Environmental Protection Technology Series
EVALUATION  OF  A NEW MICROVOLUME  3 HSc
          ELECTRON  CAPTURE DETECTOR AND
    ANCILLARY DATA SYSTEM FOR  PESTICIDE
                            RESIDUE ANALYSIS
                             Health Effects Research Laboratory
                            Office of Research and Development
                            U.S. Environmental Protection Agency
                      Research Triangle Park, North Carolina 27711

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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 ENVIRONMENTAL PROTECTION TECH-
NOLOGY series. This series describes research performed to develop and dem-
onstrate instrumentation, equipment, and methodology to repair  or prevent en-
vironmental degradation from point and non-point sources of pollution. This work
provides the new or improved technology required for the control and treatment
of pollution sources to meet environmental quality standards.
This document is available to the public through the National Technical Informa-
tion Service, Springfield, Virginia 22161.

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                                               EPA-600/2-78-010
                                               February 1978
EVALUATION OF A NEW MICROVOLUME  HSC ELECTRON CAPTURE DETECTOR

   AND ANCILLARY DATA SYSTEM FOR PESTICIDE RESIDUE ANALYSIS
                            By
            Robert C.  Hanisch and Robert G. Lewis
             Health Effects Research Laboratory
              Environmental Toxicology Division
                 Analytical Chemistry Branch
                  Project No. 7529 and 7602
                 Program Element No. 1EA615
        U.S.  ENVIRONMENTAL  PROTECTION AGENCY
         OFFICE OF  RESEARCH AND DEVELOPMENT
         HEALTH EFFECTS RESEARCH LABORATORY
         RESEARCH TRIANGLE  PARK, N.C. 27711

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                            DISCLAIMER

     This report has been reviewed by the Health Effects Research
Laboratory, U.S. Environmental Protection Agency, and approved for
publication.  Approval does not signify that the contents necessarily
reflect the views and policies of the U.S. Environmental Protection
Agency, nor does mention of trade names or commercial products
constitute endorsement or recommendation for use.
                                ii

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                             FOREWORD

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

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

     This report represents a research effort to extend and improve
analytical measurement of a variety of pesticides, polychlorinated
biphenyls and other pollutants in our environment.  The emphasis is on
the evaluation of new detector systems for such environmental contam-
inants .

                                       John H. Knelson, M.D.
                                             Director,
                                Health Effects Research Laboratory
                                 iii

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                                  ABSTRACT





The performance of a linearized  HSc electron capture detector (BCD) and



its ancillary data system was evaluated for use in the analysis of



pesticide residues.  Serial dilutions of pesticide standards were used



to determine the maximum linear range and sensitivity of the detector.



This detector was found to have a significantly greater linear range for



the test compounds than a linearized   Ni electron capture detector


                                                                63
evaluated.  The sensitivity was only marginally better than the   Ni



BCD.
                                 iv

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                             CONTENTS






                                                  Page




Disclaimer                                          ii




Foreword                                           iii




Abstract                                            iv




List of Figures                                     vi




List of Tables                                      vi




Sections




I         Conclusions                                1




II        Introduction                               2




III       Experimental                               4




IV        Discussion                                 9




V         References                                25

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                          LIST OF FIGURES


No.                                                    Page

 1        ATC 140A baseline current levels               14

 2        Linearized   Ni ECD baseline current           15
          levels

 3        Peak area integration on the ATC Model         24
          160 Memory and Display (MAD) System
                          LIST OF TABLES


No.                                                    Page

 1        Compounds Used for Detector Evaluation          5

 2        Comparison of the Lower Limits of               9
          Detection (LLD) for Two Linearized
          Electron Capture Detectors

 3        Maximum Linear Range with +5* K-Value          11
          Variation

 4        Maximum Linear Range with 4^10% K-Value         12
          Variation

 5        Data Collection Time as a Function of          20
          Dwell Time
                                vi

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                             SECTION I




                            CONCLUSIONS






The micro-volume electron capture detector evaluated in this study was




found to possess an extended linear range compared to another popular EC




detector.  In addition, the detector was a factor of ten more sensitive




for certain compounds than another popular EC detector tested.  These




two advantages were more than nullified, however, by the susceptibility




of the detector to contamination, which severely limited its useful




life.  The ancillary data system was useful in terms of data acquisition,




storage, and computation of data, but the scope of application of the




system is limited by certain design deficiencies.

