Beakers (500-1000 ml), 500 ml Kuderna-Danish evaporators (or 10 ml
nicroevaporators) and receiving tubes, three ball Snyder columns, glass
                                                         ®
bottles and caps equipped with Teflon liners, reactivials , centrifuge, and
22 mm i.d. chromatography columns.  Solvent: hexane, distilled in glass and
redistilled prior to use.  Reagents: sea sand, anhydrous sodium sulfate,
(extracted with pentane in Soxhlet extractor for 24 hr and stored in an oven
at 140°C), 60/100 mesh reagent Florisil.
6.0  Procedure
6.1  Collection of Samples
     It is anticipated that tissue samples collected from cadavers or surgery
will be obtained from a pathologist.  Personnel from RTI will work with
pathologists advising them of proper sample handling procedures.  To be of
use for extractable halogenated organics a tissue sample must be collected a
short time following death and immediately frozen in a cleaned glass container
with as small a "headspace" as possible.  Any handling or storage in contact
with polymeric materials represents potential contamination.
6.2  Extraction, Cleanup, and Concentration
     Tissue fractions are analyzed for extractable halogenated organics
using a modified procedure by Thompson (Al).  Approximately five grams of
each tissue is ground in a large glass beaker with acid-washed sea sand and
sodium sulfate (both cleaned up prior to use by extraction in a Soxhlet
extractor with hexane) using a glass rod until a dry, granular mass is
obtained.  Aldrin, 198 ng in 100 \il hexane, is added to the sample as an
internal standard.  Each tissue is then extracted, with vigorous grinding,
with three 50 ml aliquots of hexane for approximately 5 min each.  The
extracts are then filtered, concentrated in a Kuderna-Danish (KD) apparatus
to approximately 10 ml, blown down under nitrogen to dryness at room tempera-
ture and weighed to obtain a value for the percent extractable material
("percent fat").
                                       50

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     The high  lipid content of adipose tissue extract necessitates partition-
ing of the extract into acetonitrile and back-partitioning of the halogenated
hydrocarbons into hexane.  Approximately 2.5 grams of fat extract is dissolved
in 12 ml hexane and extracted two min each with  four 30 ml aliquots of
redistilled acetonitrile.  The extracts are combined with 250 ml 2% aqueous
sodium chloride and back-extracted with four 30  ml aliquots of hexane.  The
extracts are combined, dried over Na2SO,, concentrated in a KD to about 5
ml, blown down under nitrogen to approximately 2 ml, and subjected to Florisil
cleanup as described below.
     Florisil  (60/100 mesh, activated at 130°C overnight) columns (2.2 cm x
10 cm) with glass frits or glass wool plugs are  packed in hexane solvent.
Each tissue extract is transferred to the surface of the column in approxi-
mately 2 ml of solvent, and the column walls are washed with approximately 4
ml of hexane.  The halogenated hydrocarbons are  then eluted with 200 ml each
of 6% ether/hexane and 15% ether/hexane respectively.  Each fraction is
concentrated in a KD apparatus to approximately  5 ml.  The 6% eluants are
blown down under ambient nitrogen to appropriate volumes and immediately
analyzed by GC/ECD.
     Previous  studies by Thompson suggest the following halogenated hydro-
carbons should be found in the 6% eluant:  BHC isomers, £,£'-DDE, £,£'-DDT,
heptachlor, heptachlor epoxide, mirex, PCB, hexachlorobenzene, and trifluralin
(HI).  These represent the same general polarity of the halogenated compounds
of interest in tissue samples, so this fraction  is of primary interest for
analysis.  Extracts are dried a minimum of 30 minutes over about 0.5 g anhy-
drous Na.SO,.  The extract is transferred to a 500 ml KD flask (or micro
KD), topped with a Snyder column, concentrated to ca. 2-4 ml, and cooled to
ambient temperature.  The sides of the KD are rinsed with about 1.5 ml
hexane and the extract is then blown down under  nitrogen to about 1 ml,
                           ©
transferred to a reactivial  previously calibrated to a specific volume, and
.further concentrated.
6.3  Instrumental
     The detection and quantification of semi-volatile halogenated hydrocar-
bons is made using a Series 4400 Fisher/Victoreen Gas Chromatograph equipped
with a tritium foil electron capture detector.   Separation is effected on a
                                        51

