&EPA
           United States
           Environmental Protection
           Agency
          Environmental Monitoring and Support EPA-600 4-78-058
          Laboratory          October 1978
          Research Triangle Park NC 27711
           Research and Development
Collaborative Testing of
EPA Method 106
(Vinyl Chloride) that
Will Provide for a
Standardized
Stationary Source
Emission
Measurement Method

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                RESEARCH REPORTING SERIES

Research reports of the Office of Research and Development, U.S. Environmental
Protection Agency, have been grouped into nine series. These nine broad cate-
gories were established to facilitate further development and application of en-
vironmental technology.  Elimination of traditional grouping was  consciously
planned to foster technology transfer and a maximum interface in related fields.
The nine series are:

      1.  Environmental  Health Effects Research
      2.  Environmental  Protection Technology
      3.  Ecological Research
      4.  Environmental  Monitoring
      5.  Socioeconomic Environmental Studies
      6.  Scientific and Technical Assessment Reports (STAR)
      7.  Interagency Energy-Environment Research and  Development
      8.  "Special" Reports
      9.  Miscellaneous Reports

This report has been assigned to the ECOLOGICAL RESEARCH series. This series
describes research on-the effects of pollution on humans, plant and animal spe-
cies, and materials. Problems are assessed  for their long- and short-term influ-
ences. Investigations include formation, transport, and pathway studies to deter-
mine the fate of pollutants and their effects. This work provides the technical basis
for setting standards to minimize undesirable changes in living organisms in the
aquatic, terrestrial, and atmospheric environments.
This document is available to the public through the National Technical Informa-
tion Service, Springfield, Virginia 22161.

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COLLABORATIVE TESTING OF EPA METHOD 106 (VINYL CHLORIDE)
 THAT WILL PROVIDE FOR A STANDARDIZED STATIONARY SOURCE
               EMISSION MEASUREMENT METHOD
                           by

                    George W. Scheil
                    Michael C. Sharp
               Midwest Research Institute
              Kansas City, Missouri  64110
                      FINAL REPORT

               EPA Contract No. 68-02-2737
                 MR! Project No. 4420-L
                   EPA Project Officer
                    M. Rodney Midgett
                Quality Assurance Branch
     Environmental Monitoring and Support Laboratory
      Research Triangle Park, North Carolina  27711
                      Prepared for

     Environmental Monitoring and Support Laboratory
           Office of Research and Development
          U.S. Environmental Protection Agency
      Research Triangle Park, North Carolina  27711

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                                 DISCLAIMER
     This report has been reviewed by the Environmental Monitoring and Sup-
port Laboratory, U.S. Environmental Protection Agency, and  approved  for pub-
lication. Approval does not signify that  the contents necessarily reflect the
views and policies of the U.S. Environmental Protection Agency, nor  does men-
tion of trade names or commercial products constitute endorsement or recom-
mendation for use.

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                                  FOREWORD
     Midwest Research Institute,  under EPA Contract  No.  68-02-2737,  conducted
collaborative tests of Method 106,  "Determination  of Vinyl  Chloride  from Sta-
tionary Sources." A group of 10 collaborators at their own  laboratories  ana-
lyzed six simulated samples containing vinyl chloride and interferring com-
pounds. Three laboratories then obtained field samples and  analyzed  the  samples,
This report describes the collaborative tests and  includes  statistical analyses
of the test results.
Approved for:

MIDWEST RESEARCH INSTITUTE
L. J./Shannon, Director
Environmental and Materials
  Sciences Division
 October  1978
                                     iii

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                                  ABSTRACT
     A two-part collaborative test was conducted for  Method 106,  "Determina-
tion of Vinyl Chloride from Stationary Sources." A group  of 10  collaborators
analyzed a set of synthetic samples,  some of which contained interferences,
for vinyl chloride. Analytical results were reported  by peak height  and by peak
area. All samples were analyzed on both 2m Chromosorb 102  and 2m  Chromosorb
102/2m SF-96 columns. Most of the collaborators  correctly  identified the vinyl
chloride peaks. Chromosorb 102/SF-96  performed better in  the presence of
acetaldehyde and Chromosorb 102 alone was better for  isobutane  interferences.
In all cases the chromatograms showed proper responses. The errors that were
made were due to interpretation of the results.  The skill  of the  analyst is
a major factor in the use of Method 106. The collaborators obtained  values
which averaged 0.18 ppm (0.47 mg/m^)  low with a  standard  deviation of 0.72 ppm
(1.86 mg/nH). There was no overall superiority noted  for  peak height versus
area. The bias found was entirely due to low results  using only Chromosorb 102.
Chromosorb 102/SF-96 gave a bias that was 0.01 ppm (0.03 mg/m^) low.

     A field test of the method was then conducted by three groups on the vent
from a carbon bed adsorber. The group of collaborators had a standard devia-
tion of 0.46 ppm (1.19 mg/nH) for sampling and analysis combined. The standard
deviation for sampling from the same  source was  0.39  ppm  (1.01  mg/nH) and 0.24
ppm (0.62 mg/m^) for the analysis of  the samples obtained. A brief comparison
of a charcoal adsorption tube method  gave results which were about 20% lower
than results obtained using Method 106.

     This report was submitted in fulfillment of Contract  No. 68-02-2737 by
Midwest Research Institute under the  sponsorship of the U.S. Environmental
Protection Agency. This report covers a period from June  1977 to  April 1978,
and work was completed as of May 1978.
                                     IV

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                                  CONTENTS
Foreword* •••••••••••••• 	  •••••   iii
Abstract* •••••••«•••••••••••••••  	    iv
Figures 	 ••••••••••••••••••••••••••••    vi
Tables	•••••••••	••••    vi
Acknowledgments •••••••••••••••••••••••••••••   vii

     1.  Introduction ••••••••••••••••••••••••••     1
     2.  Conclusions* ••••••••••••••••••••.•••••     3
     3*  Recommendations* ••••••••••••••••••••••••     4
     4*  Selection of Collaborators •••••••••••••••••••     5
     5.  Collaborative Test Design* •••••••••••••••••••     7
     6.  Laboratory Collaborative Test Results* •••••••••••••     9
     7.  Statistical Analysis - Laboratory Test •••••••••••••    13
     8.  Field Collaborative Test ••••••••••••••••••••    18
     9.  Field Test Statistical Results .	•	    26
              Standards Data. •••••••• 	  •••••••••    26
              Field Samples	    28

References. • ••••••••••»•••••••••»»••••••••    31
Appendices

     A.  Letter to Obtain Potential Collaborators  ............    32
     B.  Final Instructions to Collaborators. ..............    35
     C.  Method 106 - Determination of Vinyl Chloride from Stationary
           Sources with Amendments. ..............•••••    38
     D.  Letter to Collaborators.	    44
     E.  Tentative Procedure for Sampling and Analysis of  Vinyl
           Chloride Using Charcoal Adsorption Tubes  ...........    48

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                                   FIGURES

Number                                                                  Page

  1       Field test sampling manifold* • •••••	•  .     19


                                   TABLES

Number       -                                                           Page

  1       Collaborators* Vinyl Chloride Analysis  Results  (mg/m^),  •  .     10

  2       Collaborators' Vinyl Chloride Analysis  Results  (ppm)«  •  •  •     11

  3       AOV of Laboratory Data	     15

  4     .  Biases in the Laboratory Test •••••••••••••••     16

  5 .      Sampling Time for Sample Identification ••••••••••     20

  6       Analysis Sequences* ••••••••••••••••••••     20

  7       Vinyl Chloride Field Test Results  	     22

  8       Vinyl Chloride Field Test Results  ••••  	     23

  9       Charcoal Tube Sampling Results* ••••••••••••••     24

 10       Results of Standards Data Analysis.  ••••••••••••     27

 11       Data Analysis of Field Test ••	     29

C-l       Retention Indices for Possible Vinyl Chloride
            Interferences ••••••••••••••••••••••     43
                                     VI

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                               ACKNOWLEDGMENTS
     This work was conducted under the technical  direction  of Mr. Fred J.
Bergman, Program Manager, Method Development  Group  of Midwest Research Insti-
tute's Environmental and Materials Sciences Division. Dr. George Scheil was
Project Leader. He was assisted by Messrs. John LaShelle and Michael Sharp of
Midwest Research Institute. The assistance of the personnel of Diamond Sham-
rock Corporation during the field test is  gratefully acknowledged.
                                     vii

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                                  SECTION 1

                                INTRODUCTION
     On December 24, 1975, under Section 112 of the Clean Air Act,  as amended,
the Environmental Protection Agency (EPA) added vinyl chloride to the list  of
hazardous air pollutantsi' because it has been implicated as the causal  agent
of angiosarcoma and other serious disorders. A national emission standard has
been promulgated?.'  that covers plants that manufacture ethylene dichloride,
vinyl chloride, and polyvinyl chloride. These regulations include a method  for
determining vinyl chloride emissions from stationary sources, EPA Method 106.
The Quality Assurance Branch of the Environmental Monitoring and Support Labora-
tory at Research Triangle Park, North Carolina, has as its task the evaluation
and standardization of EPA source test methods. While participating in this
program, Midwest Research Institute (MRI) has undertaken a collaborative test
of EPA Method 106.

     The objective of this project was to conduct a collaborative test of EPA
Reference Method 106 (vinyl chloride). A collaborative test is a procedure  in
which a group of persons from different laboratories conduct sampling and
analysis under identical conditions using the same method. It provides infor-
mation on the variability of method results between laboratories as well as
the reproducibility of a single analyst's results. A properly designed col-
laborative test should demonstrate the reliability of the method being tested
under typical, realistic sampling and analysis conditions.

     The first goal under this program was to contact potential collaborators
and determine their experience in gas chromatographic analysis and vinyl chlo-
ride sampling techniques.

     Following the evaluation of potential collaborators, 10 participants were
selected for the collaborative tests. Each collaborator was supplied with six
samples for analysis. The samples consisted of a minimum of four levels  of
vinyl chloride with at least two samples containing organic compounds that
are potential interferences. The samples were obtained from a reputable  gas
supplier who ascertained that the samples were stable and of the correct con-
centration.

     MRI analyzed one set of samples at periodic intervals during the duration
of the collaborative test. MRI also sent one set of samples to the National
Bureau of Standards (NBS) for certification of the stated concentrations.

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     A source of vinyl chloride emission at or below 15  ppm (40 mg/nr)  was lo-
cated by MRI. Arrangements were made for three collaborators to obtain  repli-
cate and simultaneous samples from the selected source using Method 106. The
collected samples were analyzed within 24 hr after collection.  Samples  were
also collected using a charcoal tube absorption technique.

     At the conclusion of the laboratory and field collaborative test of Method
106, MRI statistically evaluated the analytical results.

     The following sections of this report include the results  and statistical
analyses of the collaborative tests. General conclusions and recommendations
obtained from the study are also presented.

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                                  SECTION 2

                                 CONCLUSIONS


     The major conclusions obtained from the collaborative  tests  are:

     !•  For vinyl chloride concentrations < 10 ppm (25  mg/m^), a collaborator
has a repeatability of + 0,5 ppm (1.3 mg/m^) or better,  but at 50 ppm  (125
mg/m^) vinyl chloride this value is much larger (~ + 6 ppm, 15 mg/m^).

     2.  A set of collaborators will read a given  low concentration vinyl
chloride sample to within approximately + 1.25  ppm (3 mg/nH)  (except at  50
ppm (125 mg/m^) vinyl chloride it becomes + 10  ppm, 25 mg/m^).

     3.  The physical sample-sample contribution to collaborator  variation  is
comparable to the analytical contribution.
                                                                    o
     4»  The biasses exhibited are on the order of -0.1  ppm (0.3  mg/nr)  for
pure vinyl chloride and -0.2 ppm (0.5 mg/m^) for interferred vinyl chloride,
when reliable readings are produced. However, one  (of 10) collaborator was
fooled by all interferences, and the set of collaborators failed  to produce
reliable observations 40% of the time on the 45.1  ppm (82 mg/rn^)  acetaldehyde
sample.

     5.  There is no distinction between height and area methods. The Chromo-
sorb 102/SF-96 measurements are unbiased, and therefore  are to be preferred,
statistically, to the negatively biased Chromosorb 102 measurements. The Chromo-
sorb 102 bias (~ -0.3 ppm, 0.8 mg/m3), is, however, small compared to the re-
peatibility contributions.

     6.  The charcoal adsorption tube allows a  much simplified sampling  pro-
cedure compared to Method 106 but the analysis  procedure is more  difficult
and not as accurate.

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                                  SECTION 3

                               RECOMMENDATIONS
     Based upon the conclusions that have been obtained from this collabora-
tive test, it is recommended that:

     1.  Method 106 continue to be used in its present form as an acceptable
method for the analysis of vinyl chloride from stationary sources.

