EPA-650/2-74-133
DECEMBER 1974
Environmental Protection Technology Series
                                     DEVELOPMENT
                                 OF  A  PROTOTYPE
                               NITRATE  DETECTOR
                                   Office of Research ond Development
                                     Environmentol Protection Agency

                                         Washington, DC 20460

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                   RESEARCH REPORTING SERIES


Research reports of the Office of Research and Development, U.S. Environ-
mental Protection Agency, have been grouped into series.  These broad
categories were established to facilitate further development and applica-
tion of environmental technology.  Elimination of traditional grouping was
consciously planned to foster technology transfer and maximum interface
in related fields.  These 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
          9.  MISCELLANEOUS

This report has been assigned to the ENVIRONMENTAL PROTECTION
TECHNOLOGY series.  This  series describes research performed to
develop and demonstrate instrumentation, equipment and methodology
to repair or prevent environmental 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.

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                              EPA-650/2-74-133
      DEVELOPMENT
   OF  A  PROTOTYPE
  NITRATE  DETECTOR
               by
        J. McCoy, L. Forney,
    A. Zakak, J. Ehrenfeld, J.  Driscoll

    Walden Research Division of Abcor
          201 Vassar Street
     Cambridge, Massachusetts 02139
        Contract No. 68-02-0591
          ROAP No. 26AEK
      Program Element No. 1A1010
    EPA Project Officer:  T. G. Dzubay

    Chemistry and Physics Laboratory
  National Environmental Research Center
Research Triangle Park, North Carolina 27711
            Prepared for

 OFFICE OF RESEARCH AND DEVELOPMENT
U.S. ENVIRONMENTAL PROTECTION AGENCY
      ' WASHINGTON, D.C. 20460

           December 1974

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                        EPA REVIEW NOTICE
This report has beer, reviewed by the National Environmental Research
Center - Research Triangle Park, Office of Research and Development,
EPA, and approved for publication.  Approval does not signify that the
contents necessarily reflect the views and policies of the Environmental
Protection Agency , nor  does mention of trade names or commercial
products constitute endorsement or recommendation for use.
 This document is available to the public for sale through the National
 Technical Information Service, Springfield, Virginia 22161.
                                   11

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                         TABLE OF  CONTENTS
          TITLE PAGE

          ABSTRACT                                            ii
          TABLE OF CONTENTS                                   ill

          LIST OF FIGURES                                     iv

          LIST OF TABLES                                      v

Section
I.         CONCLUSIONS                                         1
II.       RECOMMENDATIONS                                     3

III.      INTRODUCTION                                        4

IV.       DISCUSSION OF PROGRAM                               7

          A.  GENERAL                                         7
          B.  PHASE I - DEVELOPMENT AND DESIGN                7
          C.  PHASE II - FABRICATION AND EVALUATION           7
          D.  PHASE III - DELIVER AND DEMONSTRATION           8

V.        INSTRUMENT                                          9

          A. GENERAL
             1.   Sampler and Analysis Concepts                9
             2.   Description of the Prototype Instrument      13
          B. LEAP SAMPLER                                      16
          C.  ION-SELECTIVE ELECTRODE                          20
          D.  INTERFACE SYSTEM                                 20

              1.   General Function                             20
              2.   Cell Design                                  26
          E.  BACKUP  FILTER                                    29
          F.  INLET  IMPACTOR                                   31

VI.       OPERATION                                           34

          A.  GENERAL                                          34
          B.  EXPERIMENTAL  TESTS                               34
              1.   Maintenance-free  Operation                   34
              2.   Suspended Nitrate Measurements               36
              3.   Temporal  Variations  of Suspended  Nitrate     38

VII.      REFERENCES                                         41
          APPENDIX  A                                         42
          APPENDIX  B                                          44
          APPENDIX  C                                          48
                                   11

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                          FIGURES
1     Nitrate Detector System                                  10
2    Schematic of Nitrate Monitor with  Cascade  Impactor        14
3    Physical Layout                                          15
4    Schematic of Leap Sampler                                17
5    Leap Collection Efficiency                               18
6    Solenoid Valve Interconnection Diagram                   22
7    Program Valve Diagram                                    24
8    Switching Circuits Design                                25
9    Cell Arrangement                                         27
10   Cell Response                                            30
11   Schematic Cutaway View of Impactor                       32
12   Stage Calibration Curves                                 33
13   Filter                                                   35
14   Temporal Variations                                      40
                              IV

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                           TABLES
1     Summary of Data from NASN and Contributing State        5
     and Local  Networks
2    Valve Position                                         23
3    Flow Rates                                             26
4    Unit Test Parameters                                   29
5    Results                                                37

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                              SECTION  I

                             CONCLUSIONS

      The results of this program indicate that a  practical  system for
automatically sampling and analyzing  for  suspended nitrate  can  be  suc-
cessfully implemented.

      The prototype nitrate monitor demonstrated adequate sensitivity to
meet the 1-100 yg/m3 concentration range  specifications.   Field results
                                       3            3
obtained over a range of about 1.7 yg/m  to 35 yg/m  were consistent with
high-volume measurements taken as reference.   The collection efficiency
of the LEAP sampler was about 80%, as expected on the basis of  the manu-
facturer's design characteristics.  The monitor results,  including a back-
up filter, averaged about 80% of the high-volume results.  The  difference
is believed to be due to the loss of large-diameter, nitrate-containing
particles in the monitor intake system.

      The sensitivity of the monitor at the lowest concentrations ob-
served indicates that the monitor should be able to follow concentrations
                      o
of the order of 1 yg/m  with a time resolution of 1 hour or less.
                                  3
Continuous measurements at 15 yg/m  and above appear reasonable.  Since
nitrate  formation and removal dynamics must be understood before we are
able to  develop optimal control programs, this instrument should become
a valuable scientific tool for the investigation of the fate of nitrogen
oxides.

      Further  field operations need to be carried out to gain a fuller
understanding  of the  ultimate sensitivity and  time resolutions of the
instrument, and  to characterize better its accuracy and precision.

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      The instrument concept  used  in  developing  the continuous nitrate
monitor is very general.   By  introducing  appropriate means of analysis,
other species, both anionic and  cationic,  can  be monitored in a device
of similar characteristics.

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                              SECTION  II

                           RECOMMENDATIONS
1.     The present prototype,  preferably without the  inlet-mounted  cascade
      impactor, should be used to study the dynamic  behavior of atmos-
      pheric nitrates.

2.     The prototype could be  improved by the following:
      a)  increase reliability through mechanical  improvements;
      b)  simplify operation  as part of mechanical  improvements above;
      c)  increase fine particle collection efficiency of
          the electrostatic precipitation section  of the LEAP sampler
          or using a larger type of LEAP sampler;
      d)  lower the detection threshold by decreasing the collection
          solution volume in  the system, probably  by taking advantage
          of electrode miniaturization.

3.     Additional field experience should be obtained in order to better
      characterize the instrument performance, and to establish a  de-
      tailed basis for improvements.
4.    Analytic schema for other species should  be studied to assess the
      feasibility of extending the concept.  NH.  and S04= ions, for
      which specific ion-electrode analyses are available, appear to be
      excellent choices for such extension.