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                            SECTION II




                           INTRODUCTION






Since its first application in 1960 as a gas chromatographic detection




technique/  the electron capture (EC) detector has played a major role




in the analysis of pesticides, polychlorinated biphenyls, and other




organic pollutants of environmental interest.  The various types of EC




detectors that are commercially available differ in the ionizing source




used, the design of the detector cell, and the modes of electrical




stimulation and measurement.  Each of these facets can have considerable




effect on the performance of an EC detector.






Three types of radioactive sources are commonly used in EC detectors:




tritiated-titanium, nickel-63, and tritiated-scandium foils.  The




tritiated-titanium ( HTi) sources are characterized by high specific



activities which result in greater sensitivity and linear range than




sources employing other radioactive isotopes.  In addition, the low




energy (18 keV) beta-rays emitted from such sources permit the con-




struction of a detector with minimum internal volume, a characteristic




which can be helpful in providing ionizing radiation throughout all of




the interelectrode space.   HTi sources are prepared by occluding




tritium in titanium-plated stainless steel or copper foils.  Since




tritium is easily lost from these foils, the maximum temperature at




which they can be used is about 225°C.  However, it is often necessary




or desirable to operate an EC detector at higher temperatures; e.g., for




analysis of high-boiling compounds and for "bake-out" (rejuvenation of

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the foil by heating).   The DC electrical stimulation typically employed



for these sources interposes additional obstacles in achieving optimum



detector performance.   Electron capture detectors operated in the DC



mode characteristically exhibit drifting baselines, sensitivity vari-


                                  234
ations, and limited dynamic range. ' '





Detectors utilizing nickel-63 as the radioactive source can be operated



at higher temperature (up to 375°C)  but only at the expense of linear



dynamic range and sensitivity.  By operating the detector in the fixed-



frequency pulsed modei  the limited linear range can be extended somewhat



and the problem of baseline drift encountered with tritium detectors can



be eliminated. '





Tritiated-scandium  ( HSc) sources have a maximum temperature limit of


                                                                    2
325°C and source activities are available that approach one curie/cm .



This provides a higher baseline current than any other electron-capture



beta source.  When this type of source is operated in the constant-



current/variable-frequency pulsed mode, the linear range of the detector



is significantly increased.





The purpose of this study was to evaluate an electron capture detector



employing a  HSc source operated in the constant current/variable-



frequency pulsed mode.   The ATC Model 140A detector, which is manufactured



by Analog Technology Corporation, Pasadena, California, is the only high



temperature tritium detector currently on the market.  This detector is



represented as having a maximum linear range of 10  when utilized in



conjunction with an ATC  Model 160A Memory and Display (MAD) system.

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                            SECTION III




                           EXPERIMENTAL






In order to test the sensitivity and linearity of the detector against




a wide range of response characteristics, a variety of compounds were




chosen from several different chemical classes.  Thirteen compounds or




mixtures were selected which included chlorinated hydrocarbons, organo-




phosphates, polychlorinated biphenyls and polychlorinated naphthalenes:




          e-BHC                    Ronnel




          Hexachlorobenzene        Malathion




          Aldrin                   Ethyl Parathion




          Perthane                 Phorate




          p_,£'-DDE                 Aroclor 1254




          p_,p_'-DDT                 Halowax 1014




          Mir ex




All materials were primary reference standards obtained from the Pesti-




cide Repository, Health Effects Research Laboratory, Research Triangle




Park, N. C.  Empirical formulae and chemical nomenclature are given for




each standard in Table 1.