     2.  Further consideration be given to determining the equivalence of
Method 106 and a charcoal adsorption tube method.

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                                  SECTION 4

                         SELECTION OF COLLABORATORS
     A letter, which is shown in Appendix A,  was sent  to  approximately  80
organizations to determine their interest and qualification  for  participating
in the collaborative test. Fifteen potentially qualified  collaborators  re-
sponded with bids. All 15 collaborators were  considered technically  acceptable.
The 10 firms submitting the lowest bids were  therefore selected. The collab-
orators are:

     Dr. Douglas S. Kendall
     Commercial Testing and Engineering Company
     14335 West 44th Avenue
     Golden, Colorado  80401
     Analyst:  Dr. Douglas S. Kendall

     Dr. Perry Lonnes
     Interpoll, Inc.
     1996 West County Road C
     St. Paul, Minnesota  55113
     Analyst:  Mr. Harilal Patel

     Dr. Joseph D. Banzer
     Diamond Shamrock Corporation
     T. R. Evans Research Center
     P.O. Box 348
     Painesville, Ohio  44077
     Analyst:  Dr. Joseph D. Banzer

     Dr. David C. Kennedy
     Ryckman, Edgerley, Tomlinson & Associates
     12161 Lackland Road
     St. Louis, Missouri  63141
     Analyst:  Dr. Carol Hammer

     Mr. Robert D. Soule, P.E.
     Clayton Environmental Consultants, Inc.
     25711 Southfield Road
     Southfield, Michigan  48075
     Analyst:  Mr. Kent Shoemaker

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Dr. Don L. Shull
Commonwealth Laboratory, Inc.
Chemists Building
2209 East Broad Street
Richmond, Virginia  23223
Analyst:  Mr. Dryden Reno

Dr. Don Adams
The Graduate School
Washington State University
Pullman, Washington  99164
Analyst:  Mr. Dave Harsch

Mr. Arthur Engelmen
CCA/Technology Division
Burlington Road
Bedford, Massachusetts  01730
Analyst:  Mr. Michael Oliverio

Dr. Gene Dennison
Envirotest Laboratories
103 East Prospect Street
Hopewell, New Jersey  08525
Analyst:  Mr. Robert Menichelli

Mr. Bernard J. DeWitt
PPG Industries, Inc.
P.O. Box 31
Barberton, Ohio  44203
Analyst:  Mr. James Hendershott

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                                  SECTION 5

                          COLLABORATIVE TEST DESIGN


     Six different gas mixtures were prepared by Scott  Specialty Gases  for the
laboratory collaborative test. Twelve sets of these  mixtures were then  made
using 200 liter capacity low pressure cylinders. One set was for stability
checks by MRI. One set was shipped to the NBS to obtain reference values  of
vinyl chloride assigned. Each collaborator would receive one of the remaining
10 sets.

     Each collaborator analyzed each sample according to the instructions
given in Appendix B using the current version of Method 106 with amendments
(Federal Register, Vol. 41, pp. 46569-46571, October 21, 1976;  amended  Vol.
42, pp. 29007-29009, June 7, 1977) given in Appendix C. Each collaborator re-
ported both peak height and peak area results for both  the  2m Chromosorb  102
column and for the 2m Chromosorb 102/2m SF-96 column combination. Thus, sys-
tematic differences in the methods were measurable.

     The approximate compositions of the samples were:

     1.  5 mg/nr (2 ppm) vinyl chloride

     2.  20 mg/nr (8 ppm) vinyl chloride

     3.  18 mg/m^ (7 ppm) vinyl chloride and 80 mg/m^ (50 ppm)  acetaldehyde

     4.  30 mg/m^ (12 ppm) vinyl chloride, 15 mg/m-*  (10 ppm) methanol,  and 50
mg/nr (20 ppm) isobutane

     5.  18 mg/nr (7 ppm) vinyl chloride, 7  mg/nr (5 ppm) methanol, and 25
mg/nr (10 ppm) isobutane

     6.  30 mg/nP (20 ppm) acetaldehyde

     All samples have nitrogen as the balance gas.

-------
     Samples 1 and 2 measure the accuracy of each collaborator's  calibration
gases. Sample 3 is a mixture which should be difficult  to  resolve on Chromo-
sorb 102, but easy on the combined columns. Samples  4 and  5  are  similar  and
should be easier to resolve on Ghromosorb 102.  Sample 6 contains  no vinyl
chloride and indicates the skill of the analyst's recognizing  a  false vinyl
chloride peak.

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                                  SECTION 6

                    LABORATORY COLLABORATIVE TEST RESULTS
     The samples were prepared, aged, and checked for vinyl  chloride stabil-
ity. They were then shipped to MRI, One set of cylinders was chosen at  random
and the first analysis of the samples was completed by MRI  on September 12.
After verifying that each mixture could be measured on at least one of  the
columns, the collaborators' samples were shipped. One set was also shipped  to
NBS.

     Tables 1 and 2 summarize the results of the test. The  tables include
analysis results by Scott, NBS, MRI, and the collaborators.  Collaborator D
did not submit results until 4 months after the samples were shipped. All
other collaborators completed their analyses within the 1-month period  al-
lowed. Since Collaborator D submitted results which demonstrated no obvious
anomalies, their results are included in the final data set. Vinyl chloride
in cylinders is normally stable for periods of more than 1  year without de-
tectable changes in concentration. The only component which  is unstable is
acetaldehyde and it was still clearly present in Collaborator D's chromato-
grams.

     Collaborators B and F found no acetaldehyde peaks in their samples. The
suspect cylinders were returned to MRI, Acetaldehyde was clearly detected in
all of the suspect samples by MRI, Neither collaborator has  been able to sug-
gest any reason for the loss of acetaldehyde on a Chromosorb 102 column.

     However, acetaldehyde is irreversibly retained by many  polar materials
in addition to an SF-96 column. In many instances the collaborators reported
suspect values which they rejected due to the probable presence of interfer-
ences. Collaborators E, G, and K did not indicate that Sample 10673 was not
vinyl chloride. An examination of these data by MRI indicates that the  dif-
ferences in retention time should have been sufficient to reject the peaks as
not vinyl chloride,

     MRI conducted two analyses of the samples 1 month apart. As the data in
Tables 1 and 2 indicates, the samples were all stable. Samples 60106 and 4786
were pure vinyl chloride. Both columns performed equally well. Samples  4036
and 6800 are similar. On Chromosorb 102, two peaks are seen  incompletely

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TABLE 1.  COLLABORATORS' VINYL CHLORIDE ANALYSIS RESULTS  (mg/m3)


1814 (17.6 Dg/ra3 vinyl chloride.
32 mg/a3 acctaldehyde)
Chromosorb 102 height
Chromosorb 102 area
Chromosorb 102 and SF-96 height
Chromosorb 102 and SF-96 area
4036 (33.7 mg/ra3 vinyl chloride.
9*4 mg/a3 root Hanoi, 51 tag/m3
isobulane)
Chroaosorb 102 height
Chroaosorb 102 area
Chroaosorb 102 and SF-96 height
Chroaosorb 102 and SF-96 area
6800 (18.2 ag/n3 vinyl chloride.
6*0 ng/o3 net Hanoi, 25.5 rag/ia3
Isobutane)
Chromosorb 102 height
Chroaosorb 102 area
Chrooosorb 102 and SF-96 height
Chrooosorb 102 and SF-96 area
10673 (34 og/m3 acctaldehyde)
Chroaosorb 102 height
Chroaosorb 102 area
Chromosorb 102 and SF-96 height
Chroaosorb 102 and SF-96 area
47JJ6 (22.6 mg/a3 vinyl chloride)
Chromosorb 102 height
Chromosorb 102 area
Chromosorb 102 and SF-96 height
Chromosorb 102 and SF-96 area
60106 (5.80 rag/m3 vinyl chloride)
Chromosorb 102 height
Chromosorb 102 area
Chroaosorb 102 and SF-96 height
Chromosorb 102 and SF-96 area
£/ Data received late .
b/ Data corrected for revised and
~

NBS Collaborator
(mn/r)3) A

17.5
19.frc7
17.2
Not raeii-
33.7


23.7
28.2
32.9
32.9
19.0


16.4
16.1
18.9
id. 7
< 0.13
12i£'
n.d.
n.d.
22.2
19.1
18.8
23.2
22.6
5.81
4.84
4.71
5.39
5.05
lyavs In vinyl chloride


Collaborator
fib/

12.4
12.4
15.3
15.8



24.9
24.9
30.0
31.6



15.3
15.5
16.8
17.6
n.d.
n.d.
n.d.
n.d.

16 3
17.1
19.7
19.9

3.9
4.1
4. 7
6.0
standards as


Collaborate
C

43. B£'
48.4~
18.6
17.9



35.5
36.0
34.7
35.0



19.7
21.8
20.7
19.7
10.U'
11. IS'
n.d.
n.d.

23.3
23.8
23.8
23.1

6.0
7.5
6.7
6.2
reported by


r Collaborator
rv/

f,
31.78£'
15.4
18.0



34.45
34.91
34.60
34.40



19.40
19.45
19.45
19.32
n.d.
n.d.
n.d.
n.d.

21.9
23.5
22.7
22.9

5.62
6.01
6.11
5.80
supplier.


Collaborator
E

28.0='
42. 2£'
14.2
39.95'



32.4
31.1
33. 4£'
34.2°.'



20.5
20.5
19. 9£/
22. 3£'
19.7
19.4
7.3S/
22. 3£'

22.5
22.0
23.8
23.1

6.0
5.7
6.2
7.0



Collaborator
r

15.3
15.3
14.5
16.1



31.6
30.3
31.3
30.0



17.6
16.8
16.8
16.8
n.d.
n.d.
n.d.
n.d.

20.2
20.2
19.4
20.5

6.5
4.7
5.4
4.9



Collaborator
C

50.71
52.783'
17.4
17.2



33.18
33.633'
34.34
34.34



18.9
18.93'
18.3
18.4
12.2
I3.0d/
n.d.
n.d.

21.7
21.83'
22.7
22.4

5.62
5.783'
6.40
6.48



Collaborator
H

37.B":'
72. OS.'
18.4
18.2



34.58
33.33
34.24
32.9



20.0
19.7
19.7
18.9
3.57£/
6.92?.'
n.d.
n.d.

22.9
22.9
22.9
23.0

7.23
6.89
7.23
6.89



Col laborator
J

24. (£.1
48. IS'
15.8
15.5



33.4
33.4
29. -£/
28. ?£'



18.6
18.4
19.4
19.2
n.d.
n.d.
n.d.
n.d.

21.0
21.0
19.7°'
19. IS.'

5.7
5.4
5.7
5.1



Collaborator
K

16.8
16.1
20.7
20.2



119
1SS
106
ISO



60
83
80
78
1.3
1.3
n.d.
n.d.

22.3
21.8
24.9
25.4

6.2
6.2
6.5
7.3



MRI
Sept. 12

20. 5
35.5
16.3
16.63'



28.2
30.33'
36. 5
cy



16.6
17.63'
20.5
.£.'

Oct. 13

9.1
C/
16.6
17.13'



31.1
32.43'
= '
o./



17.4
17.6
e/
e/
Wrong retention time-
not vinyl
n.d.
n.d.

20.2
19. 13'
20.5
20.53'

5.08
5.3*3'
5.46
5.3l3'



chloride
n.d.
n.d.

20.7
20.73'
20.7
21.23'

5.31
5.313'
5.49
5.543'




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                           TABLE  2.    COLLABORATORS'  VINYL  CHLORIDE ANALYSIS  RESULTS   (PPM)

1816 (6.8 ppra vinyl chlorine,
65.1 ppm acctaldchydc)
Chromosorb 102 height
Chromosorb 102 area
Chromosorb 102 and 5F-96 height
Chromosorb 102 and SF-96 area

6036 (13.0 ppm vinyl chloride.
7.1 ppm octhanol, 21.1 ppm
isobutanc )
Chromosorb 102 height
Chramosorb 102 area
Chromosorb 102 and SF-96 height
Chroraosorb 102 and SF-96 area
6800 (7.06 ppra vin)l chloride,
6.5 ppo mcthanol, 10.6 ppo
Isobutanc)
Chromosorb 102 height
Chroraosorb 102 area
Chromosorb 102 and SF-96 height
Chromosorb 102 and SF-96 area
10673 (18.6 ppm acctaldchydc)
Chromosorb 102 height
Chromosorb 102 area
Chromosorb 102 and SF-96 height
Chromosorb 102 and SF-96 area
6786 (8.73 ppm vinyl chloride)
Chromosorb 102 height
Chromosorb 102 area
Chromosorb 102 and SF-96 height
Chromosorb 102 and SF-96 area
60106 (2.26 ppm vinyl chloride)
Chromosorb 102 height
Chromosorb 102 area
Chromosorb 102 and SF-96 height
Chromosorb 102 and SF-96 area
NBS Collaborator
(ppm) A
6.75

2 .!£'
75 7 .6°'
.66
H t raco-
s rablc£'
13.0


11.1
10.9
12.7
12.7
7.34


6.36
6.21
7.30
7.22
<0.05
I3.5S'
67. t£'
n.d.
n.d.
8.57
7.38
7.27
8.96
8.73
2.26
1.87
1.82
2.08
1.95
Col laborator


6.8
4.8
5.9
6.1




9.6
9.6
11.6
12.2



5.9
6.0
6.5
6.8

n.d.
n.d.
n.d.
n.d.

6.3
6.6
7.6
7.7

1.5
1.6
1.3
2.1
Col laborator
C


16. 9J;'
18. 7£/
7.2
6.9




13.7
13.9
13.4
13.5



7.6
8.6
8.0
7.6

3.9£'
4. IS'
n.d.
n.d.

9.0
9.2
9.2
8.9

2.3
2.9
2.6
2.6
Col laborator
Da'


c/
12.271'
5.94
6.95




13.30
13.48
13.36
13.28



7.49 '
7.51
7.51
7.66

n.d.
n.d.
n.d.
n.d.

8.47
9.06
8.77
8.85

2.17
2.32
2.36
2.24
Col laborator
E


10. a£'
16.3*'
5.5
15.4S'




12.5
12.0
12.91'
13. 2£'



7.9
7.9
7.7£'
8 65.'

7.6
7.5
2.8£'
B.6S'

8.7
8.5
9.2
8.9

2.3
2.2
2.4
2.7
Col laborator
F


5.9
5.9
5.6
6.2




12.2
11.7
12.1
11.6



6.8
6.5
6.5
6.5

n.d.
n.d.
n.d.
n.d.