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                             SECTION III

                             INTRODUCTION

      Nitrate in atmospheric particles probably represents the atmospheric
end product of the nitrogen oxides produced in combustion processes.   The
original sources of nitrogen oxides and the intermediate chemical  steps
are dynamic processes which vary not only from day to day but also during
the course of a single day, due to automative traffic flow, solar  radia-
tion, etc.  A useful tool in studying this dynamic process is a real-
time nitrate monitor.  At present, almost all data on suspended nitrate
concentration has been collected by the National Air Sampling Network
(NASN).  These data were produced by the colorimetric analysis of  the
warm water extract from 24-hour, high-volume filter samples.  Hence,  from
this data the finest time resolution on the behavior of suspended  nitrate
is day-to-day variations.

      The one-day average concentration levels of suspended nitrate range
from much less than 1 ug/m3 to well over 10 ug/m3.  Summary data from
the NASN are presented in Table 1.  The particulate-bearing nitrate is
in the  fine particle size range.  Data of Lee and Patterson  -'indicate
that the particle size is approximately 0.4 pm  (mmd).

      The approach  taken in developing a nitrate monitor  is as outlined
below.  Suspended atmospheric particulate is  sampled by use of a com-
mercially available air  sampler (Environmental  Research Corp., LEAP Model
3440).  LEAP samplers are designed  to  concentrate by a  large  factor, on
a  continuous basis, the  particles  in  a large  volume of  air  into a small
volume  of solution.   In  this approach  aqueous collection  solution is used
and  the highly  soluble nitrate  is dissolved.  Then, the nitrate concen-
tration of  the  resulting solution  is  analyzed with a nitrate  ion-selective
electrode technique using commercially available  electrodes  (Orion Re-

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                                               TABLE  I

                             SUMMARY  OF  DATA  FROM  NASN  AND  CONTRIBUTING
                                      STATE AND LOCAL NETWORKS

                                          (Values  in yg/m  )
                                           Urban
Non-Urban
       Pollutant


Suspended Particulates

Nitrates

Nitrogen Dioxide (gas)
No. of
Stations
217
132
47
Arith.
Average
102
2.9
141
Max. Station
Average
254
13.5
333
No. of
Stations
30
29

Arith.
Average
38
1.3

Max. Sta
Averagi
79
2.5


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search).  The nitrate concentration of the solution is  then  related back
to the suspended atmospheric nitrate concentration through  the operating
parameters of the system such as, sample air flow, solution  volume, and
time.

      The principle design task in the program was the  design and fabrica-
tion of an interface system between the LEAP sampler and the nitrate ion-
selective electrode.  This system incorporates the functions of solution
handling, timing, calibration and sampling mode.   In the following task
evaluation of the system was performed.  The design specifications for
the monitor require automatic measurements of atmospheric nitrate concentra-
tions from 1  to 100 yg/m  with an analysis time of one  hour or less.  The
monitor designed and fabricated in this program successfully meets these
specifications.

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                              SECTION IV

                         DISCUSSION OF PROGRAM

A.    GENERAL

      The development program was divided into three phases, viz.
            Phase I - Design
            Phase II - Fabrication
            Phase III - Delivery and Demonstration

B.    PHASE I - DEVELOPMENT AND DESIGN

      The Phase I activities were directed toward gathering background
performance data on the LEAP sampler and the nitrate ion-selective electrode.
Also criteria for sampling and calibration modes were established.  An
initial  total design of the prototype instrument was generated and presented
for Project Officer approval in an informal  interim report and oral  presenta-
tion.

C.    PHASE II - FABRICATION AND EVALUATION
      Following Project Officer approval of the initial  design, fabrication
of the instrument was implemented.  Following fabrication the instrument
was operated to determine suitable operating parameters  such as flow rates,
solution concentrations operation mode times.  Also, preliminary sampling
of atmospheric air was performed.

      In the course of this evaluation a problem was observed, namely air
bubbles attached to the sensing surface of the nitrate ion-selective electrode.
When this happened data were lost unless the electrode was removed from the
sensing cell and the gas bubble removed by washing the sensing surface with a

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jet from e wash bottle.   The scope of work was  increased  to  eliminate
this problem and also to modify the instrument  for 7-day  operation  including
the placement of a coarse screen and cascade impactor U7 urn,  cutoff)  at
the air sample inlet.

      Additionally, a series of 10 comparative  tests  of  the  nitrate monitor
with the high-volume samplers were included and performed in the  increased
scope of work.

D.    PHASE III - DELIVERY AND DEMONSTRATION
      After completing the Phase II Fabrication and  Evaluation,  the  nitrate
monitor was delivered to the EPA and operation of the prototype  was  demonstrated.

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                               SECTION V

                              INSTRUMENT

A.    GENERAL

      1.    SAMPLING AMD ANALYSIS CONCEPTS

            The concept behind the design of this monitor is the concentra-
tion of the particles from a large volume sample of ambient air into a very
small volume of solution.  The very soluble nitrate compounds in the particles
are readily dissolved.  The resulting solution is then analyzed by a nitrate
ion-selective electrode.    Figure 1 depicts a block diagram of this process.
The LEAP sampler performs the functions of air sampling and concentrating the
sampled aerosol into a collecting solution.  The interface provides control
for two sampling modes and two electrode calibration modes.  The electrodes
used are a nitrate ion-selective and a fluoride reference electrode.  The
mil li voltmeter measures and displays the electrical potential difference
between the nitrate and reference electrodes.

            The general relationship between the measured nitrate concentra-
tion in solution and the suspended nitrate in the atmosphere is given by the
following general  relationship:
v.'here
      C is the atmospheric nitrate concentration
      c is the solution nitrate concentration
      v  is the solution volume
      v  is the sampled atmospheric volume
       a
                                         REGION  HI LIBRARY
                                         ENVIRONMENTAL PROTECTION AGENCY

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       ATMOSPHERIC
       PARTICULATE

          NITRATE
           LEAP

         SAMPLER
         INTERFACE
        	i	

        ELECTRODES
            ..i.
        MILLIVCLTMETER
                     J
       SIGNAL CUT PUT
            •  TO
           CE'.'7 RATION
Figure 1.  Nitrate Detector System.
             ID

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            This monitor has two sampling modes, continuous and recircula-
tion.  In the continuous mode, solution is passed only once through the
system, and in the recirculation mode, solution is recirculated for a fixed
time period.

            For the continuous mode of operation, Equation (1) is rewritten
in terms of the flow rates, viz.,

                                C = c{j.                                 (2)

where
      Q is the air sample rate
      q is the solution flow rate
If the threshold of the nitrate ion-selective electrode is taken at ~5 x 10"
molar and if the air sample rate and solution flow is taken at -600 Jl/min and
~3 ml/min respectively, then the threshold sensitivity of the detector is
-15 yg/m .