-------
40 m, 0.38 mm i.d.,  glass SCOT capillary column coated with 1% SE-30 on
0.32% Tullanox (A2,A3).   Maximum efficiency is obtained with a flow rate of
2.5 ml/min of nitrogen gas with makeup nitrogen gas adjusted to a total flow
of 25.0 ml/min, column 220°C (isothermal), and detector 285°C.
     As a confirmatory column a 190 cm x 0.2 cm i.d. 1.5% OV-17/1.95% QF-1
on 80/100 Chromosorb W-HP packing is employed.  Efficient responses are
obtained for flow rates of 18 ml/min at identical column and detector tempera-
tures .
     Final confirmation of the identity of the components of sufficiently
concentracted extracts (generally greater than 10 ng/pl) can be made using
GC/MS/COMP.
     The GC/MS/COMP systems used are a Finnigan 3300 GC/MS/COMP and an LKB
2091 GC/MS equipped with an LKB 2031 data system.  Chromatographic conditions
for the Finnigan 3300 are 20 m x 0.38 mm i.d., 1% SE-30 SCOT capillary
operated isothermally at 235°C and a flow rate of 2.0 ml/min helium.  Split-
less injection (0.2-0.3 pi) is used, with standard electron impact (70 eV)
ionization conditions.
     The LKB 2091 is operated using a 18 m 1% SE-SO/BaOX WCOT capillary
column at 240°, isothermal for PCBs and a 40 m x 0.38 mm i.d. 1% SE-30 SCOT
capillary column at 230° isothermal for the pesticides.  In both cases, the
column flow rate is 2 ml/min with 20 ml/min split off at the injector.  The
mass spectrometer is operated under standard electron impact conditions.
6.4  Qualitative and Quantitative Analysis
     6.4.1  Qualitative Analysis
     Alternate single injections of extracts and standard solutions is the
routine procedure for processing samples.  If the retention time of a given
component of an extract suggests the presence of a standard compound, a
repetitive injection  is then made.  Tentative identification is made if the
deviation between the two respective means is no greater than three percent.
A similar criterion is then applied to the retention times of both extract
and  standard component upon a second, confirmatory, column   Qualitative
identification of a component is made if both criteria are satisfied.
                                        52

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      6.4.2  Quantitative Analysis
      A mean linear response range of 5-160 pg/pl has been established for
 the compounds trifluralin and Y'BHC on a 1% SE-30/0.32% Tullanox 40 m,  0.38
 mm i.d. SCOT capillary column installed in a Series 4400 Fisher/Victoreen Gas
 Chromatograph.   Quantification of given component is made by a comparison of
 the means of recorder trace areas of two extract and two standard solutions
                                                           I
 within this linear response range.  The precision of the concentration  of a
 given component is normally less than ten percent of the mean concentrations
 and is obtained by propagation of the standard deviations of the responses
 of both the extract and standard solutions.  The effective concentration
 multiplied by the volume of extract results in the total amount of extracted
 material.
      If the extracts are deep yellow, the presence of lipids may interfere
 with either analysis or concentration of the extracts due to precipitation.
 In this case, the sample should be transferred to a 22 mm i.d.  column contain-
 ing 1.6 g of 2% aqueous-deactivated Florisil and eluted with 10 ml each of
 hexane, 5% MeCl2/hex, 10% MeCl2/hex, 15% MeCl2/hex, 20% MeCl2/hex, 30%
 MeCl2/hex, 50% MeCl2/hex, and MeCl2-  The extracts are concentrated and
 analyzed.  Most semi-volatile halogenated hydrocarbons are expected to
 appear in the first five fractions.  This estimate is based upon elution
 data of pesticides on Florisil (A4) and has not been subjected to full
 experimental verification.
      6.4.3  GC/MS/COMP Confirmation
      The chromatography conditions are similar to those used for GC/ECD.
 The samples for this study are to be screened by GC/ECD and confirmed (if
 sufficiently concentrated) by GC/MS/COMP.  Therefore, the retention times of
 the two techniques must be similar.  GC/ECD must operate isothermally,  so
.the GC/MS/COMP conditions reflect this restriction.
      The Finnigan 3300 and the 1KB 2091 systems may be operated in both the
 full scan and selective ion monitoring (SIM) modes.  In the full scan mode,
 full spectra are collected.  Spectra or mass fragmentograms (single ion
 plots) may be plotted for interpretation.  In the SIM mode, only a small
 number (up to 9 for the Finnigan 3300 and up to 16 for the 1KB 2091) of ions
 are monitored.   Full spectra are not collected.  The advantage of this
                                       53