7.8
7.8
7.5
7.9

2.5
1.8
2.1
1.9
Collaborator
C


19.58
20. 384'
6.71
6.66




12.81
12.833'
13.26
13.26



7.29
7.284'
7.08
7.12

4.72
5.024'
n.d.
n.d.

8.37
8.624'
8.77
8.66

2.17
2.234'
2.47
2.50
Collaborator
fl


16.61'
27.8='
7.11
7.04




13.35
12.87
13.22
12.7



7.71
7.62
7.60
7.30

1.38°'
2.671'
n.d.
n.d.

8.86
8.84
8.85
8.87

2.79
2.66
2.79
2.66
Collaborator
J


9. 5l'
18. 6='
6.1
6.0




12.9
12.9
11. IS'
ll.lc/



7.2
7.1
7.5
7.4

n.d.
n.d.
n.d.
n.d.

8.1
8.1
7.6='
7.5£'

2.2
2.1
2^2
2.1
Col laborator
K


6.5
6.2
8.0
7.8




46
60
41
58



23
32
31
30

0.5
0.5
n.d.
n.d.

8.6
8.6
9.6
9.8

2.6
2.4
2.5
2.8
MK1
Scot. 12


7.9
13.7
6.3
6.44'




10.9
11.74'
14.1
£'



6.4
6.84'
7.9
a/

Wrong ret
not vinyl
n.d.
n.d.

7.84'
7.64'
7.9
7.94'

1.96
2.08
2.11
2.054'
Oct. 13


3.5
c./
674
6.64'




12.0
12.54'
±1
£.'



6.7
6.8
S.I


intion tirac-
chloride
n.d.
n.d.

8.0
8.04'
8.0
8.24'

2.05
2.054'
2.12
2.164'
a/  Data received late





bl  Data corrected for rovlscd jnolyscs In vinyl chloride standards as reported by supplier.





£/  Instruacn: malfunction; not ablt to obtain reading.





d/  Best value.





e/  lnt*r[cr^nco s-jsptcti.-d--r«sul C rejected by CO 11 aborator.

-------
separated but sufficient to accurately measure both height and area. On the
combined columns, vinyl chloride becomes a slight shoulder on the leading edge
of the interference peak. The peak height can be estimated but no information
on peak area is obtainable without complex peak shape analyses. Apparently,
the methanol peak has shifted and merged with the isobutane peak. Sample
10673, acetaldehyde only, shows normal peak shape but with a retention time
of about 0.3 min shifted on Ghromosorb 102. On the combined columns no peaks
are detectable indicating permanent retention of acetaldehyde by the SF-96
column. Sample 1814, vinyl chloride and acetaldehyde, shows a single peak with
nearly double normal peak width on Chromosorb 102. On the combined columns
only a single normal peak is present at the vinyl chloride retention time. The
values measured by MRI are slightly lower than those reported by Scott, but
may be due to small errors in the last comparison against permeation tube
standards*
                                     12

-------
                                   SECTION 7

                   STATISTICAL ANALYSIS - LABORATORY TEST
     Structurally, this data set is.a 6 (levels of vinyl chloride (VC))  x 10
(collaborators) x 4 (methods) factorial analysis of variance (AOV). The  pri-
mary objective of the analysis is to estimate the components of variance,
namely:

     Oe  = The variance of repeated measurements by a single collaborator at
           a fixed level of VC.
       *\
     cr^  = The variance of VC measurements between collaborators (over and
           above that which would arise due strictly to ae )•

     0^2 = xhe variance of VC measurements due to method-method differences.*

     CTL? = The variance due to level-level differences.

    acm2 = The variance due to differences in the collaborator differences due
           to method changes, etc.

     These components "add," e.g., the variance of repeated measurements by
a group of collaborators measuring a value of VC by a method is ae2 + ac2,
etc.

     In practice, the number of levels actually analyzed was only four because:
(a) one level was a "control" level - zero VC and 18.4 ppm acetaldehyde—this
level did not "fool" nine of the collaborators in any instance, although Col-
laborator E did report ~ 7.5 ppm by Methods 1 and 2;  (b) the level consisting
of 6.8 VC + 45.1 ppm acetaldehyde produced unreliable measurements 40% (16/40)
of the time. It is felt that this result is more realistic than a formal numeri-
cal analysis of the values (the other 60% of which were reasonably close to
the nominal value).

''•  Technically, "aL.2" and "o^ " are not variances, because the methods and
     levels are fixed (not randomly selected from a population of methods or
     levels). For convenience, however, the en notation will be used.
                                      13

-------
     One collaborator (K) produced obviously discrepant values* at both of the
other interfered levels. Therefore, only nine collaborators were incorporated
in the primary analysis of variance. Of course, it should be kept in mind dur-
ing all overall considerations of the method that one (of 10) collaborators
did produce unacceptably large errors.

     Finally, in the remaining 4x4x9= 144 cells, eight values were "miss-
ing." These eight were all produced by two collaborators (Collaborators J and
E), and were all confined to the two SF-96 methods. The missing values were
replaced by a conventional procedure, i.e., by minimizing residual SS within
the VC level they fell in.

     The analysis of variance results is shown in Table 3.  The response (X)
is an individual bias, i.e., X = actual reading - NBS reference value.

     The results can be summarized as:

     *  A single collaborator reads a fixed level of VC with a single method
        within about +0.5 ppm** (+ 2 ae).

     *  A set of collaborators reads a fixed level of VC with a given method
        within about + 1.26 ppm (+ 2 ^CTg2 + ac2).

     *  The method effect is quite small, e.g., the so-called "component
        at variance" + 2 ^cre2 + ac2 + a^2 = + 1.30 ppm.

     *  A set of collaborators reads the various levels of VC in the experi-
        ment to within about + 1.31 ppm (+ 2 \KTe2 + ac2 +
     Of course, in addition to the dispersion of the measurements the accuracy
can also be evaluated with respect to the NBS values.*** Various biases of
interest are shown in Table 4. In terms of significance:
*    Collaborator K's results for 13.0 ppm VC + 7.1 ppm methanol + 21.1 ppm
       isobutane were ~ "50 ppm," and for 7.34 ppm VC + 4.5 ppm methanol +
       10.6 ppm isobutane were ~ "30 ppm." Both of these results are,  of course,
       rejectable or outliers (Dixon-Massey R - 0.931, p < 0.005 and r = 0.942,
       p < 0.005).
**   This quantity, however, is never directly observed in the experiment.
***  The various biases across levels could be "integrated" via an analysis
       of covariance with NBS values, a covariate with respect to collaborator
       values. With only four levels, however, the "piecewise" approach em-
       ployed is felt to be adequate.

                                     14

-------
                     TABLE 3.  AOV OF LABORATORY  DATA

Source
Collaborator (C)
Level (L)
Method W)
CL
CM
LM
e
aF
8
3
3
24
24
9
64
SS
43.98
2.88
3.98
11.21
10.15
1.44
3.86
MS
5.50
0.96
1.33
0.47
0.43
0.16
0.0603
F
91.2ia/
2.04
3.09k/
7.135./
2.65k/

   EMS (C) = o-2 + 16 o>2                     CTe2 = 0.0603
              C        *—                        ^




   EMS (L) = o-e2 + 4 aCL2 + 36 aL2            ac2 = 0.3400





   EMS (M) = ae2 + 4 aCL2                     CTL2 = 0.0136





  EMS (CL) = ae2 + 4 0-QM2 + 36 a^2            crM2 = 0.0250





  EMS (CM) = C7e2 + 4 o-cM2                    aCL2 = 0.1024





  EMS (LM) = ae2 + aCLM2 + 9 ^LM2            CTCM2 = °'0924





 EMS (CLM) = ae2 + crcLM2                     °"LM2 = 0.0111





   EMS (e) = ae2












a/  Significant at p = 0.01.





b/  Significant at p = 0.05.
                                    15

-------
                  TABLE 4.  BIASES IN THE LABORATORY TEST

Source (ppm)
LI (2.26 VC)
L2 (8.57 VC)
L3 (13.0 VC +7.1 methanol + 21.1 isobutane)
L4 (7.34 VC +4.5 methanol + 10.6 isobutane)
Ml Chromosorb 102 height
M2 Chromosorb 102 area
M3 Chromosorb 102 and SF-96 height
M4 Chromosorb 102 and SF-96 area
Coll. D
Coll. H
Coll. J
Coll. C
Coll. G
Coll. A
Coll. B
Coll. F
Coll. E
Avg. bias (ppm)
-0.012
-0.219
-0.386
-0.083
-0.339
-0.344
+0.014
-0.036
+0.200
+0.263
-0.044
+0.500
-0.019
-0.600
-1.325
-0.725
+0.163
Bias (%)
-0.53
-2.56
-2.97
-1.13
-4.35
-4.42
+0.18
-0.46
+2.57
+3.37
-0.56
+6.42
-0.24
-7.70
-17.01
-9.31
+2.09
All data
-0.176
-2.26
                                     16

-------
"  The bias at all levels was  negative  (-0,18  ppm overall average), but
   Ll and L4 were the closest  to true,  while L2 was significantly more
   negative, and L3 significantly the most negative* Since Ll and L2 are
   the pure levels, it is not  clear that  the interferences cause an in-
   crease in bias*

*  The two Ghromosorb methods  (Ml and M2) are  significantly more biased
   than the two Ghromosorb + SF-96 methods (-0,34 ppm versus -0.01 ppm).
   In fact, Methods 3 and 4 are not biased at  all. There is no discernible
   difference between height and area determinations (in either case).
                                 17

-------
                                  SECTION 8

                          FIELD COLLABORATIVE TEST
     The final part of this program was to conduct a test of Method 106 on an
actual vinyl chloride source*

     A field test was arranged for February 14 through 16 at the Deer Park
plant of Diamond Shamrock. Three teams participated in the test. Diamond Sham-
rock and MRI were teams, and the third team was selected by MRI from the col-
laborators on the basis of cost.

     The sampling was done at ground level from the outlet of a carbon adsorp-
tion system. The manifold was connected around a control valve so that a posi-
tive flow could be maintained through the manifold. A diagram of the sampling
system is shown in Figure 1. Since the line was at a moderate positive pressure,
the pumps were not used during sampling. A needle valve was inserted to con-
trol the flow into the bags with flow rates still measured by the air leaving
the bag enclosure. The expected vinyl chloride concentration was slightly
under 1 ppm.

     A copy of the letter sent to the collaborators requesting bids for the
test is shown in Appendix D. The field test design is given in Tables 5  and 6.
The three teams analyzed each others'  standards to determine the variability
of the different manufacturers' standards. Each team also analyzed some  of the
other teams* samples to measure precision.

     MRI also sampled using carbon adsorption tubes. The adsorption tube
procedure followed a modified form of  the EPA ambient vinyl chloride method
as given in Appendix E. This procedure was compared with the Method 106  re-
sults. The method was modified to simplify the calibration procedure and im-
prove the reliability of the method by making the calibration and analysis
procedures similar.

     The third collaborator selected was Envirotest Laboratories. The person-
nel who participated in the test were:
                                     18

-------
                                   Pressure
                                   Regulator
Sampling
Valve
                                                                         To Vcnl
                                                                         Stack
                •=1 .Shutoff  Valve       »=r, Shutoff Valve      t=<  Shutoff Valve
                                                 Sampling
                                           >T[1   Valve
                                           inn)
Sampling
Valve
              Figure  1.   Field  test  sampling manifold.

-------
              TABLE 5.  SAMPLING TIME FOR SAMPLE IDENTIFICATION
Collaborator A
Collaborator B
Collaborator C
Day 1 Day 2
I II III IV I II III IV
Al A2 A3 A4 A5 Ae A7 AS
Bl B2 B3 B4 B5 B6 B7 B8
cl C2 C3 CA C5 C6 C7 C8
TABLE 6. ANALYSIS SEQUENCES
Day 1
Collaborator A
Collaborator B
Collaborator C
Day 2
Collaborator A
Collaborator B
Collaborator C
a/
SA- AI Ci A2 B2 A3 C3 A4 B4 SA
SB BI AI B2 C2 63 A3 B4 C4 SB
SQ C]^ B^ C2 A2 03 63 C4 A4 Sg
SC A5 B5 Ae Be A7 C7 AS BS SC
SA 65 GS Be ce B7 A7 BS cs SA
SB C5 A5 C6 A6 C7 B7 C8 A8 SB
a/  SA = Standard gas set belonging to A.

All standards are analyzed by all collaborators twice.
All samples are analyzed by two collaborators.
Each collaborator analyzes all of his samples and one-half of every other col-
  laborators ' .
                                     20

-------
        Envirotest Laboratories
        Mr. Robert Menichelli - analyst
        Dr. Gene Dennison - sampler

        Diamond Shamrock
        Dr. Joseph Banzer - analyst
        Mr. Don Myers - sampler

     *  Midwest Research Institute
        Dr. George Scheil - analyst
        Mr. John LaShelle - sampler

     The field test of Method 106 was completed February 14 through 16,  1978,
at the Deer Park plant of Diamond Shamrock. On February 14 equipment was set
up and checked by the three teams.

     The results of the test are summarized in Tables 7 and 8.  On  the morn-
ing of February 15 a fresh carbon bed was put on line and sampling started for
run No. 1 at 0940. Run No. 2 sampled the same carbon bed. The  second carbon
bed was started prior to run No. 3. Run No. 4 was also made on  the second bed.
The first three runs proceeded normally with each team analyzing their own
bag and one other team's bag during each run. Run No. 4 showed  very high vinyl
chloride levels caused by intermittent bursts of steam entering the bed  which
desorbed vinyl chloride. The three bag samples show wide variations in concen-
tration. The variations were probably due to the fact that (according to the
plant on-stream analyzer) one of the two steam brusts occurred  at  the start
of sampling when flow rates into the bags were unstable.

