r*1 **»  *.r\«n«*._                  Technical Note
                                       ORP/LV-78-1
RADIOLOGICAL SURVEYS OF IDAHO PHOSPHATE
 ORE PROCESSING—THE WET PROCESS PLANT
                  APRIL 1978
                        s^»
                      A
                    t^lM^f
\
        U.S. ENVIRONMENTAL PROTECTION AGENCY
           OFFICE OF RADIATION PROGRAMS
                US VEGAS FACILITY
             LAS VEGAS, NEVADA  89114

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                                         Technical  Note
                                         ORP/LV-78-1
    RADIOLOGICAL SURVEYS OF IDAHO PHOSPHATE

     ORE PROCESSING—THE WET PROCESS PLANT
                   APRIL 1978
OFFICE OF RADIATION PROGRAMS - LAS VEGAS FACILITY
      U.S.  ENVIRONMENTAL PROTECTION AGENCY
            LAS VEGAS, NEVADA  89114

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                            DISCLAIMER
     This report has been reviewed by the Office of Radiation
Programs - Las Vegas Facility, U.  S.  Environmental  Protection
Agency, and approved for publication.  Mention of trade names or
commercial products does not constitute endorsement or recommen-
dation for their use.
                                ii

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                          ACKNOWLEDGMENTS


     The field conduct of this  project was directed by Joseph A.
Cochran whose present address  is:

          Chief,  Sanitation Branch
          Directorate of Facilities Engineering
          U.S. Department of the Army
          Fort Ord,  California   93941


     This report  has been prepared by Gregory G.  Eadie and David
E.  Bernhardt:

          Office  of  Radiation  Programs-Las Vegas  Facility
          U.S. Environmental Protection Agency
          Las Vegas, Nevada  89114

                    and by

George A. Boysen  whose present  address is:

          Deputy  Chief, Occupational  Health and
           Injury Control Branch
          Navajo  Area Office
          Window  Rock, Arizona   86515

     This study involved the cooperation and coordination of many
people.  In particular, the following persons contributed sub-
stantially to the project.

J.  R. SIMPLOT COMPANY

Jack L. Smith, Vice-President
Development and Planning
Pocatel1o, Idaho

John F. Cochrane, Director,
Environmental Engineering
Pocatel1o , Idaho

Donald Gollob
Stack Sampling Technician
Pocatello, Idaho

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IDAHO DEPARTMENT OF HEALTH & WELFARE

ENVIRONMENTAL SERVICES DIVISION

Michael  Christie
Health Physicist
Boise, Idaho

Charles  L. Freshman
Environmental Specialist
Pocatello, Idaho

     The review efforts of the J.R. Simplot Corporation, the
State of Idaho, and the U.S. Geological Survey were especially
helpful  in the preparation of this report.  Other reviewers
included the U.S.  Environmental Protection Agency-Region X office,
and the  staff of the Office of Radiation Programs-Headquarters
and Eastern Environmental  Radiation Facility.

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                              PREFACE
     The Office of Radiation Programs  of the U.S.  Environmental
Protection Agency carries out a national program designed to
evaluate population exposure to ionizing and nonionizing radia-
tion, and to promote development of controls necessary to protect
the public health and safety.  This report describes various
surveys which were conducted at the 0.  R.  Simplot's Wet Process
Plant near Pocatello, Idaho to provide  basic data  to be used for
the evaluation of the radiological  impact  associated with the
phosphate industry.  Readers of this report are encouraged to
inform the Office of Radiation Programs of any omissions or
errors.  Comments or requests for further  information are also
i nvi ted.
                                   Donald W.  Hendricks
                                   Director,  Office of
                                 Radiation Programs, LVF

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                            ABSTRACT