            For the recirculation mode of operation, Equation (1) is rewritten
in terms of air sample rate and sample time (t), viz.,

                                C = COT

If the operating parameters from the above calculation are used with 60 ml of
recirculation solution and a sample time of 60 min, then the threshold
                      3
sensitivity is ~1 yg/m  .  Mote howe'
achieved by a longer sampling time.
                      3
sensitivity is ~1  yg/m .   Mote however  any threshold  sensitivity may be
            For both modes, the higher limit of detection is four decades
higher than threshold, due to the four decade range of the nitrate electrode.
                                  11

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            The electrode measurement is the potential  difference between


the nitrate and fluoride ion-selective electrodes.   At  operating conditions


the potential  of the nitrate ion-selective electrode is given by:
                      El  • Eol
and at the fluoride electrode by,
where
      E  = reference potentials
             = Nernst constant (-59 mv/decade)
      [NO"] = nitrate concentration
         O


      [F~] = fluoride concentration





The millivolt meter reading (E) is the difference between these two potentials,


viz.,
           AE = E, - E9 = AEn - S-^F-  log [NOl] - log [F~]
                  I    f~     U      r           O
or
                                  o o DT     [NO!
                        AC   AC    2.3r)RT ,   L  ;
                        AE = AE  - 	F— log 	
                              0      r       r i-~ -
                                 12

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            Rearranging  the  last  equation  we  see  that  the  nitrate and
fluoride concentration  ratio is actually measured,  i.e.,
                      [NC]
                            _  exp
(AE -AE  )
                                            o
                                        2.3nRT
This relation also holds for the ratio  of the  mass  of nitrate  ion  and
fluoride ion in the system.   The collecting  medium  used  in  the monitor
contains fluoride ion of known concentration,  sufficiently  large that the
small amounts of fluoride ion or cations  that  tie up fluoride  ion  present
in the atmosphere will  not significantly  change the concentration.   The
solution used in these experiments contained 10  molar  fluoride ion
concentration.

            Changes in the collection medium volume due  to  evaporation
or dilution from atmospheric condensation over the  collecting  plate will
not affect the analytic results.

      2.    DESCRIPTION OF THE PROTOTYPE  INSTRUMENT

            In final form, the prototype  nitrate detector has  plumbing,
valving and timing devices to permit sampling in either  the continuous
mode, or more importantly in terms of sensitivity,  in the recirculate mode,
Provisions exist for calibrating the ion-selective  electrode by injection
of two  levels of calibration solution either automatically or  manually.
Provision is made for stablizing the temperature of the  test solution  by
a temperature sensor controlling arc immersion cooler in the cell  and
for  eliminating  nonhomogenetics by stirring the solution in the cell.
The  liquid  level  sensor/controller is provided to  prevent the system
from drying out  due  to  evaporation while operating  in the recirculate
mode.   A  schematic  of the monitor showing the  various sub-systems  is
shown in  Figure  2.   A pictorial layout is shown  in  Figure 3.  A
descriptive  list of  specific  components  is  presented  in Appendix A.
                                 13

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                                  Air  In
                                                             Cascade  Impactor
.iquid In

       Temperature
       Controller
          Digital
      pH/mv  Meter
       Sensing  Cell



       Test  Solution  —









-


I

1

                                                           Leap  Sampler
                                Liquid  Out -*l
                                                             Freezer
                                                    Liquid Level
                                                    Controller
                                                         Liquid Out
Figure2
                                  Schematic of Nitrate Monitor With  Cascade Impactor

                                             14

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jr-jr—
IN
              OUT
        Control
           &
        Output
        Module
                                Make-up Solution
                                   Two Stage
                                   Cascade
                                   Impactor
                                          - Leap
                                           Sampler
                              y$h Voltage
                              Wy   V.
                                 r      i
                                                         Collection Solution
                                                                      ,
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B.    LEAP SAMPLER

      The performance characteristics  of the LEAP  sampler  determine  the
sampling properties of the Nitrate Detector.  LEAP samplers  were  developed
several  years ago to collect biologically active particles from the
atmosphere.  A schematic of a LEAP sampler is shown in Figure  4.   During
sampling, ambient air is drawn into the sampler through the  top as shown.
The large suspended particles in the sample are impacted near  the axis of
the rotating collection disk.  Within  the instrument,  the  sampled air is
deflected to flow radially outward between the grounded rotating  collection
disk and the high voltage plate.  The  sample air is drawn  through the ring
of corona needles which emit a continuous negative corona.  Suspended particles
are charged passing through the corona field.  The charged particles are
then precipitated onto the collection  disk by the electrostatic force due
to the electric field existing between the high voltage plate  and the
grounded collection disk.

      The peristaltic liquid pump supplies a small flow of collection
solution onto the center of the rotating collection disk.   Centrifugal  force
spreads the liquid out into a thin film.  This thin film is the collection
surface for the electrostatically precipitated particles.

      The particular LEAP sampler used in this program (ERC Model 3440)
has adjustable air sample rates from 0-1.20 m -min" ,  liquid flow rates  from
0-10 ml-min"  and an applied voltage from 0-20kv.  Particle collection efficiency
is a function of  particle size, applied precipitation voltage  and flow rate
as shown  in Figure  5.    We found it convenient to operate at  an  air sample
rate of 600 liters per min with an applied  precipitator voltage of about
15 kv.  To avoid  evaporation of solution on the collection plate  a minimum
solution  flow of  about 3 to 4 ml-min"  was  found necessary.  This provided  a
reasonable collection efficiency for the particle size of interest, i.e.,
                                   16

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                 A',R
                                  COLLECTION
                                  DiSK

                                    STATIC  PICKUP

                                  DRIVE MOTOR
                                       ...GolD PUMP
c.., r:'c- uf 1ZV? s£.r.?lsr (after £.
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100
                         FRECIPITi-CR VOLTAGE: 15KV
                              0.3 1.0       2.0
                     RTrCLE SIZE, MICRONS
   LEAP collection etflciency ,*fter BUC
   1969-1970).
                      Figure  5
                         18

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-0.4 ym.   Further discussion on collective efficiency is presented in
the section on results.

      The LEAP sampler is a very poor collector of gases.   This is shown
by calculation  in Appendix B.   For this reason, the Nitrate Detector is
not expected to be affected by  such gaseous interferences  as NCL.
                                 19

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C.      ION-SELECTIVE ELECTRODES

       As stated earlier in the general  description of the instrument,
a nitrate ion-selective electrode is used to sense the nitrate ion
concentration of the resulting collection solution and a fluoride ion-
selective electrode is used as a reference electrode.   The nitrate and
fluoride ion-selective electrodes are Orion Research Models 92-07 and
94-09 respectively.  The ion-selective electrode sensing was selected for
simplicity and ease of application over the more procedurally complicated
colorimetric procedures of nitrate analysis.

       A manual method using these electrodes has been investigated for
measuring suspended nitrate concentration.  The results of this study are
discussed by Williams, et al., 1972.  In the course of this study it was
shown that the possible interferences due to Cl", Br", l", V0~ and Se04 may
be eliminated by precipitation out of the measurement solution by adding
silver fluoride.   As  indicated by Driscoll  and  Forney, 1973, and Williams, et al.,
1972, Br" from automobile exhaust is the most likely  interference.  As a
precaution the collection solution has been doped with a  concentration of
10~4 molar AgF.  Since the nitrate  ion-selective electrode selectivity
constant  K   = 0.13 for Br' versus KX = 1  for nitrate, and AgBr"  is virtually
insoluble; the Br" interference  is  removed  from at  least  equal concentra-
tion of  Br"  and  NO".