     During the first test day each collaborator analyzed the  other team's
standards. Due to the size of one collaborator's standard cylinders it was not
feasible to carry them from place to place. Instead, aluminized Mylar bags
were filled from each cylinder and analyzed by each collaborator.  Thus,  one
collaborator has different values for peak height and area for  their own stan-
dards instead of the calibrated values.

     On February 16 run Nos. 5 and 6 were made on the first bed after over-
night bed regeneration. Run No. 7 started on a fresh second bed but was  immed-
iately stopped after another burst of steam. The bags were flushed, pumped
down, and checked for contamination. Run No. 7 was then restarted  with no fur-
ther difficulty. No further runs were made since delays from the upsets  left
no additional time in the test schedule without incurring unscheduled costs.

     MRI also ran three charcoal tubes using the tentative procedure which op-
pears in Appendix E. The results of this comparison are given  in Table 9.
                                     21

-------
                                     TABLE  7.    VINYL  CHLORIDE  FIELD  TEST RESULTS"
                                                                                                     a/
Date
Time
Feb. 15
0940-1040
Feb. 15
1052-1152
Feb. 15
1404-1504
Feb. 15
1618-1718
Feb. 16
0943-1043
Feb. 16
1108-1208
Feb. 16
1458-1558

Feb. 15
Feb. 15
Feb. 15
Col laborator
Coll. A
analysis
Run 1 Ht
Area
Run 2 Ht
Area
Run 3 Ht
Area
Run 4 Ht
Area
Run 5 Ht
Area
Run 6 Ht
Area
Run 7 Ht
Area
Nominal level
5 ppm standard Ht
Area
10 ppm standard Ht
Area
50 ppm standard Ht
Area
2.72
2.47
1.55
1.46
1.05
0.97
63.7
7313
4.34
4.42
1.89
1.76
8.14
8.02

4.52>!/
4.6l£V
9.42^/
46.lt/
45.4k/
A Samples/stj
Coll. B
analysis


1.73
1.64


82.0
82.7
4.64
4.46





5.28
5.05
10.7
10.2
51.6
49.6
mdards
Coll. C
analysis
2.79
3.03


1.20
1.34




1.92
1.86
7.02
7.18

4.43
4.62
8.86
8.56
39.8
38.3
Collaborator
Coll. B
analysis
2.12
2.01
1.65
1.60
1.04
1.03
1,037
998
4.82
4.55
2.23
2.13
7.20
7.17

l'.&>
10. fff
10. &£/
49. Q£/
49. 0£/
B Samples/standards
Coll. A Coll. C
analysis analysis.
1.97
1.82


0.84
0.79




2.31
2.29
6.87
6.93

d/
5.0
I/
10.3
47.3


1.51
1.64


898
897
4.36
4.42





4.55
4.58
9.54
9.51
42.4
42.4
Col labor
Coll. C
ana lysis
1.87
2.02
1.52
1.68
0.90
1.03
1,280
1,280
3.85
3.86
1.93
1.88
5.74
5.78

4.79£/
4.79£/
9.07£/
9.07S/
41. 7£/
41. 7£/
itor C Samples/standards
Coll. A Coll. B
analysis analysis
2.14
2.05
1.47
1.44
1.15
1.09
1,207
1,362
3.71
3.75
1.99
1.89
6.26
6.17

Al 5 . 25
4.86 5.26
d/ 10.1
9.82 10.1
d/ 48.3
48.4 47.2
a/ All results arc reported as parts per million of vinyl chloride.





b_/ Manufacturer's measured value.




£/ Manufacturer's certified value.




d/ Collaborator A had instrument problems and height analysis
                                                            obtainable.

-------
                                      TABLE  8.    VINYL  CHLORIDE  FIELD  TEST  RESULTS-
                                                                                                      a/
Date
Time
Feb. 15
0940-1040
Feb. 15
1052-1152
Feb. 15
1404-1504
Feb. 15
1618-1718
Feb. 16
0943-1043
Feb. 16
1108-1208
Feb. 16
1458-1558
Feb. 15
Feb. 15
Feb. 15
Col labora tor
Coll. A
analys is
Run 1 Ht
Area
Run 2 Ht
Area
Run 3 Ht
Area
Run 4 Ht
Area
Run 5 Ht
Area
Run 6 Ht
Area
Run 7 Ht
Area
Nominal level
12 ing/ra^ standard Ht
Area
25 rog/nP standard Ht
Area
120 mg/rn-* standard. He
Arco
7.04
6.40
4.01
3.78
2.72
2.51
165
190
11.2
11.4
4.90
4.56
21.1
20.8
1 1 . 7^'
11.9V
24^'
119*'
A Sample.
Coll. B
analys is

4.48
4.25

212
214
12.0
11.6


13.7
13.1
27.7
26.4
134
128
/standards
Coll. C
ana lysis
7.23
7.85

3.11
3.47


4.97
4.82
18.2
18.6
11.5
12.0
22.9
22.2
103
99
Collaborator
Coll. B
ana lysis
5.49
5.21
4.27
4.14
2.69
2.67
2686
2585
12.5
11.8
5.78
5.52
18.6
18.6
13. 5£'
13. 5£/
27. 5£/
27. 5£'
127£/
B Samples/standards
Coll. A Coll. C
analysis analysis
5.10
4.71

2.18
2.05


5.98
5.93
17. B
17.9
T3.0
26.7
723

3.91
4.25

2326
2323
11.3
11.4


11.8
11.9
24.7
24.6
110
109
Col laborator
Coll. C
ana lysis
4.84
5.23
3.94
4.35
2.33
2.67
3315
33'.5
9.97
10.0
5.00
6.87
14.9
15.0
12.4S/
12. 4£/
23. 5£'
23. 5£/
!$
C Samples/standards
Coll. A Coll. B
analysis analysis

3.81
3.73

3126
3528
9.61
9.71


12.6
25.4
d/
125
5.54
5.31

2.98
2.82


5.15
4.90
16.2
16.0
13.6
13.6
26.2
26.2
125
122
a_l All results a re reported as rcL 11 Igratns per cubic rooter of viny I ch lor id e .





b/ Manufacturer's measured value.





c_/ Manufacturer's certified value.





d/ Collaborator A had instrument problems and height analys LS was not obta inab le.

-------
                             TABLE 9.  CHARCOAL TUBE SAMPLING RESULTS
                      Charcoal tube analysis—'
                                            a/
            2 m SF-96 at 75°C
                       2  m Carbowax 1500 on
                         Carbopak at 75°C
                        Analysis of bag used for charcoal sampling
Run 3
Run 6
Run 7
  0.75 ppm
 (1.94 mg/m3)

  1.75 ppm
 (4.53 mg/m3)

  4.85 ppm
(12.6 mg/m3)
  0.68  ppm
 (1.76  mg/m3)

  1.55  ppm
 (4.01  mg/m3)

  4.88  ppm
(12.6 mg/m3)
  0.90 ppm peak ht.
 (2.33 mg/m3)

  1.93 ppm peak ht.
 (5.00 mg/m3)

  5.74 ppm peak ht.
(14.9 mg/m3)
  1.03 ppm peak area
 (2.67 mg/m3)

  1.88 ppm peak area
 (4.87 mg/m3)

  5.78 ppm peak area
(15.0 mg/m3)
a/  Charcoal tube results were by peak height only.

-------
Each charcoal tube sampled from one of the MRI  integrated bag  samples  after
the Method 106 analyses were completed. The original  intent  of this  sampling
was to use the same Chromosorb 102 column for the  charcoal method  analysis.
The characteristic doublet impurity peak from carbon  disulfide completely
obscures the vinyl chloride peak on Chromosorb  102. The  first  0,2% Carbowax
1500 on Carbopak column prepared was unusable due  to  crushing  of the fragile
Carbopak. An attempt to use a Carbowax 400 column  (which has McReynolds  con-
stants similar to Carbowax 1500) failed when no vinyl chloride peak  could be
identified. Finally, the SF-96 secondary column used  in  Method 106 did achieve
a separation of vinyl chloride from the carbon  disulfide doublet.  However,  this
nonpolar column results in such a short retention  time for vinyl chloride that
peak area was immeasurable and peak height was  unstable  with 20 to 30% varia-
tion in successive injections. The values reported are the averages  for  dupli-
cate injections, using peak height. The agreement  is  still quite acceptable
between Method 106 and the charcoal tube procedure using the SF-96 column. The
carbon disulfide extracts were saved and the results  obtained  on a new
Carbowax 1500/Carbopak column are also given in Table 9. The Carbowax  column
gave more consistent results although the vinyl chloride retention time  is
still short.
                                     25

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                                  SECTION 9

                       FIELD TEST STATISTICAL RESULTS
STANDARDS DATA

     In this data set three standards (5, 10, and 50 ppm) were read by three
collaborators in the following way:  three physical samples (one per collabo-
rator) were taken, and each bag was read by two collaborators. This plan was
executed in duplicate according to two methods (Ml = height, M2 = area)*

     Structurally each method consists of three (one per level) balanced in-
complete block (BIB) analysis of variance models.

     In practice, one-third of the height measurements were missing, so the
formal AOV was performed only for the area method. The height method was sep-
arately compared via regression analysis for the 15 cases in which a height
value existed.

     Finally, casual inspection of the results shows that the magnitude of the
components of variance will vary according to the level. For this reason re-
sults are quoted separately per level (see Table 10). These results are preci-
sions only, i.e., no bias is included.

     Results are:

     1.  A single collaborator reading a given standard will read within about
+ 0.32 ppm (at VC = 5 ppm), + 0.47 ppm (at VC = 10 ppm, and +6.0 ppm (at VC
= 50 ppm).

     2.  A set of collaborators will read a given standard within about + 0.59
ppm (at Ll), + 1.50 ppm (at L2), and + 10.2 ppm (at L3).

     3.  A set of collaborators will read a set of standards within about +
0.80 ppm (at Ll), + 1.92 ppm (L2), and + 12.9 ppm (at L3).

     4.  Roughly speaking, the standard-standard variation is about the same
size as the collaborator-collaborator variation.
                                     26

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                TABLE  10.  RESULTS  OF  STANDARDS  DATA ANALYSIS
A.   Analyses of Variance  (area  method)

Level 1 (5 ppm)

      Source              df          SS            MS                  EMS
Collaborator (adj)
Sample (s)
Error (e)
Level 2 (10 ppm)
Collaborator (adj)
Sample (s)
Error (e)
Level 3 (50 ppm)
Collaborator (adj)
Sample (s)
Error (e)
B. Components of Variance
2
2
1

2
2
1

2
2
1

0.2353
0.5785
0.0253

1.6419
2.5375
0.0541

68.44
114.64
9.13

0.
0.
0.

0.
1.
0.

34
57
9.

1177
2916
0253

8210
2688
0541

.22
.32
13

ae2 + 3/2 ac2
22 ?
ae + ac +2 CTS^
CTe2

ae2 + 3/2 crc2
o'e + o~c + 2 o~g
CTe2

cre2 + 3/2 ac2
tfe2 + crc2 + 2 as2
-e2

LI:  ae2 = 0.0253
     crc2 = 0.0616
     CTS2 = 0.0743
L2:  ae2 = 0.0541
     CTC2 = 0.5113
     o-s2 = 0.3517

L3:  o-e2 = 9.13
     ac2 = 16.73
     as2 = 15.73
                                      27

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     5.  The 5 and 10 ppm results are more or less compatible with the lab-
oratory data; the uncertainties associated with 50 ppm VC are considerably
larger (even relatively). It was concluded that the 5, 10, and 50 ppm levels
were nominal only, so that quantitative biases were not evaluated.

     The comparison of height versus area methods was undertaken via regres-
sion analysis of the 15 pairs of such measurements. Results were

     Ht = -0.15 + 1.03 (Area), r = 0.9998, Se = 2.47.

     In this equation the slope is not distinguishable from 1, and the inter-
cept is indistinguishable from zero. Also a t-test of the sample differences
is insignificant (t = 0.60). Therefore it again appears that there is no worth-
while difference between the two methods.

FIELD SAMPLES

     This data set is organized on the same basis as the standards data, ex-
cept that seven runs (instead of three levels) were executed.

     However, on run 4 an anomalous steam burst caused preposterous readings
on Samples 2 and 3, so the AOV was restricted to runs 1, 2, 3, 5, 6, and 7.
In these data, of course, there are no reference values, so variabilities are
the only quantities produced from the analysis. Also, run-run variability was
considered a nuisance (the block in a balanced incomplete block design) so
that quantification of "oR2" was not performed.

     The 12 balanced incomplete blocks were analyzed individually (Table 11),
resulting in aggregate estimates of crc2, as2, and aQ2. The six runs varied
(evidently) in VC concentration from about 1 to 8 ppm. The components of var-
iance are significantly larger on R7 than on the otner tive runs.

     A regression analysis of results by method (Ml = 0.03 + 1.00 M2, r =
0.998, and Se = 0.120) again fails to indicate any significant difference be-
tween them. The other components of variance indicate:

     1.  A single collaborator reads a single sample to within about + 0.33
ppm.

     2.  A set of collaborators read a given sample to within + 0.7 ppm.

     3»  A set of collaborators read a set of samples (taken "simultaneously")
to within about + 0.91 ppm.