     Radiological  surveys conducted at the J.  R.  Stmplot's  Wet
Process Plant in Pocatello,  Idaho indicate slightly elevated
ambient levels of  natural radioactivity.   Compared to an estimated
natural background annual dose equivalent rate of about 79  mrem,
net gamma dose rates ranged  from 42 mrero  in general plant areas
to 152 mrem per work year (2000 hours) on the  ore piles.  Ambient
radon-222 concentrations,~ranging from 0.14 to 1.9 pCi/1, were
measured in various indoor locations.   Elevated airborne radio-
activity concentrations were measured  in  several  work areas,  with
pol onium-210 and radiurn-226  being the  most predominant radio-
nuclides of the natural uranium decay  series.   Particle size
characterization indicates roughly 52  percent  of the arithmetic
total  radioactivity is associated with the particle size fraction
less than one micrometer equivalent aerodynamic diameter.  Stack
sampling results also show that appreciable concentrations  of the
naturally-occurring radionuclides are  being discharged into the
local  environs.  In general, the dose  estimates and the interpreta
tion of results have been oriented toward evaluating the maximum
potential impact of the plant on the environment; however,  no
attempt has been made to determine the annual  average dose  to
workers within the plant from all exposure pathways.
                                vt

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                             CONTENTS
ACKNOWLEDGMENTS                                              11i

PREFACE                                                        v

ABSTRACT                                                      vi

LIST OF FIGURES AND TABLES                                    1x

INTRODUCTION                                                   1

THE WET PROCESS                                                2

THE RADIOLOGICAL ASSESSMENT OF THE WET PROCESS PLANT           5


     Gamma Radiation Surveys                                   5

     External  Dose Assessment                                  8

          Background Radiation and Population Dose Limit       8
          In-Plant Radiation Exposures                         8

     Ambient Radon-222 Concentrations                         10

          Sampling System and Analytical  Methods              10
          Radon Measurement Results                           11
          Radon Dosimetry                                     12

     Wet Process Samples                                      13

     Environmental Samples                                    19
     Scrubber Discharge Samples                               22

     Airborne Particulate Radioactivity                       22
          Background Airborne Radioactivity Concentrations    22
          In-Plant Air Sampler                                25
          Gross Versus Net Results                            26
          In-Plant Air Sampling Net Results                   28
          Specific Activity of Airborne Particulate Sampling  28

     Particle Size Characterization                           35

          Cascade Impactor Sampling                           35
          Gross Results of Impactor Sampling                  36
          Comparison of Air Sampling Results                  43
          Particle Size Distribution                          45
     Stack Sampling                                           52

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                       CONTENTS (Continued)


                                                            Page

SUMMARY                                                       57

REFERENCES                                                    59

APPENDIX A - RADIOCHEMICAL ANALYTICAL METHODS                 62

APPENDIX B - AIRBORNE PARTICIPATE SAMPLING - GROSS
             RADIONUCLIDE CONCENTRATION RESULTS               70

APPENDIX C - UNCERTAINTIES IN LEAD-210 AND
             POLONIUM-210 AIR SAMPLE DATA                     77

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                          LIST OF FIGURES

Number                                                      Page
  1.  Flow Diagram of the Wet Process                           4
  2.  Ore Unloading and Storage Area.  Log-Probability
     Plot of the Particle Size Distribution                   46
  3.  Calciner Building.   Log-Probability Plot of the
     Particle Size Distribution                               47
  4.  200 Plant.   Log-Probability Plot of the Particle
     Size Distribution                                        48
  5.  Gypsum Pile.  Log-Probability Plot of the Particle
     Size Distribution                                        49
                          LIST OF TABLES

Number                                                      Page
  1.  Gamma Radiation Surveys - General  Work Areas            6-7
  2.  Ambient Radon-222 Concentrations                         12
  3.  Raw Materials Input to the Wet Process                   16
  4.  Phosphoric Acid Samples                                  17
  5.  Gypsum Samples                                           18
  6.  Fertilizer Samples                                       20
  7.  Portneuf River Samples                                   21
  8.  Water Samples                                            23
  9.  Scrubber Discharges                                      24
 10.  Radioactivity Content of Blank Glass Fiber Filters       27
 11.  Airborne Particulate Sampling                            29
 12.  Airborne Particulate Sampling in the Calciner Building   30
                                ix