The test solutions of various concentrations were prepared from each




standard in n_-hexane (pesticide quality).  Each of the standards con-




sisted of a series of concentrations covering each decade from 1 pg/yl




to 1 pg/pl.  This provided a total of seven different concentration




levels over which the linearity and sensitivity of the detector could be




evaluated.  The standards were evaluated individually to simplify

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         Table 1.  COMPOUNDS USED FOR DETECTOR EVALUATION
Common Name
8-BHC

Hexachlorobenzene
Ronnel

Malathion
Perthane
Aldrin
Ethyl Parathion
Mirex
p,p'-DDE
p,p'-DDT
Aroclor 1254
Halowax 1014
Phorate
Empirical
 Formula
C6H6C16
C6C16
C8H8C13°3PS
C10H19°6PS2
C18H20C12
C12H8C16
C10C112
C14H8C14
C14H9C15
C12H5C15
C10H2-5Cl5-5
     Chemical Name
£ isomer of hexachlorocyclo-
hexane
Hexachlorobenzene
0,0-Dimethyl-O-(2,4,5-tri-
chlorophenyl)phosphorothioate
S-[1,2-bis(ethoxy carbonyl)
ethyl]-O,O-dimethyl phosphoro-
dithioate
1,l-Dichloro-2,2-bis(p-ethyl
phenyl)ethane
1,2,3,4,10,10-Hexachloro-
1,4,4a,5,8,8a-hexahydro-
1,4-endo-exo-5,8-dimethano-
naphthalene
0,0-Diethyl-0-p_-nitro-
phenylphosphorothioate
Dodecachlorooctahydro-1,3,4-
metheno-2H-cyclobuta[cd]-
pentalene
1,l-Dichloro-2,2-bis
(p-chlorophenyl)ethylene
1,1,l-Trichloro-2,2-bis
(pj-chlorophenyl) ethane
mixture of polychlorinated
biphenyls
mixture of polychlorinated
naphthalenes
0,0-Diethyl-5-[(ethylthio)-
methyl]phosphorodithioate

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identification and avoid potential coelution from the gas chromatograph.






The compounds were analyzed on a Tracer 560 gas chromatograph equipped




with a 183 cm x 4 mm (i.d.) glass column packed with 3% OV-1 on 80- to




100-mesh Gas Chrom Q.  The column was maintained at a temperature of




200°C with a 70 ml/min flow of 5% methane/95% argon carrier gas.  The




inlet ports and detector were maintained at 210°C and 240°C, respec-




tively.






The Model 160A MAD system is designed to allow the collection of data in




the form of automatically calculated peak area and peak heights, as well




as simultaneous production of gas chromatograms on a conventional strip




chart recorder.  In addition, it has the capability of data retrieval




from the disk file for later generation in the form of hard (paper)




copy.  Consequently, the data obtained in this study was reported from




all four outputs when possible.  Peak height was used as the response




parameter for the data obtained from the strip chart chromatogram.






To ensure the statistical validity of the data, five replicate injec-




tions were made for each concentration level of each standard used in




the study.  The response data obtained was then normalized to a 5.0 yl




injection volume to eliminate variation in response due to injection




technique.  The normalized data were averaged and the standard




deviation and percent relative standard deviation for each

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of the data outputs were calculated using a small sample statistics

      Q

table.   The average response data for each of the output modes at



each concentration level for a given standard were used for the final



linearity calculations.





For a given standard, the linearity of response was calculated from



the average response for each concentration level of each test



solution.  The calculation used in this analysis is:




               ,.   , _        ,,,.    Response X Attenuation Factor
          Normalized Response (K)	P   Sample       	
If a detector is linear, K should be constant within +5% over the



entire range of concentration levels.  For automatically-calculated



peak area and peak height data, the equation is reduced to:





                      _   Response

                        Sample Amount



since the attenuator control has no effect on these two forms of



data output.





The sensitivity of the detector was established by injecting progressively



smaller amounts of the standards into the GC system until the lower



limit of detection(LLD) was reached.  The LLD was defined as that



amount of sample which would produce a signal equal to twice the noise



level.





An aldrin standard with a concentration of 20 pg/pl was selected to



serve as a reference to determine the long-term response stability of



the detector.  The standard was analyzed on a daily basis under identical

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chromatographic conditions in order to detect any variation in response




over the duration of the study.  Some of the late-eluting compounds




required more than one day of analysis time to complete the entire




concentration series.  In these cases, the data obtained from the




analyses were adjusted in a corresponding fashion for any variations




observed in the response from the aldrin standard.  All data were




corrected to the response level observed on the first day of analysis.






Since the baseline current available to an electron capture detector




critically affects the overall system sensitivity and performance,




this parameter was monitored on a daily basis.  With the electrometer




offset control centered and pure carrier gas flowing through the




detector, the adjustable reference current was varied until a recorder




output of zero volts was obtained.  At this point the nominal base-




line frequency was 5 kHz.  The available baseline current was then




recorded and the system was operated at that current level for the




remainder of the day.  Any subsequent variations in the baseline were




corrected through use of the offset control.