D.      INTERFACE SYSTEM

        1.     GENERAL  FUNCTIONS

              The functions  of the interface system is the following:
              a.     convey liquid sample  from the  LEAP sampler to
                    the electrodes
              b.     control  the sample modes
                                    20

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             c.     control  the calibration  modes
             d.     program  the flush  cycle  on recirculation  sampling
             e.     thermally stabilize the  electrode measurement
             f.     control  volume of  recirculation solution
             g.     mix the  sample solution

             A schematic of the elements of interface system is shown in
Figure  2.     Figure  6 shows a solenoid valve interconnecting diagram of
the system connecting the LEAP sampler with the electrode in the cells.
When the Detector is operating in the  continuous sampling mode solution is
pumped out from the LEAP sampler through V4 to the cell.  Solution from the
cell pumped through V2 to the LEAP sampler.  Any decrease in recirculation
solution volume due to evaporation is sensed and deionized water is added
through V9 to maintain constant solution volume.   At the end of a sample "
cycle the recirculation solution is flushed out and replaced by fresh
collective solution.  The flush is initiated either automatically or
manually.  Collection solution flows  under gravity through V8 to the cell.
Solution from the cell flows out through the overflow indicated.  Fresh
solution is also pumped into the LEAP sampler through VI.  (It is necessary
to maintain a continuous flow on the collection plate of the LEAP sampler
or liquid will be splashed  about shorting out the applied high voltage).

             During calibration, calibration solution flows through either
V5 or V6 to the cell.  Solution  in the  cell  flows out the indicated over-
flow port.

             The valve position  for each function is shown in  Table 2.
The method of controlling the  solenoid  valves  is  shown  in Figure 7.
Figure  8  shows the  wiring schematic for  the  solenoid  valve switching  and
timing.
                                  21

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            Gravity Flow
   2
I  v
i.—_._
     Gravity  Flow  \
   L.
                                                                     -
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                                TABLE  2
                            VALVE POSITION

                               Continuous
                       V      V     V     V     V     V          V
                       V3     V4    V5    V6    V7    V8         V9
Open      X                  X
Closed           XX            X     X      x     X

                              Calibration A
          V1    V2     V3     V4     V5    V6    V7    V8         V9
Open      XXX
Closed          X            X            X     x     X          X

                              Calibration B
          V1    V2     V3     V4     V5    V6    V7    V8         V9
Open      XX                  X
Closed          X            XX           XX          X

                              Recirculate

          V1    V2     V3     V4     V5    V6    V7    V8         V9
Open            XX                              (On Demand)
Closed    X            X            X     X     X      X

                       Flush  Between Recirculation
          V1    V2    V3     V4     V5     V6     V7    V8         V9
Open            XX                        X
Closed    X                        X      X     Y                X
                                   23

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C A !••! T I M E R
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         ,  . . .„_. . ._  . _

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                  figure  7   Program Valve Diagram
                                                         "T"
                                24

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                                     Figure  8   Switching Circuits Design
J^—'.
 I.	'.
                      -e-
                   ©     o
                      LINE
                                                                              TIMCR'Z
                                                                                       LICUIO

                                                                                       ICVCL

                                                                                      COHTPOLUEB
                                                                                            NITRATE MONITOR SWITCHING DIAGRAM

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       2.    CELL DESIGN

             The cell was designed to hold the following:
             a.    solution to be analyzed
             b.    nitrate and fluoride electrodes
             c.    temperature sensing probe
             d.    liquid level sensing probes
             e.    cold finger
             f.    magnetic stirring bar
These elements are shown schematically in Figure 2.    The cell was
machined from lucite as shown in Figure 9.    With all components installed
the solution capacity of the conical cavity is about 45 ml.  The conical
cavity was chosen to provide a small solution holding volume while providing
space to accommodate all the required elements plus provide a sensitive
liquid level detector for sensing small changes in solution volume.

             The volumetric flow rates through the cell are listed in
Table 3.

                                TABLE  3

                               Flow Rates
       Operating Mode           ml min"             Method

       Continuous                 0-12             Leap Pump
       Recirculate                0-12             Leap Pump
       Calibrate                 15-20             Gravity
       Flush                      -25              Gravity

             An effort was made to give the solution cavity the
characteristics of an ideal stirred vessel in which entering solution is
dispersed instantaneously throughout.  Assuming an ideal stirred vessel
                                26

-------
Temperature
Probe
Fluor ide--
Electrode
Liquid Level
Controller
                   Liquid Inlet
                   and Vent
                   Top Flange
                            Nitrate
                             Electrode
                  Cold Finger
        Overflow

[




1
!
Mm
i
!
i
!/'
/
/
1 1
i i
[

1
1
1
1
L
/
/




k

—
1
1
1
1
1 1 I
1 ll 1
" ,'
ii
Si1 1 f«
!> 1
-f1 1
~\
\
\

\
i
i .. . i.
                                    Figure 9 Cell Arrancerv.ent
                                        5
                                      SCALF
7     K5     i C
                                           27

-------
of volume V through which a solution is slowing at rate Q, one has the


relationship [4].
                                         t/T
             [N0~] = ([N0~]o - [N03]i) e     + [N03]i
where [NO"] = [NOJ  at t = 0 and   = V/Q the solution residence time.
         o       o u

Moreover, if the concentration of NOZ within the vessel  is measured with


a nitrate and fluoride reference electrode operating within the Nerstian

               -5      2
region (~5 x 10   - 10   M N0~) where the electrode voltage response is
                             O

given by
                         AE - AEQ -    ln
                                          [NO]
These equations can be combined to yield:
AE - AE.
        RT/nF
                = -In
                    [NOji
                                                t/i
                                             + 1
- In
To check the validity of this equation, two tests were conducted using a


gravity feed NO" solution to the flow-through unit.   The results of both


tests are shown in Figure 10,  where the parameters  of the system are


summarized in Table  4   below.
                                  28

-------
                                TABLE 4
                          UNIT TEST PARAMETERS

                               AE   =  73 mv
                                 o
                             RT/nF  =  26.9
                                 T  =  38.5°C
                                 n  =  1
                              [F~]  =  10~2 M
                                 V  =  44 cc.

             As can be seen in Figure  10  the flow-through unit response
conformed closely to that of a well-stirred vessel  (solid lines).   The
small drift in the data relative to theory was a result of a decrease
in head above the unit as the experiment progressed.   From this result
the cell behaves as a well-stirred vessel, hence the cell response time
for an e-fold time chance to a step change in concentration is simply V/Q.