-------
method is that the detector spends more time "looking" at the selected ion
and therefore better (generally 10-50 times) sensitivity is obtained.
     To determine the limits of detection, standard solutions of selected
pesticides and PCB isomers have been analyzed on the Finnigan 3300 and 1KB
2091.  In the full scan mode, the limit of detection was the amount of
compound required for an interpretable spectrum.  In the SIM mode, the limit
of detection was the amount of compound required to yield a peak 2-4 times
the noise level.
     The estimated limits of detection for the Finnigan 3300 and LKB 2091 are
presented in Table A-2.
     Quantitation using GC/MS/COMP is achieved by comparing the computer-
calculated integrated area of the unknown with the integrated response for a
known amount of standard.  To compensate for differences in ionization
cross-section, the relative molar response of authentic compounds is obtai-
ned.
     The calculation of the relative molar response (RMR) factor allows the
estimation of the levels of sample components without establishing a cali-
bration curve.  The RMR is calculated as the integrated peak area of a known
amount of the compound, A° , , with respect to the integrated peak area of a
                         UQ.K
known standard, A°  , (in this case d,Q-pyrene), according to the equation

     R = A°unk/molesunk   =    (A°unk)  <                                      '""5 (RMR)
     The use of RMR for quantitation by GC/MS has been successful in repeated
applications to similar research problems.
     The RMRs for the compounds were calculated from the numerical inte-
grations of peaks observed in the appropriate SIM channel.  Typical RMRs
listed in Table A-3 and A-4 are mean values of three injections of each of
three replicate standard mixtures .
                                      54

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Table A-2.  ESTIMATED LIMITS OF DETECTION FOR EXTRACTABLE HALOGENATED
                       ORGANICS ANALYSIS3

LKB
2091b
Finnigan 3300a
Full Scan SIM
Compound
trifluralin
atrazine
Y-BHC (lindane)
heptachlor
chlordane
£,£f-DDE
2-chlorobiphenyl
hexachlorobiphenyl
decachlorobiphenyl
ng/yl
12
>12<20
>12<20
12
^30C
12
*1
<1
12
m/z
264
200
181
272
375
246
188
360
498
ng/yl
0.4
0.4
0.10-0.4
0.10-0.4
5
>0.3
0.004
MD.016
0.42
Full Scan SIM
ng/yl
5-10
<50
5-10
10-20
25-50
5-10
•x.2.5
25-50
150
m/z
264
200
181
272
375
246
188
360
498
ng/yl
<0.5
5-10
1
1-1.5
5-10
0.5-1
^0.025
M).15
•vO.3
 See text for conditions.
 15:1 split at injection,  only 1/15 of injection is on column.
C0.2 yl injected with no split.
                                 55

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        Table A-3.   RMRs FOR PCBs AND PESTICIDES OF INTEREST
                         TO THIS PROGRAM3
9
Compound
2-chlorobiphenyl
hexachlorobiphenyl
decachlorobiphenyl
trif luralin
atrazine
lindane
heptachlor
£,£'-DDE
chlordane (peak 1)
chlordane (peak 2)
Concentration
104 ng/yl
3.8 ng/yl
570 ng/yl
10. A ng/yl
1156 ng/yl
8.4 ng/yl
100 ng/yl
100 ng/yl
100 ng/yl
100 ng/yl
100 ng/yl
100 ng/yl
100 ng/yl
Ion
188
360
498
264
200
202
181
183
272
246
373
375
373
375
RMR
elutes with solvent
and was two scans wide -
not detenninable
.38 -1- 3%
.35 + 10%
.14 + 7%
not detenninable
1.32 + 20%
.74+7%
.25 ± 8%
.74+9%
.62 + 12%
.74 + 6%
.45 + 6%
.71 + 5%
.65+5%
.051 + 6%
.045 + 13%
SStandard is d  -pyrene (m/_z = 212)
              10
                                  56

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                      Table A-A.  RMR FACTORS FOR STANDARD PCB SOLUTIONS,
                                  SELECTED ION MONITORING MODE
     Standard
      RMR
    ffl/z 188
2-Chlorobiphenyl
        RMR
      m/z 358
Hexachloroblphenyl
                                                         RMR
                                                       m/z 498
                                                Decachlorobiphenyl
   I  PCB-STD-20