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                            SECTION IV

                            DISCUSSION


DETECTOR

As can be seen from the data presented in Table 2, the sensitivity of

the detector was found to be comparable to that of a commercially-

available linearized   Ni electron capture detector.  Although the  HSc

detector was more sensitive by a factor of 10 for three of the 13

standards tested, this was not considered to be a significant advantage

over other EC detectors.
     Table 2.  COMPARISON OF THE LOWER LIMITS OF DETECTION (LLD)
               FOR TWO LINEARIZED ELECTRON CAPTURE DETECTORS
Compound
B-BHC
HCB
Ronnel
Malathion
Perthane
Aldrin
Ethyl Parathion
Mirex
p,p'-DDE
p,p/-DDT
Aroclor 1254
Halowax 1014
Phorate
LI
ATC Model 140A
5
0.05
0.5
50
50
0.5
5
5
0.5
5
50
50
50
J) (pg) 63
Tracor Linear Ni
5
0.05
5
5
50
5
5
5
5
5
50
50
50

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The results of the linearity determinations are found in Tables 3 and 4.


The detector has been represented  as having a linear range of 10 .   The


results listed in Table 3 indicate that the maximum linear range achieved

                         4
in this laboratory was 10  with a +_5% deviation allowance.  Linearity


was not measurably greater when the response factor was allowed to vary


by +10%.  As can be seen from the tabulated data, the observed linear


range was highly dependent on compound type.




This, behavior has been previously reported for constant-current EC


detectors which utilize a low-frequency pulsed operation.    The high-


frequency operation employed in the ATC Model 140A should have circum-


vented this difficulty but apparently did not.  Despite these aberrations,


the linear range of the  HSc detector was found to be significantly


greater than that of a Tracer linearized   Ni EC with which it was


simultaneously compared.
Background noise from the detector was monitored on a daily basis in


order to establish the maximum usable sensitivity of the instrument.


The short-term noise characteristics of the detector when operated at


maximum sensitivity were quite good.  The amplitude of the short-term


noise was usually less than 0.5% full-scale deflection (f.s.d.).  With


the exception of the four-minute period immediately following injection,


the long-term noise was typically less than 2% f.s.d. when the detector


was operated at maximum sensitivity.  At the most sensitive attenuation,


the chromatograms exhibited a 10% overshoot after the solvent peak which


usually required approximately four minutes of recovery time to return




                                  10

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Table 3.  MAXIMUM LINEAR RANGE WITH +5% K-VALUE
          VARIATION
Compound
B-BHC
HCB
Ronnel
Malathion
Perthane
Aldrin
E. Parathion
Mirex
p,p'-DDE
p,p'-DDT
Aroclor 1254
Halowax 1014
Phorate
Linearity
MAD Peak
Area
io3
io2
<101
io1
io1
io4
io1
io1
io2
1
io1
1
io3
as calculated
MAD Peak
Height
io3
io1
io2
io1
1
io3
io1
1
io1
1
io2
1
io1
from:
MAD Recorder
Peak Height
io4
io2
io1
IO1.'
io1
io4
io2
io2
1
1
<10
io2
io1
io1
Recorder
Peak Height
io4
io2
io2
1
io2
io3
io1
1
1
1
io2
io1
io1
                         11

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          Table 4.  MAXIMUM LINEAR RANGE WITH +10%
                    K-VALUE VARIATION
Compound
8-BHC
HCB
Ronnel
Malathion

MAD Peak
Area
io4
2
io3
io1
,«2
MAD Peak
Height
io3
io2
io3
io1
,~1
MAD Recorder
Peak Height
IO4
io2
io3
io1
,~1
Recorder
Peak Height
io4
io2
io3
1
<10
-,,,2
Aldrin

E. Parathion

Mi rex

p, p'-DDE

p,p'-DDT

Aroclor 1254

Halowax 1014

Phorate
10
10
10
10'
10
10
10
10
10
10
10"
10"
10"
10
10
10'
10
10
10"
10
                            10J
10
10
10
10
10
10
10
                             10
10
                                 12