E.     BACKUP FILTER

       The design of the prototype instrument incorporated the provision
for using a backup filter on the LEAP Sampler.  A high volume filter may
be installed to filter the exhausted gas from the LEAP sampler.  Originally
a full-size high volume sampler sheet was used.   However, due to the small
quantity of nitrate particles which penetrate the sampler relative to the
background of nitrate or filter paper blanks, the effective filtering area
was reduced to a diameter of about 7 cm.   This provided a more favorable
signal to raise ratio.  Data were gathered on the efficiency of the LEAP
Sampler for atmospheric suspended nitrate.  This data is presented in the
Section IV.
                                  29

-------
                                                    "T	i     I  	i
      1	I  _ L	JL	L	
Figure 10. Cell Response

-------
F.     INLET IMPACTOR

       A contract requirement was the installation of our impactor with
a particle cut-off of 7 ± 2 urn.   Upstream of the LEAP sampler inlet,a BGI-30
(BGI-Incorporated) high volume cascade impactor was installed to remove  the
particles greater than approximately 7 ± 2 ym.   The BGI-30 is a four stage
impactor  (Figure 11)   with particle penetration characteristics as shown
in Figure  12  for a sample flow rate of 0.85 m -min  .   Since the LEAP
sampler is operated at 0.60 m -min" , the particle size  penetration was
assumed to be approximated by increasing particle size by the ratio of the
flow rates.  For example the 50% penetration of the second stage (Figure 12)
is taken as:
             Particle size = 3.8 ym  -85 (m -mm
                                   x .60 (m -min"1
Since this is within our tolerance of 7 ± 2 ym, the impactor was used with
the first two stages installed.   Actual penetration was not measured.

       In conventional  impactor operation, the collection stages are greased
to decrease re-intrainment of impacted particles.   However, in our operation
where it was required to measure the total nitrate in the sample stream, the
stages were not greased because the grease interferred with a subsequent
manual analysis (ion-selective electrode method) for nitrate on the collection
stages.
                                 31

-------
OJ
                                   Filter
IrnpacMon
Plato
                                                                       Tie Rod
                                                                       Nut
                                                                       Flowmefr©r
                                                                       Tap
                       Figure 11  Schematic Cutaway View of Impactor

-------
          100
00
OJ
                                    345

                                    SCLE  SIZE  -

                        Figure 12 Stage Calibration Curves

-------
                               SECTION VI

                               OPERATION

A.     GENERAL

       Two types of experimental tests were made.  The first was a test
of long-term maintenance-free operation.  The second was a set of
suspended nitrate measurements using the prototype detector along with
three high-volume samplers run in parallel.  During the latter set of
.tests, the collection efficiency of the LEAP sampler was measured as well as
the difference between the prototype measurement and the high-volume sampler
measurement.

B.     EXPERIMENTAL TESTS

       1.    MAINTENANCE-FREE OPERATION

             One objective of this test was to obtain 7 days of maintenance-
free operation.  The  prototype instrument was set-up to sample in the
recirculate mode.   In this mode, the  instrument  recirculated collection
solution  for 105 minutes, then automatically flushed out the system (15
minutes)  and initiated  another 105 minute  recirculation sample cycle.
Every six hours, the  analyzer was automatically  calibrated with two levels
of calibration  solution.  A  liquid filter was installed at the liquid output
from the  LEAP sampler to  trap the preponderance  of insoluble particles
collected by the sampler.  This  filter  is  depicted in Figure 13.

             The  test ended  after almost  four days of continuous operation.
Termination was due to  particles clogging  the liquid  filter.  Also  the
 liquid  level controller failed  about  the  same time, due to  fine particles
collecting  on  the  grounded electrode  of the  sensor probe,  thus  insulating
                                      34

-------
          Flow Direction
                            Glass
                            Sand
                           Glass Wool
Figure 13    Filter
                        35

-------
this electrode from the level  sensing system.   It was  also  observed that
the tubing of the peristaltic  pump in the LEAP  sampler had  begun  to leak.
(This tubing had considerably  more than four days of testing and  this
failure was not a direct result of this test.)

             During this test  period, an old five-story building  across
the street from the test-site  was being demolished.   This produced very
heavy dust concentrations which made these four days an extremely severe
test of the instrument.  Under ordinary conditions,  a much  longer uninter-
rupted test period could have been expected.

       2.     SUSPENDED NITRATE MEASUREMENTS

              A  series of ten, 24-hour  tests were  run  in which the  ambient
atmosphere  at our  Cambridge facilities was  sampled  for suspended nitrate
concentration.   The  prototype Nitrate  Detector was  operated with inlet
impactor  and  backup  filter  installed as  explained in  Section V.

              The referee measurement consisted of three  high-volume  sampler
measurements  made  simultaneously and in  proximity to  the sample  intake  of
 the prototype detector,  which  was a  conventional  hi-vol  shelter.   There
were about 6-8 meters  of 10 cm diameter flexible hose connecting the
 detector to the sample intake.   All  analyses  for nitrate were  performed by
 selective ion electrode techniques.   All filter  and impaction  stages were
 extracted and analyzed by  techniques similar to  those reported by  Williams
 et al.(2)  Nitrate collected  by the LEAP Sampler was analyzed  automatically
 in the detector cell.

              The results are presented in Table 5.     Detailed data for
 individual tests are presented  in Appendix C.   In  reporting the results,
 the impactor  catch  is summed with cell  collection  and reported as the
 "Detector  Results."  These values are summed because the  impactor is not  a
                                     36

-------
                                              TABLE  5
                                               RESULTS
      Te'st    "~  Hi-Vol    ,     Detector Results  Total Catch   Impactor3Catch   Backup Filter     Sample
       No      Results  (pg/m3)          (ug/m5)        (yg/m3)        (yg/mj)       Catch (yg/m )   Cycle Time
             13.3  Mean  Std.Dev.
             12.5  13.3     .7
             14.0
                          7.1
8.3
                                                       0.6
                                1.2
                                                                                    24 hr.
              5. I
              4.9   5.0    .1
              4.9
                          4.3
4.7
                                                       0.4
                                0.4
                             24  hr.
              4.7
              4.3  4.6    .2
              4.7
                           3.7.
4.4
                                                       0.4
                                0.7
                                                                                    24 hr.
00
•—I
4.4
4.5  4.7    .4
5.2

1.7
1.4  1.7    .3
2.0
                                         3.1
                                         2.1
3.8
2.7
0.1
                                                                      nil
                                                                                      0.7
                                0.6
                                            1.75 hr.
                             1.75 hr.
              3.0
              2.7  3.2    .7
              4.0
                           1.5
 2.0
                                                        0.1
                                0.5
                                                                                     1.75  hr.
              7.1
              6.7  7.1    .4
              7.6

              35. 5
              24^6  35.5  10.5
              45.7
                           1.9
                           4.1
 2.5
 4.9
                                                        0.2
0.6
                                0.6
                                                                         0.8
                             1.75 hr.
                                             1.75  hr.
        10
 9.9
 3.9  4.5     .5
 4.7

 1.7
 1.7  1.8     .2

 2.1
                                         3.7
                                         1.8
 4.6
 1.8
 0.4
                                                                      nil
                                                                                       0.9
                                             24  hr.
              not used        24  hr

-------
necessary element for the operation of the Nitrate Detector,  and it
is assumed that the large particles caught in the impactor would be
readily caught by the LEAP sampler, then analyzed automatically by the
cell if the impactor was not installed.  The sum of the "Detector Catch"
and the backup filter catch is reported as "Total Catch".