  II  PCB-STD-2
 III  PCB-STD-0.2
Ol
-J
  IV  PCB-STD-0.04
0.60

0.620"^

0.466  f
0.643J

0.566"^
0.840
0.637
0.597
0.705
                                         0.640+ .171
                                         (0.699 +.171
      1.020"\
      0.692  > 0.763 +.257
      0.57&J
                                 0.257
                                 0.291"^
                                 °'334  \0 325 +  009
                                 0.319  /U-J23 ± -oov
                                 0.321J
0.366
0.293
0.301
0.239
0.273
                                         0.294 + .072
                           0.320~\
                           0.528  10.
                           0.528 J
                                                                      459 + .072
                                   0.341

                                   0.430
                                   0.474
                                   0.462
                                   0.431
                                                                                              J
0.372*^
0.361
0.373
0.303
0.394
                                          + .018
                                           0.361    .033
                                   0.287*^
                                   0.543  ) 0.401 -1-  .142
                                   0.372 J
  Standard is d._-pyrene  (m/z = 212).

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     The RMRs given here are to be regarded as typical values.  Not only
must they be determined for each instrument, but day-to-day variations are
sometimes large enough to require daily calibration.
7.0  Quality Assurance Program
     In addition to the validation procedures described above, an on-going
quality assurance program is required to assure the data quality.  Quality
control (QC) procedures determine artifacts, losses, etc. through a system
of blanks and controls.  Quality assurance (QA) procedures monitor the
execution of the procedure and check data interpretations and calculations.
7.1  Quality Control
     7.1.1  Field Blanks and Controls
     Prior to a field sampling trip, enough blanks and controls are prepared
to equal 10% each of the anticipated number of field samples.  Blanks consist
of 50 ml of distilled water in the same type of sampling container as is
used in the field.  Controls consist of 50 ml of plasma spiked at 10-15 ng
with the compounds listed in Table A-5.  These blanks and controls are
carried to the field and receive the same handling as tne field samples.
Workup and analysis of field blanks and controls is interspersed with the
field samples on a regular basis.  This method allows assessment of sample
storage stability.
     7.1.2  Procedural Blanks and Controls
     7.1.2.1  Extraction Blanks
     With each set of samples, a procedural blank is run.  This consists of
5 ml of prepurged distilled water which is extracted under the same conditions
as the samples.  These blanks are designed to detect artifacts from dirty
glassware, laboratory atmosphere intrusion, and other sources.
     7.1.2.2  GC/MS Procedural Control
     At the start of each working day, a mixture of 2,6-dimethylphenol,
2,6-dimethylaniline, and acetophenone (PA mixture) is analyzed to monitor
the capillary GC column performance.  This also serves to check the mass
spectrometer tuning.
     Field, samples, field controls, field blanks, and procedural blanks are
queued up for GC/MS analysis such that at least one QC sample is run each
working day.  In addition, a standard solution is analyzed each day to serve
                                      58

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  Table A-5.  SEMI-VOLATILE HALOCENATED HYDROCARBONS  113
                METHANOL SPIKING SOLUTION
     .Compound                             Ai-.t. spiked, ng

4-Chlorobiphenyl                                13.2

Trifluralin                                     14.8

a-BHC                                           14.0

e-BHC                                           14.5

Y-BHC                                           15.2

4,4'-Dichlorobiphenyl                           15.8

2,4,5-Trichlorobiphenyl                         14.0

Heptachlor                                      13.6

Aldrin                                          14.8

Heptachlor epoxide                              14.2

Endosulfan                                      13.1

Dieldrin                                        15.8

p,p'-DDE                                        11.6

p.p'-DDT                                        12.5

Endrin                                          11.5
                              59

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as a procedural control and also to update the RMR value.  Thus, in a typical
working day, 4 field samples, 1 blank or control, and 1 RMR standard are
run.
     The Finnigan 3300 GC/MS is a quadrupole mass spectrometer which requires
frequent tuning.  Daily tuning is achieved using FC-43 and decafluorotriphenyl-
phosphine (DFTPP).
7.2  Quality Assurance
     7.2.1  Supervision and Monitoring of Activities
     There are three levels of quality assurance (QA).  The primary quality
assurance is the person conducting the sampling and/or analysis.  This
person must be aware of their actions, observe events which may effect the
data, and maintain appropriate records.  At the second level,  the chemist's
supervisor monitors their daily activities, reviews the notebook, checks
data and calculations, and assists in "troubleshooting" problems.  At the
tertiary level, a QA coordinator interviews all personnel on the project.
The interviews cover the operations they perform (precisely),  the data they
obtain, a spot-check of their calculations, and any problems they have had.
     7.2.2  Documentation
     7.2.2.1  Chain of Custody
     From the initial preparation of a sample container through reporting of
the analytical results, each sample is accompanied by a chain  of custody
sheet-.  Each person signs in the time of receipt, operations performed,  and
transmittal of the sample.  This record is important for tracing a contaminant,
bad standard, or some other problem.
     7.2.2.2  Sampling Protocol Sheets
     When a sample is collected, a sampling protocol sheet is  filled in
which contains a discrete sample code which identifies project number, area,
site, locations, trip number, sampling period, and sample type.   Also included
are sample times, volumes, addresses, meteorology, and other pertinent
information.  Where appropriate, a map is made to precisely identify the
location.
     7.2.2>i3  Sample Log
     Upon return from a sampling trip, each sample code is entered into a
sample log book.  This log is updated as samples proceed through workup and
                                        60