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to baseline.  The negative peaks reported by Olds   were not observed in



this evaluation.
As previously mentioned, the zero-volt baseline is a measure of the



detector baseline current, and is therefore a useful parameter for



monitoring the condition of the detector source foil, the carrier gas



purity, air leaks into the system, and all other conditions that can



result in reduced baseline current.  The stability of the detector in



terms of baseline current variations is illustrated in Figure 1.  As



indicated in the graph, it was necessary to change the first foil (A)



after the sixteenth day of use.  It should be noted that the actual time



from the beginning of the evaluation to the point at which the baseline



current had degenerated to an unacceptable level spanned a period of 42



days.  A statistical analysis of the baseline current levels shows that



for foil A the arithmetic mean, standard deviation, and percent relative


                                —8               —9
standard deviation are 1.24 x 10   amps, 2.5 x 10   amps, and 20%



respectively.  For foil B, the same analysis results in the respective


                    —8               -9
figures of 1.66 x 10   amps, 2.3 x 10   amps, and 14%.  This foil was



used for a total of 25 days out of 72.  In either case the variance is



unacceptable when compared to the baseline current variations of a



linearized   Ni EC detector as shown in Figure 2.





It could be argued that the observed variations for the ATC 140A are the



results of factors independent of the detector itself.  However, when



it is considered that the detector under study and the linearized



  Ni BCD against which it was compared were both mounted on identi-



cal gas chromatographs employing identical columns, ferrules, and septa,
                                13

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          1      I      I      I       [
2.00
0.75
i      i       i      i      r
                                     11      13     15

                                  DAYS OF ACTUAL USE*
      17
21
23
25
   Figure 1. ATC 140 A baseline current levels. Currents monitored only on day of use. Total
   time Foil A in detector ca. 6 weeks; Foil B, ca. 14 weeks.
     Does not include weekends or other inoperative periods.

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    9
          I     I.   I    I    I    I     I    1          I     I    I              I     I     I    7  7
 I  7P:OK>OO-OK>O<>OO^
en

-  6
^x

t-

uj  5
DC
oc

3  4
C9
               I     I     I     I    I     I     I     I     I	I     I     I    I    I    I    I    I    I
          3     5     7    9    11    13    15   17   19   21   23    25    27    29   31    33    35   37   39    41

                                               DAYS OF ACTUAL USE*


        Figure 2. Linearized 63Ni EC baseline current levels. Currents monitored only on day of use. Total time 20 weeks.


        * Does not include weekends or other inoperative periods.

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and utilizing a common source of carrier gas, it is apparent that the



difference in performance must either lie in the detector or in the



possibility of an air leak in the system.  The latter possibility was



eliminated through periodic inspections of all the gas lines and



connectors.





It can be concluded from the data presented in Figure 1 that the overall



lifetime of the source foil is unacceptably limited.  When using most



EC detectors, it is good practice to reduce the carrier flow rate to a



minimum and add a purge flow at the end of the operating day in order



to conserve the argon-methane carrier gas.  This procedure was initially



used in the evaluation of the ATC '140A with the exception of the



application of a purge flow.  The design of this detector did not include



a purge line for the source cell.  It was observed that the baseline



current level steadily decreased with each day that the carrier flow



rate was minimized for overnight operation.  Consequently, it was



necessary to maintain the carrier flow at operating level throughout



the duration of the study.





On one occasion it was necessary to reduce the carrier flow rate



overnight to conserve argon-methane.  When the carrier flow was returned



to normal operating level on the next day, it was discovered 'that the


                                         —8            -9
baseline current had fallen from 1.3 x 10   to 4.4 x 10   amps, an



unacceptable level for operation.  The flow was maintained at 70 ml/min



for a period of three days with the hopes that the baseline current



would be restored.  The temperature of the detector was also increased



from 240°C to 280°C in an attempt to decontaminate the foil, but this



only resulted in further decrease of the baseline current.





                                 16

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In another instance, a regional electric power "brownout" required that




all of the GC column ovens in the laboratory be shut down overnight.




After power had been restored the following morning, the ATC detector




required three days to return to its former baseline current despite the




fact that the detector temperature and carrier flow rate had been main-




tained at normal operating levels.  The   Ni EC detectors in the lab-




oratory had returned to their former baseline current levels within an




hour after power restoration.