     4.  Sampling variability contributes about + 0.58 ppm to the method's
error limits.
                                     28

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                    TABLE 11.  DATA ANALYSIS OF FIELD TEST
	 2
Run 1 (VC = 2.25) CTQ =
a!2 =
CTC2 =
s
	 2
Run 2 (VC =1.57) ag =
ac2 =
CTs =
Run 3 (VC = 1.04) ae2 =
a =
c2
CT =
S
2
Run 5 (VC = 4.27) ae =
CT =
C2
CT =
S
2
Run 6 (VC = 2.01) a
a62 =
Co
£.
a =
s
o
Run 7 (VC = 6.87) ag =
CT 2 =
CTs =
All Runs (VC = 3.00) 
-------
     Although qualitatively comparable,  it can be seen  that  the  field  results
are somewhat more precise than the laboratory data (+ 0,91 ppm versus  +  1.26
ppm). This is because the three collaborators used in the field  test are much
more alike than the 10 collaborators used in the first  test.
                                     30

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                                 REFERENCES







1.  Federal Register 40:59477,  December  24, 1975,





2.  Federal Register 41:46564-46573, October 21, 1976.
                                      31

-------
               APPENDIX A
LETTER TO OBTAIN POTENTIAL COLLABORATORS
                   32

-------
                                                              MIDWEST RESEARCH INSTITUTE
                                                                         425 Volker Boulevard
                                                                     Kansas City. Missouri 64110
                                                                       Telephone (816) 753-7600
You are invited to participate in a collaborative test of a modified ver-
sion of EPA Method 106 - "Determination of Vinyl Chloride From  Stationary
Sources," a copy of which is enclosed.  Midwest Research Institute  (MRI)
is under contract to the U.S. Environmental Protection Agency to  conduct
this collaborative test.  The test will consist of two parts:   a  laboratory
test of the analysis procedure and a  field test of the entire method.

For the laboratory test a minimum of  eight collaborators will each  receive
a set of six samples of vinyl chloride with various  interferences present
in some of the samples.  Each sample will be supplied in a 3-liter  capacity
(at STP) aerosol-type can.  A heated  sampling valve  must be used.   Inject-
tion by syringe is not acceptable.

Samples will be introduced into the sample valve loop by inserting  the
needle on the sample can through a septum mounted in the line going to  the
valve.  Since the sample flow is under positive pressure, no sample pump
is used.  Each sample will be analyzed in triplicate using two  different
columns—a 2 m x 3.2 mm OD stainless  steel column packed with 60/80 Chrom-
osorb 102 and a composite column consisting of the Chromosorb 102 column
followed by a 2 m x 3.2 mm OD stainless steel column packed with  20% SF-96
on 60/80 mesh AW Chromosorb P.  Vinyl chloride concentrations on  each  sam-
ple/column combination are to be calculated by both  peak area and peak
height.  The original strip chart recordings must be submitted  to MRI with
the results.

The sample cans must be returned to MRI after the analyses with sufficient
pressure to allow a final check for stability.

Cylinders containing approximately 5, 10, and 50 ppm vinyl chloride in  ni-
trogen are to be used as standards and will not be supplied by  MRI.  Each
cylinder must be certified by the manufacturer by comparison against  (a) a
gravimetrically calibrated vinyl chloride permeation tube,  (b)  a  vinyl  chlo-
ride gas mixture analyzed by the National Bureau of  Standards,  or  (c)  stan-
dard gas mixtures prepared in accordance with Section 7.1 of Method 106.
                                    33

-------
                                                             MIDWEST RESEARCH INSTITU1 -
                                                                         425 Volker Boulevard
                                                                     Kansas City, Missouri 641
                                                                      Telephone (816) 753-76
If you are interested in participating  in  the  laboratory  test  of the
method, you are asked to submit a  firm,  fixed  price bid for  the  collabor-
ative test.  The collaborators will be  selected on the basis of  the  ana-
lyst's experience in the analysis  of vinyl chloride,  the  analyst's exper-
ience in gas chromatography, the ability to  supply the necessary equipment
for the test, and cost.  The experience  of the person who will perform the
analysis and the model numbers of  the gas chromtograph and sample valve
that will be used should be submitted with your bid.  The person perform-
ing the analysis is designated as  Key Personnel.  If  this person does  not
perform the analyses the contract  may be declared void.   Bids  must be  re-
ceived by April 15, 1977.  The samples will  be sent on or about  June 15th
and results must be submitted to MRI within  1  month.

The field test of the method will  consist  of a smal-1  group of  collabora-
tors obtaining samples and analyzing the samples at a vinyl  chloride plant.
Collaborators will obtain duplicate samples  with a minimum of  three  sets
of samples per day for 2 days of testing.  For this test  each  collaborator
must be able to supply the necessary Tedlar  bags and  enclosures.  All  sam-
ples must be analyzed within 72 hr.  This requires either a  gas  chromato-
graph which can be taken to the test area or provision for rapid shipment
and analysis after each test.  A crew of two is anticipated  for  each col-
laborator.  The site for the field test  has  not been  selected.   You  are
asked to indicate your interest in participating in the field  test.  If
interested, please state the model number of the gas  chromatograph which
would be used and the number of rigid leakproof containers with  100  liter
Tedlar baigs that you could supply  for the test.  MRI  is not  at this  time
soliciting bids for the field test.

If you have any questions in regard to  the test, please call George  Scheil
or Paul Constant at (816) 753-7600.

Sincerely,

MIDWEST RESEARCH INSTITUTE
George W. Scheil
Associate Chemist

Enclosures

GWS:sw                             34

-------
            APPENDIX B





FINAL INSTRUCTIONS TO COLLABORATORS
                 35

-------
                                                             MIDWEST RESEARCH INSTITUTE
                                                                         425 Volker Boulevard
                                                                     Kansas City, Missouri 64110
                                                                      Telephone (816) 753-7600
July 28, 1977
The EPA sponsored collaborative test of Method  106  - "Determination  of  Vinyl
Chloride from Stationary Sources," has now started. Your  laboratory  is  one
of the 10 collaborators selected  for the laboratory test  of  the procedure.
This letter is to inform you of the revised test schedule and other  changes
in the test.

Each collaborator should receive  six cylinders  of vinyl chloride  in  nitrogen
during the week of September 12,  1977. These cylinders may or may not contain
vinyl chloride and interferences. The sample cylinders are moderate  pressure
Freon-type canisters with a volume of about 8 ft 3  (at STP).  An adapter  to
connect the cylinders to 1/4 in.  Swagelok fittings will be supplied. If you
prefer a different adapter, please contact MRI. The samples  are introduced
into the sample valve loop via Teflon tubing by partially opening the cylin-
der valve. A stainless steel valve or capillary restrictor may be needed to
limit flow into the sample loop.  A sample pump  is not needed.

Each sample will be analyzed in triplicate using two different columns--a
2 m x 3.2 mm OD stainless steel column packed with 60/80 Chromosorb  102 and
a composite column consisting of  the Chromosorb 102 column followed  by  a
2 m x 3.2 mm OD stainless steel column packed with  20% SF-96 on 60/80 mesh
AW Chromosorb P. Vinyl chloride concentrations  on each sample/column combi-
nation are to be calculated by both peak area and peak height. The original
strip chart recordings must be submitted to MRI with the results. The chart
recordings and calculated results for all six samples must be mailed to MRI
by October 15, 1977.

The sample cylinders should be saved with sufficient pressure for additional
measurements until MRI has reviewed your results.  After your results have
been examined at MRI you will be  notified if the samples need to  be  returned
to MRI to resolve any questions.  If your results are satisfactory you may
keep the sample cylinders.

Cylinders containing approximately 5, 10, and 50 ppm vinyl chloride  in  nitro-
gen are to be used as standards and will not be supplied by  MRI.  Each cylinder
must be certified by the manufacturer by comparison against:  (a) a  gravi-
metrically calibrated vinyl chloride permeation tube; (b) a  vinyl chloride
gas mixture analyzed by the National Bureau of  Standards; or (c)  standard gas
mixtures prepared in accordance with Section 7.1 of Method 106.
                                      36

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Page 2
July 28, 1977
These requirements have been published in the Federal Register and a copy is
attached together with a copy of the Method 106 procedure.  The gas supplied
should provide a certificate stating compliance with the Federal Register
requirements. Please send MRI copies of the certificates with your data.

A check of several gas suppliers indicates that Matheson and Air Products
do not supply vinyl chloride standards. Airco in Riverton,  New Jersey,  Ana labs
in North Haven, Connecticut, and Scott Specialty Gases in Plumsteadville,
Pennsylvania, state that they can supply standards which conform to the
Federal Register requirements.

You will receive additional information regarding the field test at a later
date. If you have any questions in regard to the test, please call Dr.  George
Scheil or Mr. Fred Bergman at (816) 753-7600.

Sincerely,
George W. Scheil
Associate Chemist

GWS:clk

Enclosure
                                      37

-------
                         APPENDIX G
METHOD 106 - DETERMINATION OF VINYL CHLORIDE FROM STATIONARY
                   SOURCES WITH AMENDMENTS
                             38