              For five of the ten days of testing the detector was
operated continuously in recirculation mode for 24 hours.   In the
remaining  five tests the detector was operated in two-hour cycles with
recirculation sampling  for  1.75 hours and  flush  for 0.25 hours.  The
average  of values  for the 2 hour cycle  is  reported as  the 24-hour  value.
The operation mode  for  each test is  indicated  in  Table 5   under  "sample
                                      •
cycle  time."

              The results from these  tests  indicated  that  the  Nitrate
 Detector performs  well.  The  "total  catch" on  the average  was about 80%
 of the high-volume sampler  measurement, with moderate  scattering.   The
 failure to account for all  nitrate is thought to be  due,  in  part at least,
 to the loss of nitrate present on  large particles in the  sampling line
 connecting the Detector to the sample inlet.  Variations  in  the quantity
 of nitrate on large particles and/or variations in the large particle
 size distribution could result in  the variability of the  "total catch"
 results relative to the hi-vol determination.   The "detector results-
 are about 81% of the "total catch".  This result is as expected due
 to the  collection efficiency of the LEAP  sampler and  previously reported
 particle  size (mmd) for nitrate bearing particles in  the atmosphere  - .

         3.    TEMPORAL  VARIATION OF  SUSPENDED  NITRATE

               During  the test  period temporal  variations of suspended
  nitrate were measured.   These  data  were  collected  in  tests where  the
  Nitrate Detector  was  operated  with  a  1.75 hour  sample recycle  time
                                    38

-------
(see Figure 14)-   These data are important,  since it is the first data
we know of which shows the temporal  variation of suspended nitrate within
a 24-hour period, and it indicates that this  prototype instrument is
capable of obtaining the dynamic data needed for experimentally
investigating models for the fate of oxides of nitrogen in the atmos-
phere.  Since only the cell collection fraction of the suspended nitrate
is shown  (the impactor collected the large particle fraction, ~7 um)
care should be  used  in theorizing with the data presented.
                                    39

-------
  lr>  f,
   F 5:-
  UJ  :
  t-
  
-------
                              REFERENCES


1.    Lee, R.F.  and R.  K.  Patterson,  Atn.  Environment.  1969,  Vol.  3,
     pp.'249-255.

2    William, D.,  J.  Driscoll, C.  Curtin  and R.  Hebert, "Methods  for
     the Rapid and Accurate Measurement of Nitrate and Sulfate in
     Atmospheric Particles", Final  EPA report on Contract No.  68-02-0564,
     EPA-650/2-73-050, December,1973.

3    Driscoll, J.  and L.  Forney, Chapter 8, Analytical Methods Applied
     to Air Pollution Measurements, Stevens and Herget  (eds.),  Ann
     Arbor Science Publisher, Ann Arbor, 1974.

4.   Perry, J.H.  fFd.l. Chemical Engineers' Handbook   McGraw-Hill (1963)
                                    41

-------
                             APPENDIX  A
                         LIST OF  COMPONENTS
Component

Electrode, Nitrate
Electrode, Reference, Fluoride
Electrode Meter (pH/mv)
Cell and base
Lead Sampler
Cascade  Impactor

Peristaltic pump  silicone

  rubber  tube

Liquid Level  Controller
Liquid Level  Controller Probe
Temperature  Controller
Temperature  Controller Probe
 Immersion Cooler
 Refrigerator

 Pump
  S
  Sl
  S2
  S3
  Magnetic Stirrer
  Stirring Bar
  14  Relays [K   K]
             Description

Orion Model  92-07
Orion Model  94-09
Orion Model  701
Fabricated from Plexiglass
Environmental Research Corp. Model 3440
BGI-30 High Volume Cascade  Impactor
2 stages  (No. 1 and 2)BGI Inc.Waltham.Ma.
Silichem  1/8" Bore, 1/4" O.D.,
New  Brunswick
Scientific  International  Inc., New
Brunswick,  New  Jersey.
Dyna-Sense  Controller,  Model  7188
Dyna-Sense  Sensing  Probe  Cat.No.  7186-12
Versa Therm Model  2158
Versa Therm Liquid  Immersion  8446
 Fabricated from Glass
 1.5 ft3 Sears  Cat.  No.  3467370N,  Sears
 Roebuck & Co.
 Oscillating type, Model 7103-10 cap.  1/2
 GPM at O'head, Cole Palmer Inst.  Co.,
 Chicago, II.
 4 circuit Egal BL 340 Timer, 6 hr.
 Daton 2E026, Prog. Time Control  (Variable
 On-off 4/hr to I/day in 96 steps)
 SPST  Switch
 SP3T  Switch
 SP2T  Switch
 SPST  Switch
 Fabricated using  240 Kpm  sychronour  motor
 3/8"  Dia x 3/8"
  Daton,  4 x 809,  115  V  SPOT Relay
                                   42

-------
                            APPENDIX A
                  LIST OF COMPONENTS (CONTINUED)
Component                                    Description

9 Valves [V  - V ]              Asco Solenoid Valve, Cat.  No.  836015
Connecting Tubing               Teflon, 1  mm Dia.
4 Reservoirs                    2 Gal and 1/2 Gal  Plastic Carboy
Cabinet                         Bud CR 1737
                                   43

-------
              APPENDIX B




ESTIMATE OF ABSORPTION IN LEAP  SAMPLER
                   44

-------
     The  geometry  of  the  LEAP  sampler  is  schematically  shown below.
     We shall  examine the absorption from the gas stream entering at the
center and flowing outward to the edge of the dish.   This portion of the
inlet gas will exhibit maximum absorption.  We will  neglect any rotational
effects due to the motion of the collecting plate.  Considering an in-
finitesmal annual section at radius, r, from the center, we can write a
material balance for the absorbent species in the gas, for example, nitro-
gen dioxide, as follows:
               FC - F
fc + {£drj  - k 27rr dr [C - C.] = 0
(C-l)
where   F = gas flow rate in cc/min
                                           2
        k = mass transfer coefficient in cm /min
        C = concentration of absorbed species in moles/cc
       C. = equilibrium concentration above liquid

This reduces to:

                        FJJt.-khrCC-C,]

and  can be  integrated  between  any  two radii as:
                                             (C-2)
                                 45

-------
                            dc  -             rdr                    (C-3)
                           C-C  ~     F
                              1          ri
or
The equilibrium concentration of. nitrogen  oxide  is  essentially  zero  so
this simplifies to

                            c2    4
                            ^- e F   2  ]                         (C-5)
                            Ll

     In order to evaluate the expression on  the  right,  we  must  know  the
value of the mass transfer coefficient.   Being conservative,  we assume
the diffusion is mass transfer controlled  (gas side).   This  is  the  fastest
rate feasible, even if liquid-side chemical  reaction  is infinitely  rapid.