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analysis.  Thus, at a glance, project personnel can tell the status of each
sample and find out how many are at different stages in the analytical
procotol.
     7.2.2.4  GC/MS Log
     Each sample.run by GC/MS is logged into a notebook, detailing analysis
conditions, where the data are archived, and what hardcopy data has been
produced.
8.0  References
Al.  Thompson, J. F., Analysis of Pesticide Residues in Human and Environ-
     mental Samples, A Compilation of Methods Selected for Use in Pesticide
     Monitoring Programs, Environ. Toxicol. Div., Health Effects Research
     Lab., USEPA, RTP, NC, December, 1974.
A2.  Hines, J. W., R. Shapiro, E. Pellizzari and  A.  Schwartz, HRC and
     CC, submitted for publication (1978).
A3.  Hines, J. R., R. Shapiro, A. Schwartz, and E. D.  Pellizzari,  HRC  and
     CC, submitted for publication (1978).
A4.  Sherma, J., Manual of Analytical Quality Control  for Pesticides and
     Related Compounds, EPA-600/1-76-017, 1976, Table  7-1.

Revised, April, 1979
                                       61

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                                   TECHNICAL REPORT DATA     .
                                  d Instructions on the reverse before completing/
1. REPORT NO.
EPA-560/13-80-006
                                                           3. RECIPIENT'
4. TITLE AND SUBTITLE
Sampling  and Analysis of Selected Toxic Substances
Task  2:   Analysis  for Semivolatile Brominated  Organics
          in Fish and Turtles
                                                           5. REPORT DATE
6. PERFORMING ORGANIZATION CODE

 31U-1706-2	,	
7. AUTHOR(S)
M. D. Erickson,  K.  B.  Tomer, J. T. Bursey, M.  A.  Moseley
and E. D. Pellizzari
                                                           8. PERFORMING ORGX
                                                            Tm/1706/02-F
9. PERFORMING ORGANIZATION NAME AND ADDRESS
 Research  Triangle  Institute
 Post Office Box 12194
 Research  Triangle  Park,  North Carolina  27709
                                                           10. PROGRAM ELEMENT N
11. CONTRACT/GRANT NO.

  68-01-5020
12. SPONSORING AGENCY NAME AND ADDRESS
 Office of Pesticides and Toxic Substances
 U. S. Environmental Protection Agency
 Washington,  D.  C.   20460
13. TYPE OF REPORT AND PERIOD COVERED

  Final
14. SPONSORING AGENCY CODE
 15. SUPPLEMENTARY NOTES
 Project Officers are Vincent J. DeCarlo and  Thomas  E.  Kopp
 16. ABSTRACT
       Fish  and turtle (5 from Arkansas and  3  from Louisiana) caught downstream of
  the brominated organic chemical industry near  El Dorado,  AR were extracted,  cleaned
  up, and  analyzed by GC/MS for brominated organics using full scan and  single ion
  monitoring electron impact GC/MS and negative  ion chemical ionization  GC/MS.  PBBs
  (C^Hi+Brg  and C^f^Bry) were identified in one sample and several other  brominated
  compounds  were tentatively identified in several samples.  Due to the  high levels
  of interferences and very low levels of the  compounds of  interest, further identi-
  fications  were impossible.  The compounds  were not quantitated, but levels appear
  to be much less than 1 ppm.
17.
                                KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
                                              b.IDENTIFIERS/OPEN ENDED TERMS
                                                                         c. COSATI Field/Group
  Brominated  Organics
  Fish
  Turtles
  GC/MS
  PBBs
  GC/NICIMS
  Polybrominated  biphenyls
  Release unlimited
                                              19. SECURITY CLASS (This Report)
                                                unclassified
              21. NO. OF PAGES
                   70
                                              >0. SECURITY CLASS (This page/
                                                unclassified
              22. PRICE
                                             62

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