-------
  METHOD 108—DCTCRMINATION  or  VINYL
     CfTLORlDC  FROM STAT1ONHRV SOL'RCZS
               INTRODUCTION

  Performance of this method should not oe
attempted by  persons  unfamiliar with the
operation  of a gas chromatograph, nor by
those who are unfamiliar with source  sam-
pling.  »s  there  are  many details  that are
beyond the scope of this  presentation. Care
muat be  exercised  to  prevent exposure of
sampling personnel to  vinyl chloride, a  car-
cinogen.
  1. Principle and Applicability.
  1.1  An Integrated bap sample of stack gas
containing vinyl  chloride (chloroethylenei
la subjected  to chromatographlc  analysis.
using a flame lonl/.atlon detector.
  1.2  The method Is applicable to the  meas-
urement of vinyl chloride In stack gases from
ethytene dlchlortde. vinyl  chloride and  poly-
vinyl chloride  manufacturing processes, ex-
cept where the vinyl chloride Is contained in
participate matter.
  2. Range and Sensitivity.
  The  lower limit of detection will vary ic-
cordlng to the chromatograph used. Values
reported Include 1  x  10-' ing and 4  x  10-'
mg.
  3. Interferences.
  Acetaldehyde.  which  can occur  In   some
vinyl chloride sources, will Interfere with the
vinyl chloride peak from the Chromosnrn 102
column. See sections 4.3.2 and 6.4. If resolu-
tion of the vinyl chloride peak Is  still not
satisfactory for  a  particular  sample,   then
chromatograph  parameters can  he  further
altered  with prior  approval of the  Admin-
istrator. If alteration of the chromatoyraph
parameters fulls to resolve the vinyl chloride
peak, then supplemental confirmation of the
vinyl chloride  peak through  an  absolute
analytical  technique, such 0.1  mans spectro-
acopy, must be performed.
  4.  Apparatus.
  4.1  Sampling (Figure 1).
  4.1.1   Probe—Stainless  steel. Pvrer  glass,
or Teflon  tubing  according to  stack temper-
ature, each  equipped with a glass wool  plug
to remove partlculuic matter.
  4.1.2  Sample line—Tenon. 6.4 mm outside
diameter, of  sufficient  length  to  connect
probe to bag. A new unused piece Is employed
for each series of hog samples that constitutes
an emission test.
  4.1.3  Male  (2)  and  female  (2)  stainless
steel quick-connects, with ball checks  (one
pair without) located as shown In Klgure 1.
  4.1.4  Tctllar  bags, 100 liter  capacity—To
contain sample. Teflon bays  are not accept-
able.  AlumLnlzcd  Mylar bays may  be used.
provided  that  the  samples  are   analyzed
within 24 hours of collection.
  4.1.5  Rigid Icakproof containers  for 4.1.4.
with covering to protect contents from sun-
light.
  4.1.6  Needle  valve—To adjust sample flow
rate.
  4.1.7  Pump—Leak-free. Minimum  capac-
ity 2 liters per minute.
  4.1.8  Charcoal  tube—To  prevent  admis-
sion of vinyl chloride to atmosphere  in vicin-
ity of samplers.
  4.1.9  Flow  meter—For observing  sample
flow rate: capable  of  measuring a now range
from 0.10  to 1.00 liter per minute.
  4.1.10  Connecting  tubing—Teflon, 6.4 mm
outside diameter,  to assemble  sample train
(Figure 1).
  4.1.11  Pilot tube—Type S (or equivalent),
attached  to the probe so that  the sampling
flow rate  can  he  regulated  proportional  to
the stack gas velocity.
  4.2   Sample recovery.
  4.2.1  Tubing—Tefloo.  64   mm   outside
diameter,  to connect bag to gas chromato-
graph  sample loop. A  new unused piece Is
employed for each series of bag samples that
constitutes an emission test,  and U to be dis-
carded upon conclusion of analysts of those
bags.
  4.3   Analysis.
  4.3.1  Gas  c'.iromatograph—With   flame
lonlzatlon  detector,  potentiometric   strip
chart recorder and 1.0 to 5.0 ml heated sam-
pling loop in  automatic simple valve.
  4.3.2  Chromatographlc column—Stainless
steel. 2.0  x  3.2  mm, containing 80/100 mesh
Chromosorb  102. A secondary  colum of OB
SF-96. 20% on  60'80 mesh AW Chromosorb
P, stainless steel.  2.0 m  x  3.2 mm.  will  be
required u*  acetaldehyde Is present. If used.
the SF-96 column is placed after the  Chromo-
sorb  102  column.  The  combined  columns
should then be operated at 110'C.
  4.3.3  Flow meters  (2)—Rotameter type.
0 to 100 ml/mln capacity, with flow  control
valves.
  4.3.4  Gas  regulators—For   required  gas
cylinders.
  4.3 5  Thermometer—Accurate to one de-
gree centigrade, to measure temperature of
heated sample loop at time of sample Injec-
tion.
  4.3.6  Barometer—Accurate to 5 mm Hg. to
measure  atmospheric  pressure around  gas
chromatograph  during  sample  analysis.
  4.3.7  Pump—Leak-free. Minimum  capac-
ity 100 ml/mln.
   4.4  Calibration.
  4.4.1  Tubing—Teflon. 6.4   mm    outside
diameter, separate  pieces marked  for  each
calibration  concentration.
  4.4.2  Tedlar  bags—Slxtcen-lnch  square
size, separate bag  marked for  each  calibra-
tion concentration.
   4.4 3   Syringe—0.5 ml. gas tight.
   4.4.4  Syringe—50/.1.  gas light.
                                                1 Mention of trade names on specific  prod-
                                              ucts does not constitute endorsement by  the
                                              Environmental Protection Agency.
  4.4.6  Flow  meter— Rotaineter  type,  0  to
1000  ml/mln  range  accurate to  ±1%,  to
meter  nitrogen  In preparation of standard
gas mixtures.
  4.4.0  Stop watch—Or Known accuracy,  to
tlmo gas flow In preparation of standard gas
mixtures.
  5. Reagents.  It  In necessary that  all rea-
gents be of  chromatographlc grade.
  5 1   Analysis.
  5.1.1  Helium gas  or nitrogen  g
-------
•nd  the attenuator getting.  Record the lab-
oratory pressure. Krom the chart,  select the
peak hAving the retention time correspond-
ing to vmyl chloride,  cvs determined In Sec-
tion  72. Measure the  peak aren. Am.  by use
of H.I.. and a. dKc Integrator or n planlmeter.
Measure the peak height, II,,,. Record Am and
the retention time. Repeat  the Injection at
lea«t two times or until two consecutive vinyl
chloride peaks do not  vary In nrea more than
6';,.  Til* murage value for  these  two areas
v;in  be vi.'»• il 10 compute the bag concenira-
tloit.
   Comp.iie the ratio of H,., to Am for the vinyl
chloride sample  with  the came ratio for the
standard prnk which  Is closest  In height. As
a  guideline, if  these  ratios  dlfTer  by  more
tliiui 10', .  Hie vinyl chloride peak may not
be pure ir>i  M'M-'in o the ambient  temperature and
b.ironirlri'.1  pressure near the bag. (Assume
'.lie  reuti.e humidity  to be 100  percent.)
From a writer saturation vapor pressure table,
determine the record  nnd water vapor con-
tent of the bag.
   7  Calibration and  Standards.
   7 1  PiepAi-atlon of  vinyl chloride standard
gas mixtures. Evacuate a sixteen-lnch square
Tedlwr  br.g  that has passed a  leak  check
(described  In Section 7.4)  and  meter In  5.0
liters of nitrogen. While the bag Is fllllng. use
the 05 ml syrmre to  Inject  250jil of 99.9 + %
vinyl chloncle through  the  wall of the bag.
Upon  withdrawing the syringe needle. Im-
mediately  cover the  resulting hole  with a
piece of adhesive tape. This gives a concen-
tration of 50 ppm of 7inyl chloride. In a like
manner use the other  syringe to prepare dilu-
tions  haviri; 10 and  5 ppm vinyl chloride
concentrations  Place  each bag on  a smooth
eurftce and alternately depress  opposite
sides of the bng 50 times  to further mix the
gases.
   73  Determination  of  vinyl  chloride  re-
tention tliv.e  This section can  be performed
simultaneously  with  Section 7.3.  Establish
chromatopraph  conditions   Identical  with
those  In Section 6.3,  above. Set attenuator
to X  1 position.  Flush the sampling loop
with zero  helium or nitrogen  and activate
the  sample valve. Record  the Injection time.
the  sample loop  temperature,  the  column
temperature, the  carrier  gas flow rate, the
chart  speed and  the  attenuator  setting
Record  peaks and detector responses that
occur In the absence  of vinyl chloride Main-
 tain conditions  With the equipment plumb-
ing  arranged identically to Section 6.3, flush
 the  sample loop for 30 seconds  at the rate of
 100  ml  mln with  one of the vinyl chloride
calibration mixtures and activate the sample
 valve. Record  the Injection time. Select  the
 peak  that  corresponds  to  vinyl chloride.
 Measure the distance on the chart from the
 Injection time to the  time at which the peak
 maximum  occurs  This quantity, divided by
 the  chart speed, is den.ied as  the retention
 time Record
   73   Preparnnon of  chromatoyraph cali-
 bration curve.  Mnke  a  g;'.s  chromatognphlc
 measurement  of cacn standard gas mixture
 (described  in  Section 71)  using  conditions
 Identical  with  those listed In  Section  83
 above  Flush the sampling loop  for 30 seconds
 at the rate of 100 ml  mln with  each standard
 gas  mUture  and activate the  sample  valve.
 Record  C.. the concentrations  of vinyl chlo-
 ride Injected, the  attenuator  setting, chart
 speed,  peak area, sample loop  temperature.
 column temperature, carrier gns  flow rate.
 and  retention  time.  Record the laboratory
 prensiire Calculate At,  the  peak area multl-
   tucV hit
                            NntlM it tnd« «•«« »« fM<:'<* ftcki.tti <••• MC c»»tltuce
                                     tr ck« anil	ul rntwIlM Acme?.
plied by the attenuator netting Repeat until
two Injection areas an within 5%, then plot
those points vs C,. When the other coaoeo-
traUons have  been plotted, draw  a  smooth
curve through the points.  Perform calibra-
tion daily, or before and  after each set  of
bag  samples,  whichever  !» more  Irequeut.
  7.4  Bug leak checks. While performance
of this section Is required subsequent to bag
use. It Is  also advised  that It be performed
prior to bag use. After each use. make sure
a bag did not develop lealcs a* follows. To leak
check, connect a water manometer and pres-
surize the bag to 5-10 cm  H.O (24 ui H.O).
AJlow to stand for  10 minute* Any displace-
ment In the  water manometer  Indicate* a
leak. Also check the rigid container lor leeks
In thl* manner.
   (NOTE:  An  alternative leak  check method
la to pressurize the bag to 5-10 cm  H.O or
2-4  In. H.O and  allow to stand  overnight.
A deflated bag  Indicates  a leak.) For  each
sample bag In  Its rigid container,  place a
rolametrr  In-line between the bag and the
pump Inlet. Evacuate the  bag  Failure of the
rotame'.er to register zero  flow when the bag
appears to be empty  indicates a leak.
   8. Calculations.
   8.1  Determine the  sample peak  area a*
follows:
  8.3  Tlnyl  chloride  concentrations.  Prom
the  calibration curve described In  Section
7.3, above, select the  value  of  C,  that cor-
responds to A,., the sample  peak are*. Cal-
culate Cb M follows:

                    c,r,r.
                           Equation 106-3

Where:

 JJ.t-Tlio «3ter vapor cwiU-.m of the bag laniMv, u

    • The concentration of vinyl chloride 10 the b«f
      sample in ppm.
    • The concenlrution of rlnyl chloride UidiomUd by
      the gin chronifvU'craph, la ppm.
    •The reference pressure, the laboratory pnsvire
      reoorded during cahhrivtlon. nun H%.
    • The sample  loop  temperature oo the
      Kale at the tliuo of analysis. °K.
    • The laboratory prc&suro ut tune of aiialyiu. mm
      Hg.
   ",-The referents t«nipcniUire,  the  wmple  loop
      temperature reeoruod diulnf oalibratlon, *R'
  Ct
  C.
  p,
  r.
  p.
                 A,
 where:
   X.—Tin* sninplo p^ik ivrna.
   A . — The mf^uro
-------
                                            29008
                                                                                              RULES  AND REGULATIONS
   9: Section 1.1  of Test Method  106
 is corrected as follows:
 v 1-1. An . integrated bag  sample of naek
 ga> containing vinyl chloride (chloroeth«o»)
 is subjected to chromatographlc analysl*. sift-
 ing  a flame ionlzailon detector.--;.
        - 13.  Section 4.1.10 of Test Method 106 Is
        corrected as follows:     '.."-.•*
          4.1.10  Connecting   tuWny.  Teflon.  6.4
        mm outside diameter,  to assemble  sample
        crain (Figure 10«-1).              -
   10. Section 3 «f Test
. corrected as follows:...:, .
   3. Interferences. Aceialdehvde. which CAO
 occur In tome vinyl chloride sources. will In-
 terfere with  .the vinyl  chloride peak  from
 the Chromasorb  103 ' column. Se« sections
 4.3-2  and 6.4.  II resolution  of  the  vinyl
 chloride peak Is soil not satisfactory  for a
 particular sample, then cnromatograph pa-
 rameters can be  further altered -with  prior
 approval  of the Administrator. If alteraaon
 of the chromatograph  parameters falls to
 resolve the vinyl chloride  peak,  then  sup-
 plemental confirmation of the vinyl chloride
 peak  through an absolute analytical  tech-
 nique. such as mass spectroscopy.  must b*
 performed.

   11.  Section 4.1 of Test Method 106 is
 corrected as follows:
   4.1  Sampling < Figure 106-1).

   12.  SecUon 4.1.3 of Test Method 106 is
 corrected as follows:
   4.1.3  Male (2) and female  (2)  stainless
 steel quick-connects, with ball checks  (one
 pair without) located as -shown  In
 106-1.
'•  --     14.  Section 4.3.2 of Test Method 108 is
108 is  amended as follows:'
          4.32 Chramatogra-phic column, stainless
        st«el. 2 mx3J "»«. containing 80/100 mesh
        Chromasorb  103. A secondary column of OE
        SP-98, 20  percent on 60/80 mesh AW Chroma-
        sorb P, stainless steeL 2 m x 3.3 mm or Pora-
        pak T. 80/100 mesh, stainless steel. 1 mx3J
        n-.m 15 required If acetaldehyde Is  present. If
        used, a secondary column-is placed after the
        Chromasorb   103   column.   The  combined
                should, then be operated at  120* C..
          15.  Section 5.2. of Test Method 108 Is
        revised as follows:  .....     .....:.
          S3  Calibration, Use one of the  following
        options:- either 5J.1 and 3.2.3, or 3J2JJ... -•   -
          3Ja  -Vinyl. cWorule, . 99.S-t- percent. Pure
        vinyl chloride gaa certified by tb» manufac-
        turer to contain a minimum of 99.9 percent
        vinyl, chloride for use In  the  preparation of
        standard gas mixtures In Section 7.1. If-the
        gta manufacturer maintains a bulk cylinder
        supply of 99.9+ percent vinyl chloride, the-
        certtflcaC"*  analysis  may  have been  per-
       formed on this supply rather than on  esch-
        gm» cylinder prepared from thu hulk, supply.
        Th« dat* of.gas cylinder preparation and the
        certtfled analysis must havo been  affixed to
        tha  cylinder before- shipment from Oe gas
        manufacturer to the buyer.    - .
          3.2.2  Nitrogen gas.  Zero grade, for prepa-
        ration of  standard gcs nurtures.  . • • •
          S-3-3  Cylinder  standards  (3).  Gas  mix-
        ture  standards  (SO. . 10.  and  3 ppm vinyl.
        chloride In nitrogen cylinders) for wnlch the
        ga*  composition  haa been  censed by the .
        manufacturer. The manufacturer must  have
        recommended a maximum shelf life for each
        cylinder i~  Uiat the concentration does not
        change greater  t.han  =5  percent  from, the
        certified value. The date of gaa cylinder prep-
        aration. certified  nnyl chloride concentra-
        tion and  recommended maximum  Jbelf Life
        must have been afflxed to- the cy Under before
        snip men: from the gas manufacturer to the
        buyer. These gaa mixture standards may be
        directly used to  prepare a  chromatograph
        calibration curve as described In section 7.3.
          5.2.3.1  Cylrmter Jtandordj   certification:
        Tie concentration of vinyl chloride In nitro-
        gen In each cylinder must have been certified
        by the manufacturer by a direct analysis of
        each cylinder using an analytical procedure
        that the manufacturer had calibrated, on the
        day of  cylinder analysis.  The calibration of
        the analytical procedure shall,  as a minimum.
        have utilized a three-point calibration curve.
        It is recommended that  the manufacturer
        maintain  two calibration  standards and usa
        these standards In. the following way: (1)  a
        high concentration standard (between 50 and
        100  ppm)  for preparation of  a calibration
        curve by in appropriate dilution technique:
        (2)  a  low concentration standard  (between
        5 and 10 ppm) for venflcaclon  of the dilution
        technique used.
          5.2.3.2  Establishment and  verification of
        calibration standards. The concentration of
        each calibration  standard must have  been
        established   by  the  manufacturer  using
        reliable  procedures.  Additionally,   each
        calibration  standard must  have been  7erl-
        Sed bv the manufacturer by one  of  tbe
        following   procedures,  and tie agreement
        becwees  tie  Initially  deterT^iced  concen-
        tration value and the verification concen-
        tration value  n^ust he witritn  — 5  percent:
        .':)  -.••r::±;atlon  value dererzilzed iy  csm-
        par'-son  w.:h  a   cailbra^d   vinyl  chlar'.ie

                         41
 permeation  tube.  (2)  verification   value
 determined by  comparison with a gas mix-
 ture prepared  In accordance with the  pro-
 cedure described In section  7.1  and  using
 99.9+ percent  vlnyle chloride, or (3)  verifi-
 cation  value   obtained   by  having   the
 calibration standard  analyzed by  the Na-
 tional Bureau of Standards.  All  calibration
 standards  must  be  renewed  on  a  time
 Interval  consistent with  the shell  life  of
 the cylinder standards sold.