     Consider the case of flow over a flat plate.   For  gases  (air),  the
Schmidt number (N  ) is approximately unity,  so  that
                 O w

                            Nsh = 0.6 Re°'5                         (C-6)

                                kr
where   N ,  = Sherwood number = -~-
         Re = Reynolds number =
                                 y
          k = mass transfer coefficient
          r = radius
          D = diffusivity in cm/sec
          p = gas density in gm/cc
          y = gas in viscosity
          V = velocity in cm/sec


                                  46

-------
     Using dimensions,  characteristic  of the  sampler,  at  500  1/min  flow,

the Reynolds number is


                                Re  =  103


so that



                        ^= 6 x (lOOO)0'5  =  19                     (C-7)


                                             2
     For gas, the diffusivity is about 0.1  cm /sec,  so that  for  a total

travel distance (r) of 15 cm,


                     k = 0.12 cm/sec  = 7.2  cm/mi n


Now, returning to Equation C-5, we  find that  the ratio of concentration

from center to edge is
                           ~ = e
and, at
                     F = 500 1/min = 5 x 10  cc/min
we find that


                            C
                             2 ~  -0.01  - ,
                             ~ " e      " '
     This calculation indicates that no significant absorption will  occur

during the passage of the gas through the sampler.
                                   47

-------
                           APPENDIX  C
                       ATMOSPHERIC  TEST  DATA
                             BY  TEST

        This Appendix shows  the  test  data  by  individual  tests.   The
following notations were used:

        B.F. - backup filter to  the LEAP sampler
        S,   = first inspection  stage
        S9   = second inspection stage
        F    = multiplying factor where analysis was
               performed on 1/2 or 1/4, etc.  of filter area.
                                48

-------
   Test No.  1
Date:  (8/21/74)-
Sampling Rate, Sampling Time
(m /min) (min)
Hi Vol A
Hi Vol B
Hi Vol C
Av. Hi Vols.
B.F.
Sl
s2
Cell
1.67
1.47
1.75

0.57
0.57
0.57
0.57
1455
1455
1455

1455
1455
1455
1455
Total
Sampled
, Volume,
(m3)
2430
2139
2546

829
829
829
829
Moles N03
Collected
(y moles)
58.0
48.0
64.0

4.1 -
2.05
1.75
87.0
F
X
9
9
9

4
2
2
1-
Total Moles
(u moles)
522
432
576

16.4
4.1
3.5
87.0
Weight Nitrate
Collected
fog)
32364
26784
35712

1016.8
254.2
217.0
5394.0
Nitrate
Concentration
(yq/m3)
13.3
12.5
14.0
13.3
1.2
0.31
0.26
6.5

-------
  Test No.  2
Date:  (8/22/74)
Sampling Rate,
(m /mi n )
Hi Vol. A 1.27
Hi Vol. B 1.41
Hi Vol. C 1.39
Av. Hi Vols.
B.F. 0.60
S1 0.60
S2 0.60
Cell 0.60
Sampled Moles NO- Total Moles Weight Nitrate Nitrate
Sampling Time, VoTume, Collected F N03 . Collected Concentration
(min) (m3) (u moles) X (y moles) 	 (vjo) 	 (]^J. 	
1425 1810 37.2. 4 148.8 9225.6 5.1
1425 2009 40.0 4 160.0 9920.0 4.9
1425 1980 39.2 4 156.8 9721.6 4.9
4.9 • .
1425 855 1.7 4 6.8 421.6 0.50
1425 855 0.8 2 1.6 99.2 0.12
1425 855 2.1 2 4.2 260.4 0.30
1425 855 54.0 1 54.0 3348 3.9

-------
  Test No.  3
Date: (8/26/74)


Hi Vol.
Hi Vol.
Hi Vol ,

Av. Hi
B.F.
Sl
S2
Cell

Sampling Rate,
o
(m /min)
A 1.27
B 1.47
. C 1.39

Vol.
0.6
0.6
0.6
0.6

Sampling Time,
(min)
1300
1300
1300


1300
1300
1300
1300
Total
Sampled
Volume,
(m3)
1651
1911
1807


780
780
780
780

Moles N03
Collected
(u moles)
31.4
33.4
34.2


2.07
0.56
1.83
41.4

F
X
4
' 4
4


4
2
2
1

Total Moles
N03
(u moles)
125.6 .
133.6
136.8


8.3
1.1
3.7
41.4

Weight Nitrate
Collected
(yg)
7787.2
8283.2
8481 . 6


514.6
68.2
229.4
2566.8

Nitrate
Concentration
4.7
4.3
4.7
4.6

0.66
0.09
0.29
3.3

-------
en
r-o
                                                        Test No. 4

                                                      Date:(8/29/74)
Sampling Rate,
(m /min)
Hi Vol. A 1-42
Hi Vol. B 1.61
Hi Vol. C 1.47
Av. Hi Vols.
B.F. 0.6
S, 0.6
1
S9 0.6
2
Cell 1 0.6
2
3
4
5li

6
7

Total
Sampled Moles NO-
Sampling Time, Volume, Collected
(min)
1425
1425
1425
1425
1425
1425
105
u
ll
u
ll
M
ll

(m ) (u moles)
2023 35.6
2294 41.6
2095 43.6
855 2.3
855 0.02 .
855 0.55
63 2.7
3.3
2.04
2.04
2.04
4.5
5.1

Total Moles
F N03
X (u moles)
4 142.4
4 166.4
4 174.4
4 9.31
2 0.04
2 1-10
1 2.7
3.3
2.04
2.04
2.04
4.5
5.1

Weight Nitrate
Collected
(ua)
8829
10317
10813
577
2.5
68
167
205
126
126
126
279
316

Nitrate
Concentration
/ / 3\
	 	 diq/m )
4.4
4.5
5. 2
4.7
0.68
0.00
0.08
2.65
3.25
2.01


4.23
5.02
3.02 .
       Cell  Av.

-------
                                                       Test No. 5

                                                     Date: (9/3/74)
tn
CO
Sampling Rate,
(m /mi n )
Hi Vol. A 1.29
Hi Vol. B 1.63
Hi Vol. C 1.44

Av. Hi VolS.
B.F. 0.6
S, 0.6
|
l
Sp 0.6
Cell 1 0.6
2
3
4
5
6
7
8
9

Cell Av.
Sampling Time,
(min)
1465
1465
1465


1465
1465

1465
105
ll
ll
ll
II
"
ll
ll
75


Total
Sampled
Volume,
(m3)
1890
2388
2110


879
879

879
63
II
ll
ll
II
It
ll
11
45


Moles N03
Collected
(u moles)
12.6
13.0
16.6


2.0
0.0

0.14
3.9
2.6
2.4
2.3
2.4
2.4
1.3
1.3
0.7


Total Moles
F N03
X (y moles)
4 50.4
4 52.0
4 66.4


4 8.0
2 0.0

2 0.3
1 3.9
2.6
2.4
2.3
2.4
2.4
1.3
1.3
0.7


Weight Nitrate
Collected
3125
3224
4117


496
0.0

18.6
242
161
149
143
149
149
81
81
43


Nitrate
Concentration
(yg/m3)
1.7
1.4
2.0
1.6

0.56
0.0

0.02
3.8
2.6
2.4
2.2
2.4
2.4
1.3
1.3
1.0
2.1


-------
Test No. 6
Sampling Rate,
(m /mi n )
Hi Vol. A 1.39
Hi Vol. B 1.64
Hi Vol. C 1.44