The loss of baseline current, and consequently detector sensitivity in




all cases cited above was probably caused by the adsorption of material




eluted from the GC column onto one or both of the electrodes or by the



coating of the electrodes with "dirt" or carbonaceous material.  Such




contamination can give rise to the formation of a contact potential




that may either enhance or oppose the applied potential.  The fact that




the internal volume of the cell is only 180 microliters and that the




detector has no provision for purging probably makes the ATC.140A more




susceptible to contamination than other EC detectors.






The ATC Model 140A EC detector employs a scandium tritide source with




an activity of one curie.  Consequently, the safety aspects of operating




and maintaining the device should be considered.  The beta-particles




emitted from the source have a maximum energy of 0.018 MeV and are




absorbed by less than 1 mg/cm2 of aluminum.  As a result, there should



be no detectable radiation from the tritium external to the detector
                                 17

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chamber.  However, there is a possibility of tritium leakage from the




cell through the exhaust port, especially at high temperature operation.






The installation kit provided with the detector includes several meters




of flexible tubing which is used to vent the effluent from the exhaust




port of the detector into a fume hood.  Several of these detectors




operated in an inadequately ventilated room could constitute a potential




health hazard.






For laboratories that have in-house EC detector maintenance programs




involving replacement of foils and cleaning of detector cells, additional




safety considerations are necessary.  When the foil of the ATC 140A




EC detector employed in this evaluation was changed, wipe tests were




made on various detector components -during the disassembly process.




One of the tests indicated low level contamination on the exterior




surface of the detector housing.  Another demonstrated that the outside




surface of the detector cell itself was contaminated at the 0.5 yCi




level.  It could not be determined whether this high contamination




resulted from tritium leakage from the source foil or from external




contamination by the manufacturer during the assembly process.  In




either case, regular maintenance of this type of detector would require




stringent observation of radiation safety practices.






MEMORY .AND DISPLAY  (MAD) SYSTEM




The Model 160A Memory and Display (MAD) system was evaluated in terms of



display utility, storage and recall capability, ease of integration, and



mechanical reliability.  Data recorded in the MAD data memory is shown
                                 18

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graphically on the CRT display monitor with operator control of all




display parameters including the memory segment displayed, attenuation,




baseline offset/ and linear or semilogarithmic presentation.  The




maximum number of data memory channels that are available in this




system is 4096 (4K mode).  The system is capable of splitting the




memory into two equally-sized segments of 2048 channels each (2K mode).




This capability offers two distinct advantages:  first, when the CRT




display is operated in the split-screen format two chromatograms that




have been previously recorded in the 2K mode can be displayed simul-




taneously for comparison; secondly, a chromatogram capable of being




contained within 2K of memory will only occupy half as much disk storage




space as a chromatogram contained within 4K of memory.  This latter




characteristic becomes important when it is considered that the MAD




system stores all available memory channels in the disk file whether or




not data collection was terminated prior to filling all of the channels.




Consequently, in order to conserve disk storage space, it is necessary




to use the minimum allowable memory range.  The frequency with which




data points are collected can be controlled by the dwell time selector.




With this control, the sampling interval can be varied from 0.01 seconds




to 40.95 seconds in 0.01 second increments.  Since the CRT is only




capable of displaying 512 data points at any given time, depending on




the selected display span and memory range, the display will show a




maximum of every fourth data channel (2K mode) or every eight data




channel (4K mode).  The MAD system selects 512 equally-spaced channels




for display if the displayed memory region contains more than 512




channels.






                                19

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In this evaluation the display system was found to be quite useful to

the extent that a chromatogram could be manipulated or attenuated after

it was generated.  The original chromatogram and any alterations thereof

could be stored in the disk file memory for later retrieval or generated

in hard copy form as a strip chart chromatogram or both.  The primary

difficulty encountered with the display system was the limited capa-

bility for real-time data acquisition.  Table 5 lists the maximum data

collection time as a function of dwell time for each of the memory

ranges.  In theory, these collection times should be adequate for most

chromatographic applications.  For example, at a dwell time of 40.95

sec/channel over a range of 4096 channels the system can collect data

for over 46 hours.  However, when actual chromatograms are generated

while using the MAD system, it becomes apparent that the maximum useful

dwell times and resulting data acquisition and display times are con-
          Table 5.  DATA COLLECTION TIME AS A
                    FUNCTION OF DWELL TIME
Dwell
Time
(sec)
0.01
0.1
1.0
10
40
Maximum Data
2K
. .Mode
0.34
3.4
34
340
1365
Collection Period (min)
4K
Mode
0.68
6.8
68
680
2730
                                20