 '   16. Section  6.2 of Test Method 106 Is
 •amended as follows:
 -8.2  Sam-pie storage. Sample bags must  be
 kept  out of  direct  junllght. When  at  all
 possible  analysis  is to be performed xlthln
 24 hours, but  In no- case in excess of  72
 hours of sample collection.

    17. Section  7.1 of Test Method 106 Is
 'amended as follows:.-              '   ' •
 - 7.1  .Preparation of vinyl chloride stand-
• ant gaa  mtxrunj. Evacuate  a sixt«en-lnch
 square Tedlar  bag  that has  passed i  leak
 check (described In Section 7.4)  and meter
 In. 5  liters of  nitrogen. . While  the bag is
 fllllng, use  the  0.3-  ml syringe to  Inject
 250uJ   of  99.94-  percent  vinyl  chloride
 through  the  wall of .the  bag. Upon with-
 drawing, the  syringe  needle,  immediately
 cover- the  resulting hole  with  a piece  of
. adhesive tape.  Too  bag  now  contains a
 vinyl  chloride concentration  of  JO-ppm.  In
. a " tike manner • use  the  other  syringe-  to
 prepare gas mixtures having  10 and 5 ppm
 vinyl  chloride  concentrations.  Place  each
 bag on  a  smooth  surface and  alternately
 depress  opposite  sides of the bag iO  times
 to further mix. the gases. These gas mixture
 standards may  be used for  13 days from  the
 date of preparation, after .which  time  prep-
 aration  of new  gas - mixtures is- required.
 fCADTtow.—Contamination  may  be a  prob-
 lem when  a  bag is reused if tbe  new  gas
 mixture  standard  contains  a  lower  con-
 centration  than  tbe  previous  gas  mixture
 standard did.)

   _18. Section  7.3 of Test Method 106 is
 amended as follows:
   7.3  Preparation  of  Cfiromatograpti. cali-
 bration curve. Make a ga»-cbroma:o?raphlc
 measurement of *ach gas mixture standard
 (described In section 5.2.2 or 7.1)  using con-
 ditions Identical with those listed In sections
 8.3 and 8.4. Flush the sampling loop  for  30
 seconds at the race of 100 mi/min with each
 standard gas mixture and activate the sam-
 ple valve. Record C..  the  concentration  of
 vinyl  chloride Injected, the attenuator set-
 ting,  chart  speed,  peai area, sarr.ple loop
 temperature, column  temperature,  carrier
 gas flow rate, and retention time.  Hecord trie
 laboratory  pressure. Calculate A«. the peax
 area multiplied by the attenuator setting.
 Repeat until  two Injection areas  are within
 5 percent, then plot these points 7. Ce. TThen.
 the other concentrations nave been plotted.
 draw  a smooth curve through  the  polnto.
 Perform calibration dally, or before and a.'ter
 each set  of bag samples, wblchever is  more
 frequent.

-------
RETENTION INDICES FOR POSSIBLE VINYL CHLORIDE  INTERFERENCES
                            42

-------
                      TABLE C-l.  RETENTION INDICES FOR POSSIBLE VINYL CHLORIDE  INTERFERENCES
U>




Methane*
Echylene
E thane *
Propane'"
Methyl chloride
Methanol

Acetaldehyde

Echylene oxide

Vinyl chloride
Isobutane
Isobutylene
1-Butene
n- Butane*
1,3-Butadiene
trans-2-Butene
Ethanol
Ethyl chloride
cis-2-Butene
1 , 1-Dichlo roe thy lone
trans- 1 , 2- Dichloroethy lene

2 m Chromosorb 102
100°C
100
180
200
300
320
330

355

355

360
380
395
395
400
400
400
415
415
415
480f
510f
2 m Chromosorb 102
4- 1 in Porapak T
120°C
100
180
200
300
340
395

400

395

375
380
395
395
400
410
410
475
430
415
490f
495f
2 m Chromosorb 102
+ 2 m SF-96
120°C
100
175
200
300
320
350

375

375

360
380
385
395
400
395
400
435
415
410
480f
505t
2 m Chromosorb 102
+ new 2 m SF-96
120°C
100
-
200
300
325
375
(low levels retained)
400
(low levels retained)
-
(low levels retained)
360
380
390
-
400
395
_
-
410
-
-
—

* Reference compounds for
t Column at 150°C.
indices.








-------
      APPENDIX D
LETTER TO COLLABORATORS
          44

-------
                                                            MIDWEST RESEARCH INSTITUTE
                                                                       425 Volker Boulevard
                                                                   Kansas City, Missouri 64110
                                                                    Telephone (816) 753-7600
December 1, 1977
The results of the laboratory part  of  the  collaborative test of EPA Method
106 are now complete. The preliminary  analysis  of  the  data indicates that
no serious errors occurred. A few chromatograms were misinterpreted and
two collaborators did not detect any acetaldehyde  with the chromosorb 102
column. The contents of the samples are  given  in  the  the table attached.
Vinyl chloride and isobutane have proved to  be  stable.  The acetaldehyde
concentration is decaying gradually in most  samples and methanol has
either disappeared or is eluting with  isobutane.  The chromosorb 102 col-
umn should have resolved all samples except  1814,  but  acetaldehyde is
retained on the SF-96 column. The separation of isobutane is usually
reduced on SF-96. Analyses conducted by  NBS  was only for vinyl chloride.
Sample No.


  1814


  4036



  4786

  6800



 10673

 60106
Components (N  Balance)


 6.8 ppm vinyl chloride
45.1 ppm acetaldehyde

13.0 ppm vinyl chloride
 7.1 ppm methanol
21.1 ppm isobutane

 8.73 ppm vinyl chloride

 7.04 ppm vinyl chloride
 4.5 ppm methanol
10.6 ppm isobutane

18.4 ppm acetaldehyde

 2.24 ppm vinyl chloride
Vinyl Chloride Found by
       NBS (ppm)


           6.75
          13.0



           8.57

           7.34



           0.05

           2.26
                                  45

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                                                           MIDWEST RESEARCH INSTITUTE
Page 2
December 1, 1977

The field part of the collaborative test of EPA Method 106 under MRI's
prime EPA Contract No. 68-02-2737 is scheduled for February 14-16, 1978.
The test will be conducted at the Diamond Shamrock facilities in Deer Park,
Texas. The participants in the laboratory test are requested to submit
fixed-price bids if they are interested in participating in the field test.
A total of three groups will conduct simultaneous sampling from a manifold.
Each collaborator must have two personnel on the site, a sampler and a
gas chromatograph operator. The person who preformed the original labor-
atory analyses must be the GC operator and shall be designated as key per-
sonnel for this test.

Each team must provide the following equipment for the test:

     1.  A gas chromatograph (FID) with gas sampling valve and recorder.
     2.  Three calibration gas cylinders (5, 10, and 50 ppm vinyl chloride).
     3.  A minimum of 2 tested 100 liter bags and enclosures as required
           by Method 106. Tedler or aluminized Mylar bags are acceptable.
     4.  Rotameter, pump, and other necessary items to obtain samples from
           the manifold and perform leak tests.

An area (indoors) will be provided for the chromatographs. Air, hydrogen,
and carrier gas will be provided to all teams as well as suitable 110 V
AC power. The samples will probably contain low levels of vinyl chloride.
The instrument used must have sufficient sensitivity to accurately measure
vinyl chloride as low as 0.5 ppm.

Since sampling will be done from a common (ground level) manifold, no pitot
or oxygen measuring equipment is needed. Sampling will be done at a constant
rate of about 0.5  pm for 1 hr periods. The manifold will probably be under
slight positive pressure so that the pump can be removed during sampling,
although it must be available for emptying bags and making leak checks.
The sampling will be done in a restricted access area where explosion-
proof pumps are required. If an AC pump is used it must be inside an ex-
plosion-proof or inert purged housing. Battery driven approved personnel
sampling-type pumps are also acceptable.

The tentative work schedule is:

February 14 - Set-up and test equipment.

February 15 - Sampling - each team will collect 4 samples. Analysis - each
team will analyze their own vinyl chloride standards and one of the other
teams' standards. Each team will also analyze their own 4 samples and 4
samples obtained by other teams.
                                  46

-------
                                                          MIDWEST RESEARCH INSTITUTE
Page 3
December 1, 1977

February 16 - Same as February 15; pack equipment and clear the site.

Each test day should be completed within 8-10 hr. All samples and standards
will be analyzed in triplicate in the same manner as used in the laboratory
collaborative test, except that only one column will be used. Each team
must bring both the Chromosorb 102 and SF-96 columns to the test and the
column(s) to be used will be selected on the set-up day. All samples will
be measured by peak height and area, and the original recorder charts must
be sent to MRI.

The participants will be chosen on the basis of ability to meet the nec-
essary requirements, performance on the laboratory test, and cost. Firm,
fixed-price bids must be submitted to MRI by January 4, 1978 to be con-
sidered. Technical questions should be referred to Dr.  George Scheil. Con-
tractual questions should be referred to Ms. Sequin Lukon. The MRI phone
number is (816) 753-7600.

Sincerely,

MIDWEST RESEARCH INSTITUTE
George Scheil
Associate Chemist

GSrsw
                                  47

-------
                   APPENDIX E
TENTATIVE PROCEDURE FOR SAMPLING AND ANALYSIS OF
 VINYL CHLORIDE USING CHARCOAL ADSORPTION TUBES
                       48

-------
                                                    December 1977
               TENTATIVE METHOD FOR THE DETERMINATION OF
                            VINYL CHLORIDE
1.  Principle and Applicability.

    1.1    Vinyl chloride (chloroethene) is absorbed from air onto charcoal

adsorbers, which are subsequently extracted with carbon disulfide.  The

resulting solutions are then measured chromatographically, using a flame

ionozation detector.

    1.2    The method is applicable to the measurement of vinyl chloride

in ambient air using a 24-hour sampling period.*



2.  Range and Sensitivity.  The limit of detection is approximately

          3                                              1
0.003 mg/m  (1 ppb).  The maximum of the range is 20 mg/m  (8 ppm); it

may be increased by extending the calibration range or by diluting the

sample.



3.  Interferences.  At the present time, there are no known common pollu-

tants in the ambient atmosphere in sufficient concentrations to interfere

with the measurement of vinyl chloride.  However, certain volatile hydro-

carbons and Freons have elution characteristics similar to vinyl chloride.
* Warning:  Vinyl chloride is a suspected carcinogen.  Care must be exercised
to protect operators from breathing vinyl chloride fumes.  Carbon disulfide
is toxic and its vapors form explosive mixtures with air.  Work with this
material in a well ventillated fume hood.
                                    49

-------
Among the latter is Freon 12 (dichlorodifluoromethane).   Under certain

conditions, a peak is associated with the injection and  subsequent with-

drawal of the microsyringe into and from the G.C.  septum.  These peaks can

also give interferences with the vinyl chloride peak.


4.  Precision and Accuracy.  Replicate gas chromatographic analyses of

standard gas mixtures and sample aliquots should not deviate by more than

3 per cent relative standard deviation.  When the  entire analysis is

repeated, preliminary studies indicate that relative standard deviations

of 6 per cent are attainable.  No information is presently available on

accuracy.


5.  Apparatus.

    5.1    Sampling - Air Monitoring materials.

    5.1.1  Pump - Capable of maintaining an air pressure differential

greater than 0.5 atmospheres at the desired flow rate.

    5.1.2  Critical Orifice - Twenty-seven gauge 3/8"  hypodermic needle.

To control flow rate at approximately 200 ml/min.

    5.1.3  Tubing - 18 cm length of 10 mm O.D.  borosilicate glass with

tapered ends, to prepare adsorption tube.

    5.1.4  Serum caps - 5 x 9 ram and 7 x 11 mm  sizes.

    5.1.5  Vibrator - To achieve close packing  of  the  adsorption tube.

    5.1.6  Air flow meter - Rotometer type; 1 - 260 ml/min range.   To

calibrate critical orifice.
                                    50

-------
    5.1.7  Furnace, muffle - To operate at 400°C.

    5.2    Sample recovery.

    5.2.1  Graduated cylinder - Glass stoppered; capacity, 25 ml (TC).

    5.2.2  Pipette, dropping - 2 ml.

    5.2.3  Serum bottle - Narrow mouth for septum sealing; 2 ml.

    5.2.4  Serum cap - With Teflon coating on the side of the septum

exposed to the sample 5 x 9 mm size.  (Hewlett-Packard #5080-8713  has

been found to be satisfactory).

    5.2.5  Aluminum serum cap seal.

    5.2.6  Crimper - For use with aluminum serum cap seals.

    5.3    Analysis.

    5.3.1  Gas chromatograph - With flame ionization detector and

potentiometric strip chart recorder.

    5.3.2  Chromatographic column - stainless steel, 2.5 m x 3.2 mm O.D.,

containing 0.4% Carbowax 1500 on Carbopak A packing, (w/w)

    5.3.3  Microsyringe - 0 to 10 microliter range,  graduated.

    5.3.4  Gas regulator - 4 to 50 psig range.

    5.3.5  Needle valve - to control standard gas flow.

    5.3.6  Teflon tubing - 10 mm O.D.

    5.3.7  Tygon tubing sleeve - 10 ram I.D.
  Mention of trade names or specific products does not constitute endorsement
   by the Environmental Protection Agency.
                                    51

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6.  Reagents

    Unless otherwise indicated, it is intended that all reagents be chromato-
graphic grade or conform to the specifications established by the Committee

of Analytical Reagents of the American Chemical Society, where such speci-
fications are available; otherwise, use best available grade.
    6.1    Sampling.
    6.1.1  Charcoal - Activated coconut shell charcoal.  (Fisher Scientific
Company,  6 to 14 mesh is effective.)
    6.1.2  Glass wool - borosilicate
    6.1.3  Aluminum foil.
    6.2    Sample recovery.
    6.2.1  Carbon disulfide.
    6.3    Analysis.
    6.3.1  Nitrogen gas - Zero grade, for chromatographic carrier gas
and for preparation of standard gas samples.