Av. Hi Vols
B. F. 0.6
S1 0.6
S2 0.6
Cell 1 0.6
2
3
4
5
6
7
P
9
10
Cell Av.
Sampling Time,
(min)
1430
1430
1430


1430
1430
1430
105
II
ll
li
ll
"
ll
ll
n
ll

Total
Sampled
Volume,
(m3)
1988
2345
2059


858
858
858
63
ll
II
ll
II .
ll
II
ll
"
ll

\ -" / — / • • /
Moles NO-
Collected
(u moles)
24.3
25.5
33.1


1.7
0.25
0.65
1.38
1.38
1.44
1.08
1.08
1.44
1.44
1.56
1.44
1.56

F
X
4
4
' 4


4
2
2
1
ll
ll
ll
ll
ll
ll
ll
M
II

Total Moles
(u moles)
97.2
102
132.4


6.8
0.5
1.3
1.38
1.38
1.44
1.08
1.08
1.44
1.44
1.56
1.44
1.56

Weight Nitrate
Collected
(yg)
.6026
6324
8209


422
31
81
86
86
89
67
67
89
89
97
89
97

Nitrate
Concentration
(yg/m3)
3.0
2.7 .
4.0
3 2
:
0.5
0.03
0.09
1.4
1.4
1.4
1.1
1.1
1.4
1-4
1.5
1.4
1.5
1.4

-------
  Test No.  7
Date:  (9/9/74)

Sampling Rate,
o
(m /min)
Hi Vol . A 1.39
Hi Vol. B 1.58
Hi Vol. C 1.44
Av. Hi Vols.
B.F. 0.6
S1 0.6
S2 0.6
Cell 1 0.6
2
3
4
5
6
7
8
9
10
11
12

r * 1 1 A . ,
Total
Sampled
Sampling Time, Volume,
(min) (m )
1410 1960
1410 2228
1410 2030.

1410 846
1410 846
1410 846
105 63
H H
n H
n n
n i>
n "
n n
n n
M II
II H
II II
II II



Holes NO.
Collected
(u moles)
56.2
60.2
62.2

2.3
0.42
0.77
2.0
1.3
1.3
1.5
1.2
1.3
1.5
1.9
2.5
2.0
1.8
2.4



F
X
4
4
4

4
2
2
1
ll
M
ll
ll
M
11
II
II
11
II
II



Total Moles
N03
(y moles)
224.8
240.8
248.8

9.1
0.8
1.5
2.0
1.3
1.3
1.5
1.2
1.3
1.5
1.9
2.5
2.0
1.8
2.4



Weight Nitrate
Collected
(yg)
13938
14929
15426

565
52
95
124
81
81
93
74
81
93
118
155
124
112
149



Nitrate
Concentration
(yg/m3)
7.1
6.7
7.6
7.1
0.67
0.06
0.11
2.0
1.3
1.3
1.5
1.2
1.3
1.5
1.8
2.. 5
2.0
1.8
2.4
1 .7


-------
                                                        Test No. 8
                                                      Date: (9/10/74)
cr>

Hi Vol
Hi Vol
Hi Vol.

Av. Hi
B F
U.I •
Sl
S2
Cell













Cell

. A
. B
. C

Vol



2
3
4
5


7
8
9
10
11
12

Av.
Sampling Rate,
I m /mi n \
1.30
1.50
1.35

s.
0.57
0.57
0.57
0.6
0.6
0.6
0.6
0.5
Or
. b
0.5
0.5
0.6
0.6
0.6
0.6


Sampling Time,
(min)
1595
1595
1595

1595
1595
1595
105
ii
ll
ti
II
M

II
II
II
II
II
II


Total
Sampled
Volume,
(m3)
2073
2393
2153

909
909
909
63
63
63
63
52
52

52
52
63
63
63
63


Moles N03
Collected
(u moles)
297
237
397

5.6
2.0
2.6
3.6
2.5
2.4
2.4
2.9
4.0

4.6
3.6
2.9
4.1
4.3
3.1


Total Moles
F NO,
X (u moles)
4 1188
4 948
4 1588

2 U
2 4
2 5
1 3.6
2.5
2.4
2.4
2.9
4.0

4.6
3.6
2.9
4.1
4.3
3.1


Weight Nitrate
Collected
(yg)
73656
58776
98456

696
248
310
223
155
149
149
. 180
248

285
223
180
254
267
192


Nitrate
Concentration
35.5
24.6
45.7
o c n
3b. U
0.76
0.27
0.34
3.5
2.5
2.4
2.4
3.4
4.7
•
5.4
4.2
2.8
4.0
4.2
3.0
3.5,


-------
  Test No.  9
Date:  (9/12/74)
Total
Sampled Moles NO, Total Moles Weight Nitrate
Sampling Rate, Sampling Time, Volume, Collected F N03 Collected
(m3/min) (min) (m3) (u moles) X (u moles) (yg)
Hi Vol. A 1.2 1440 1728 34.0 4 136.0 8432
Hi Vol. B 1.5 1440 2160 34.0 4 136.0 8432
Hi Vol. C 1.3 1440 1872 35.6 4 142.4 8829
Av. Hi Vols.
B.F. 0.5 ' 1440 720 2.7 4 10.9 677
s 0.5 1440 720 0.8 2 1.6 99
s 0.5 1440 720 1.6 2 3.2 201
Cell 1 0.5 1440 720 39 1 39 2418
2
3
Nitrate
Concentration
(yg/m3)
4.9
3.9
4.7
4.5
0.93
0.14
0.28
3.3



-------
                                                        Test  No.  10
en
00
ua i.c . \?/ivii ^j 	 , 	 — .
Sampling Rate
o
(m /mirO
Hi Vol. A 1.39
Hi Vol. B
Hi Vol. C

Av. Hi Vols.
B.F.
Sl
S2
Cell
1.58
1.44


none
0.6
0.6
0.6
Sampled Moles NO, Total Moles Weight Nitrate
. Sampling Time, Volume, Collected F NO., Collected
(mini (m3) (H moles) X (u moles) .... (vg)
1440 2002 13.8 4 55 3422
1440 2275 15.8 .4 63 3918
1440 2074 17.8 4 71 4414

V
used
1440 864 -02 ~0 -0
1440 864 0.2 2 0.4 26
1440 864 25.8 1 26 1600
Nitrate
Con cent rat Jon
(yg/m3)
1.7
1.7
2.1
1.8


~0
0.03
1.8

-------
                                  TECHNICAL REPORT DATA
                          (Please rczd li:sa-.iciit":s • >n ti:c i<.".\ w hctorc cinnr. IDE.VTIFIERS'OPf.' =\'DED TERMS
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                                  07D
                                  07B
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                                  14B
                                                                           £'•-
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-------
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-------