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siderably less than the theoretical limit.  This is illustrated by the




following case in which an aldrin standard was used to generate chro-




matograms for display on the MAD system.  Initially the 2K memory range




was used in conjunction with a display span of 2048 channels.  Repeated




injections of the aldrin standard at dwell times varying from 0.1




seconds to 3.0 seconds produced chromatograms which exhibited several




interesting characteristics.  It was found that a dwell time of 0.1




seconds was inadequate in that the display filled so rapidly there was




insufficient time for the peak of interest to completely fit on the




screen.  In addition, as the dwell time was increased, the baseline




noise increased correspondingly and increasing amounts of background had




to be subtracted from the chromatogram to keep the baseline at roughly




the same level from sample to sample.  As the dwell time increased, it




became more and more difficult to distinguish small sample peaks from




the background noise.  Additionally, the apparent position of the aldrin




peak was shifted from right to left on the display as the dwell time was




increased.  While quantification by peak area measurement was not




affected by this behavior, the peak height was found to increase pro-




portionally with dwell time as expected.






The experiment was repeated using dwell times of 0.3, 10, and 40 seconds.




Each dwell time was tested at span ranges of "2048, 1024, and 512.  This




was done in order to determine whether or not the GC peak of interest




would be visible as it shifted to the extreme left side of the display




at the higher dwell times.  With the exception of the sample run at the




40-second dwell time, the peak was discernable at all span ranges.  At
                                21

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a dwell time of 40 seconds no peak was readily apparent at a span range




of 2048.  Neither the span range nor the dwell time had any affect on




the peak area measurement.  The measured peak height increased with




increasing dwell time, but in a non-linear fashion.  Again background




noise increased appreciably as dwell time increased.






Using the results of these experiments/ it was deduced that for most GC




applications encountered in this laboratory the optimum dwell time is




0.3 seconds.  This setting yields an acceptable compromise between




maximum data collection time and acceptable background noise.  However,




this means that the chromatographic conditions of an experiment will




have to be adjusted so that the compounds of interest will elute in less




than 20.48 minutes, as this is the maximum allowable data collection




period at this dwell time.  Somewhat longer run times can be achieved by




increasing the dwell time to a level required to collect the data while




at the same time attenuating the display to the point where background




noise is minimized.  Unfortunately, this must be accomplished at the




expense of sensitivity.






The MAD system exhibited another interesting characteristic during the




course of the evaluation.  When extremely dilute samples were being




analyzed, the system sensitivity was not as good as that derived from




data presented on a simultaneously-generated strip chart chromatogram.






When using the MAD system, peak parameter computations are performed by




manually defining the boundaries of a peak and allowing the system to




automatically compute the peak area, amplitude, and retention time.  The






                                22

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peak is defined by setting movable upper and lower level cursors, which




appear on the video display with the data.  The area bounded by the data




curve and the straight line joining the two cursors is automatically




shaded by the MAD system so that the defined area is clearly indicated.




An example of this can be seen in Figure 3.  For single-component




chromatograms, peak parameter computations were found to be no problem.




However, in a multicomponent mixture, calculation of peak area and




amplitude was tedious as each peak had to be defined manually prior to




computation.






The storage and recall capability of the disk file is quite useful.  As




mentioned previously, data can be stored for later manipulation and




calculation.  During the course of the evaluation, no variations in a




recalled data set in terms of peak limits, area, amplitude, and re-




tention time were found.  The major difficulty encountered with the




memory system was the poor mechanical reliability of the disk file.  The




disk system had to be returned to the factory on three separate occasions




for repairs.  The MAD system can be operated without the disk unit but




this severely limits the utility of the system.
                                23

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-
            Figure  3.  Peak  area  integration on  the  ATC Model 160 Memory and Display (MAD)  system.