    6.3.2  Vinyl chloride - 128, 25.6, and 12.8 mg/ra3  at 25  C,  1 atm
50 ppm v/v, in zero nitrogen.  Analyzed.   For calibration.
    6.3.3  Combustion Air - Containing less than 1.3 mg/m^ hydrocarbons
(2 ppm as methane).  To operate flame ionization detector.


7.  Procedure.
    7.1    Sampling.
    7.1.1  Activation of charcoal - Heat  charcoal to 400°C for one hour
to remove adsorbed gases.  Store in a sealed container.
                                    52

-------
    7.1.2  Preparation of adsorption tube - Insert glass wool into tubing

(see Section 5.1.3) and tamp into position at one end to a depth of

approximately 2.5 cm.  Mount tube on vibrator in a verticle position.  Add

charcoal a little at a time and vibrate after each addition to prevent

channelling.  Fill tube to a depth of 13 cm with charcoal.  Insert glass

wool into remainder of tube.  Prepare additional adsorption tubes in a

similar and uniform manner.  Cover ends of tubes with serum caps.  Wrap

with aluminum foil to protect tubes from light during storage and subsequent

use.  Insert critical orifice through septum at one end of tube.  Retain

until calibration, sampling and recalibration procedures have been completed.

Sufficient tubes should be prepared from a single lot of charcoal to complete

the sample analysis and associated calibration.

    7.1.3  Sample collection.  Remove serum cap from one end of the adsorp-

tion tube and mount it with open end downward.  Connect critical orifice

to the sampling train.  Begin drawing air through the tube.  Record time

and adsorption tube number.  Continue sampling for 1 hr.  At end of sampling

interval, record time, disconnect adsorption tube from sampling train and

protect open end with serum cap.  Remove sample to analytical area.  Protect
tube from light.

    7.2    Sample recovery.  Fill the graduated cylinder to the 25 ml mark
with carbon disulfide, stopper and cool in an ice bath.  Remove cap and

glass wool from one end of the adsorption tube and, with continued cooling,

rapidly add charcoal to the carbon disulfide.  Stopper cylinder immediately.

(Note:  the mixing of charcoal and carbon disulfide is an exothermic process
                                    53

-------
that causes local boiling of the solution.  The mixture must be cooled

and the container stoppered to prevent loss of vinyl chloride.)  Mix

thoroughly.  Allow mixture to stand for one half-hour in the ice bath.

Mix throughly and draw off 2 ml of the supernatant liquid.  Completely fill

2 ml serum bottle, cap and seal.

    7.3    Analysis.

    7.3.1  Column preconditioning.  Prior to its initial use, the chroma-

tographic column is heat treated to remove impurities.  To do this,

establish a 40-60 ml/min flow of zero nitrogen through the column and raise

its temperature from ambient by 2°C/min to 200°C.  Maintain these conditions

for 48 hours, or until base line drift is eliminated.

    7.3.2  Chromatographic analysis.  Set the column temperature to

60°C and the sample inlet port temperature to at least 170°C.  Operate

the flame ionization detector at the temperature specified by the manu-

facturer.  Using zero nitrogen as the carrier gas, establish a flow rate

in the range consistent with the manufacturer's requirements for the satis-

factory detector operation.  A flow rate of 40 ml/min has been shown to

produce adequate separations.  Observe the base line periodically and

determine that the noise level has stabilized and that base-line drift has

ceased.  Inject a 2.5 microliter aliquot of the supernatant solution of

the sample into the gas chromatograph.  Mark the injection point on the

chart.  (The injection point is defined as the position of the pen on the

chart at the time of sample injection.)  Record the sample number, the

column temperature, carrier gas flow rate, chart speed and the attenuator
                                    54

-------
setting.  From the chart, select the peak having the retention time



corresponding to vinyl chloride.  (See Section 8.3 below).  Measure the



peak height, IL., the distance in chart divisions from the average value



of the baseline to the maximum of the wave form.  Record H  and the reten-



tion time.  Purge the column at 160°C for five minutes.






8.  Calibration and Standards.



    8.1    Calibration of absorption tube flow rates.  Connect absorption



tube to sampling train as in 7.1.3, above.  Connect flowmeter in series.



Turn on pump and measure flow rate.  Record rate and adsorption tube



number.  Repeat flow rate calibration procedure after sample collection.



Denote flow rate before sampling as F^; denote flow rate after sampling



as F2«



    8.2    Preparation of vinyl chloride standard mixtures.  Connect


                          o
regulator to the 12.8 mg/m  standard gas cylinder as shown in Figure 12.2.



Put needle valve on regulator outlet.  Remove serum caps from a fresh ad-



sorption tube.  Connect needle valve to the adsorption tubes with 10 mm



Teflon tubing using an end-to-end sleeve joint at the inlet end of the



adsorption tube.  Connect rotometer to outlet side of the adsorption tube.



           Disconnect sleeve on inlet of adsorption tube.  Purge sample line



briefly, venting gas in a safe area.  Reconnect line and set flow rate to



200 ml/min.   Sample cylinder gas for 1 hr, maintaining constant flow.  Record



sampling start and stop times, inital and final flow rates, tube number,



and cylinder vinyl chloride concentration.  Disconnect adsorption tube and

                                    55

-------
replace  serum caps.  Repeat with fresh adsorption tubes using the 25.6 and

128 mg/nr standards.  Recover the standard samples following the procedure

described in 7.2.

    8.3    Determination of vinyl chloride retention time.  Establish

chromatographic conditions identical with those in 7.3.2 above.  Set

attenuator to X 1 position.  Inject a 2.5 ^1 portion of carbon disulfide

into gas inlet port.  Mark the injection point on the chart and record the

column temperature, the carrier gas flow rate, the chart speed and the

attenuator setting.  Record peaks and detector responses that occur in the

absence of vinyl chloride. Maintain conditions.  Inject 2.5 nl of the
12.8 mg/m3 standard into gas chromatograph.  Mark the injection point on
the chart.  Select the peak that corresponds to vinyl chloride.  Measure

the distance on the chart in mm from the injection point to the peak maximum.

This distance, divided by the chart speed in mm/min, is defined as the
retention time.  Record.

    8.4    Preparation of chromatograph calibration curve.  Make a gas

chromatographic measurement of each standard mixture described in Section 8.2
(12.8 through 128 mg/m3), using conditions identical with those listed in

Section 7.3.2, above.  Record Wvc  V  x C   x Vi/Vs, the attenuator setting,

chart speed, peak height and retention time.  Calculate H , the peak height

multiplied by the attenuator setting.  Plot W   vs H .  Repeat until

replicate measurements do not deviate by more than 370 relative standard

deviation and draw a smooth curve through the points.  Check calibration

after every fifth analysis using the 12.8 mg/m3 (5 ppm) standard mixture
                                    56

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and either the 25.6 or  128 mg/nr*, whichever exceeds the highest unknown





analyzed.  Recalibrate  daily, and whenever remeasurement of a standard gas




sample deviates from its calibration value by more than 6%.










9.  Calculations.




    9.1    Uncorrected  volume.  The volume of air sample is not corrected




to S.T.P., because of the uncertainty associated with 24-hr average




temperature and pressure values.  Determine the air sample volume taken




for analysis.







                    F1 + F2



               Vm ~	 x T x 10'6,





where:




       Vm = The volume of gas sampled (uncorrected), m^.




       F^ = The measured flow rate before sampling, ml/min.




       F2 = The measured flow rate after sampling, ml/min.




        T = The sampling time, min.










    9.2    Determine the sample peak height as follows:





                HC — HmAni>




whe re:




       Hc = The sample peak height, chart divisions.





       ^ = The measured peak height, chart divisions.




       ^ = The attenuator setting.





                                    57

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    9.3    Vinyl chloride concentration.



    9.3.1  Calculate the vinyl chloride concentration as mg/m3.  From the



calibration curve described in Section 8.4, above, select the value of



Wyc that corresponds to HC, the sample peak height.
                     W  V
                      vc s
               Cvc =
                     V V.
                      m i

                      W

                       VC      4

                      V
                       m

where



       Cvc = The concentration of vinyl chloride in the air sample, mg/m •



       Wvc = The quantity of vinyl chloride measured by gas chromatography, mg,



       Vs  = The total volume of carbon disulfide in which the vinyl chloride


              sample is contained, 25 ml.



       Vm  = The uncorrected sample volume, from 9.1 above, m3.



       V^  = The volume of carbon disulfide solution injected into the


              chromatograph for analysis, 0.0025 ml.



    9.3.2  If desired, the concentration of vinyl chloride may be calculated



as parts per million vinyl chloride,



          ppm VC = mg VC/m3 x 0.3915.
10.  Effects of storage.  Charcoal tubes containing adsorbed vinyl



chloride have been found to be stable for more than seven days though



there is some evidence that they are adversely affected by strong sunlight.



Carbon disulfide solutions lose vinyl chloride to the atmosphere but have



been stored unchanged for more than a month in sealed serum bottles having

                                    58

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minimum headspace.  Gas standards may be kept in'poly (vinyl fluoride) gas




sample bags for several weeks without undergoing concentration changes.




However, present knowledge of the stability of vinyl chloride samples is




based on studies with pure substances.  No information is available on the




storage of samples containing other active substances as are commonly




found in ambient air.
                                    59

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11.   References.





     Lodge,  J.  P.,  Pate,  J.  B., Ammons,  B.  E.  and  Swanson, G. A.




    "The Use of Hypodermic Needles  as Critical Orifice  in Air Sampling."




     J.  Air  Pollution Control  Association.   16:4,  197-200, (1966).










    "Vinyl Chloride Monitoring Near the  B.  F.  Goodrich  Chemical Company in




     Louisville,  Kentucky."  Region IV,  U.S. Environmental Protection Agency,




     Surveillance and Analysis Division, Athens, Georgia.  June 24, 1974.
                                    60

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 SERUM CAP-





GLASS  WOOL
GLASS WOOL
                 s^
                 wys?'.S
                 •Vi'fi??-.
                 >CSV5?X-
                 >Vi.C^->>
                                              AIR PUMP
-CRITICAL ORIFICE
                             CHARCOAL
                               61

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                                   TECHNICAL REPORT DATA
                           (Please read Instructions on the reverse before completing}
1. REPORT NO.
                             2.
                                                           3. RECIPIENT'S ACCESSION-NO.
4. TITLE AND SUBTITLE
  COLLABORATIVE TESTING OF EPA METHOD  106  (VINYL CHLORID
  THAT WILL  PROVIDE FOR A STANDARDIZED STATIONARY SOURCE
  EMISSION MEASUREMENT METHOD
                       6. REPORT DATE
                       E)    August 1978
                       6. PERFORMING ORGANIZATION CODE
7. AUTHORI?'
                                                          8. PERFORMING ORGANIZATION REPORT NO.
  George  W.  Scheil  and Michael C.
  Midwest Research  Institute
Sharp
9. PERFORMING ORGANIZATION NAME AND ADDRESS
  Midwest  Research Institute
  425 Volker  Blvd.
  Kansas City,  Missouri  64110
                       10. PROGRAM ELEMENT NO.

                         1HD621
                       11. CONTRACT/GRANT NO.

                         68-02-2737
12. SPONSORING AGENCY NAME AND ADDRESS
  Environmental  Monitoring and Support  Laboratory
  Office of  Research and Development
  U. S. Environmental  Protection Agency
  Research Triangle Park.  N. C. 27711	
                       13. TYPE OF REPORT AND PERIOD COVERED

                         Final	
                       14. SPONSORING AGENCY CODE


                         EPA-ORD
15. SUPPLEMENTARY NOTES
  To be  published as an Environmental Monitoring  Series report
16. ABSTRACT
       Method  106 -  Determination of Vinyl  Chloride from Stationary Sources was
  evaluated  in  a  two-part collaborative  test.   Gaseous samples, prepared  in cylinders
  and containing  interferences in some cases,  were analyzed by a group of 10
  collaborators.   The results showed that Chromosorb 102/SF-96 columns performed
  better when  acetaldehyde interference  was  present, but Chromosorb 102 alone was
  better when  isobutane interference was present.   Collaborator biases averaged
  0.18 ppm  (0.47  mg/mj) low with a standard  deviation of 0.72 ppm (1.86 mg/m  ).
  Both peak  height and area measurements yielded  similar results and the  bias found
  was due entirely to low results from using Chromosorb 102 and not from  the
  Chromosorb 102/SF-96 column.

       A three  collaborator field test was conducted on the vent of a carbon bed
  absorber at  a vinyl  chloride polymer facility.   The group had a standard deviation
  of 0.39 ppm  (1.01  mg/m3) and 0.24 ppm  (0.62  mg/m3) for sampling and analysis,
  respectively.   Analyst skill is a major factor  in the use of Method 106.
                               KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
          b.IDENTIFIERS/OPEN ENDED TERMS  C.  COSATI Field/Croup
  Air pollution
            Collaborative  testing
            Vinyl Chloride
            Stationary Sources
   13B
13. DISTRIBUTION STATEMENT

  Release to Public
          19. SECURITY CLASS (This Report I
               UNCLASSIFIED
21. NO. OF PAGES
  61
                                             20. SECURITY CLASS (This page)
                                                   UNCLASSIFIED
                                                                        22. PRICE
EPA Form 2220-1 (9-73)
                                         62

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