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                             SECTION V

                            REFERENCES

 1.   Lovelock, J. E., and S. R. Lipsky.  J. Am. Chem. Soc. 82, 431
     (1960).

 2.   Lovelock, J. E..  Nature 182, 1460 (1958).

 3.   Wentworth, W. E., R. S. Becker, and R. Tung.  £. Phys. Chem. 71,
     1652 (1967).

 4.   Steelhammer, J. C.,  and W. E. Wentworth.  J_. Chem. Phys. 51, 1802
     (1969)I

 5.   Wentworth, W. E., E. Chen, and J. E. Lovelock.  £. Phys. Chem. 70,
     445 (1970).

 6.   Lovelock, J. E., and N. L. Gregory.  3rd Int. Symp. Gas Chromatogr.,
     Academic Press, New York 1962, p. 219.

 7.   Maggs,  R. J., P. L.  Joynes, A. J. Davies, and J. E. Lovelock.
     Anal.  Chem. 43, 1966 (1971).

 8.   Dean,  R. B., and W.  J.  Dixon.  Anal. Chem. 23, 636 (1951).

 9.   Karasek, F. W., and L.  R. Field.  Research/Development 28, No. 3,
     42 (1977).

10.   Sullivan, J. J., and C. A. Burgett.  Chromatographia 8, No. 4, 176
     (1975).

11.   Olds,  K. L.  "Pesticide Monitoring Special Study 44-0107-77:
     Evaluation of Linear Electron Capture Detector," U. S. Army,
     Environmental Hygiene Agency, Aberdeen Proving Ground, Maryland,
     May, 1976  (NTIS No.  AD A030980).
                                25

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                                   TECHNICAL REPORT DATA
                            (Mease read Instructions on the reverse before completing)
1. REPORT NO.

:PA-6QO/2-78-01Q
J:
4. TITLE AND SUBTITLE
 Evaluation of A NEW MICROVOLUME 3HSc ELECTRON CAPTURE
 DETECTOR AND .ANCILLARY  DATA for Pesticide  Residue
 Analysis	
                                                            3. RECIPIENT'S ACCESSION-NO.
                                 5. REPORT DATE

                                   Fphriiarv
                                 6. PERFORMING ORGANIZATION CODE
7. AUTHOR(S)
                                                            8. PERFORMING ORGANIZATION REPORT NO.
  Robert C. Hanisch and  Robert G. Lewis
9. PERFORMING ORGANIZATION NAME AND ADDRESS
 Analytical Chemical  Branch
 Environmental Toxicology Division
 Health Effects Research  Laboratory
 Research Triangle  Park.  N.C. 27711
                                 10. PROGRAM ELEMENT NO.

                                   1EA615
                                 11. CONTRACT/GRANT NO.
 12. SPONSORING AGENCY NAME AND ADDRESS
  Health Effects Research Laboratory
  Office of Research  and Development
  U.S. Environmental  Protection Agency
  Research Triangle Park, N.C. 27711
                                                            13. TYPE OF REPORT AND PERIOD COVERED
                  RTP.NC
                                 14. SPONSORING AGENCY CODE
                                    EPA 600/11
 16. SUPPLEMENTARY NOTES
 16. ABSTRACT
       The performance  of a linearized  3HSc electron capture  detector (ECD) and  its

  ancillary data  system was evaluated for use in the analysis of pesticide residues.

  Serial dilutions  of pesticide standards were used to determine the maximum  linear
                     %.
  range and sensitivity of the detector.   This detector was found to have a

  significantly greater linear range for  the test compounds than a linearized &3Ni

  electron capture  detector evaluated.  The sensitivity was only marginally better

  than the 63Ni ECD.
17.
                                KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
                    b.lDENTIFIERS/OPEN ENDED TERMS  C. COSATI Field/Group
  electron capture
  chemical detection
  pesticides
  residues
                                                 14  B
                                                 07  C,  D
18. DISTRIBUTION STATEMENT

  RELEASE TO PUBLIC
                    19. SECURITY CLASS (ThisReport)'

                      UNCLASSIFIED
21. NO. OF PAGES

  32
                                              20. SECURITY CLASS (Thispage)
                                                 UNCLASSIFIED
                                               22. PRICE
EPA Form 2220-1 (9-73)
                                             26

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