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                   LIST OF TABLES (Continued)
Numb e r                                                      Page
 13. Airborne Participate Sampling in the 300
     Phosphoric Acid Plant                                    31
 14. Airborne Participate Sampling in the TSP  Areas           32
 15. Airborne Participate Sampling in the Ammophos Areas      33
 16. Airborne Participate Sampling in the Storage Areas       34
 17. Cascade Impactor Sampling in the Ore Unloading and
     Storage Area                                             37
 18. Cascade Impactor Sampling in the Calciner Building       38
 19. Cascade Impactor Sampling in the 200 Ammophos Plant      39
 20. Cascade Impactor Sampling at the Gypsum Pile             40
 21. Radioactivity Content of Blank Impactor Whatman #41
     Paper Filters                                            41
 22. Radioactivity Content of Blank Glass Fiber Filters
     (8 x 10-inch)                                            42
 23. Summary of Gross Results of the Cascade Impactor
     Sampling                                                 44
 24. Radioacti-ity Content of Blank Glass Fiber Filter
     (2.5-inch diameter)                                      53
 25. Stack Sampling                                           54

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                           INTRODUCTION
     Recent reports (Windham et a!.,  1976;  Guimond and Hindham,
1975) Indicate that mining and processing of phosphate ores
technologically enhance the quantities of naturally-occurring
radioactive materials such as radium  and uranium available to man
in the environment.  Such radionuclides have relatively long
half-lives and will therefore persist in man's habitat for
thousands of years.

     Current estimates show that the  phosphate Industry has
generated about twenty times the volume of waste materials as
compared to that from the uranium mining and milling industry.
The total radioactive waste inventory generated by the uranium
and the phosphate mining and milling  industries are comparable to
each other although the per gram radioactivity content of the
phosphate waste is much less than that of uranium waste material
(EPA, February 1977).
     In general, the phosphate industry is neither regulated nor
monitored for the possession, use, or discharge of radioactive
materials associated with phosphate rock and its products and by-
products.  Recently, the State of Idaho (June 1, 1977) has
prohibited the use of phosphate slag  material in the construction
of habitable structures, but has permitted the continued use of
slag for road construction, railroad  ballast, and other general
purposes.
     Of immediate concern is the accumulation of a data base
which will ultimately lead to an assessment of the impact on
public health due to the phosphate industry's activities.  This
report discusses various radiological surveys conducted in the
J. R. Simplot's Wet Process Plant in  Pocatello, Idaho.  The
intent of the study was to obtain a general Indication of the
concentrations of radionuclides In the ore, process streams,
products, by-products, and effluents  of the plant.  In general,
the dose estimates and the interpretation of results have been
oriented towards evaluating the maximum potential  Impact of the
plant on the environment.  A similar  study, conducted 1n a thermal
process plant, has been discussed in  another report.
                                1

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                          THE WET PROCESS

     Phosphate rock is shipped by rail  from the Conda and Gay
Mines to the J.  R.  Simplot's Wet Process Plant near Pocatello,
Idaho.   The rock is conveyed from the stockpile to the Calciner
where it is heated  to about 1500° F, burning out the organic
material.   This  calcining also upgrades the phosphate content by
two to three percent, with the calcined ore containing approxi-
mately 32  to 34  percent phosphorus pentoxide (P^Og).  The calcined
ore is ground into  a fine powder which  is then reacted with
sulfuric acid in the Phosphoric Acid Plant to produce phosphoric
acid and by-product gypsum.  This reaction is approximated by the
equation :
2 H20 + Ca3(P04)2, + 3 H2S04+ 2 H3P04 + 3 CaS04
                                                      2 H20

Water + Phosphate Ore + Sulfuric Acid •*• Phosphoric Acid + Gypsum
     The phosphoric acid produced in this process is 30 to 32
percent P205.  This acid is then used to make several grades of
fertilizers.  Phosphoric acid, ammonia and sulfuric acid are
mixed together to produce various grades of ammonium phosphate
and to make ammonium sulfate.  Three basic grades of solid
ammonium phosphate (anmo-phos), two grades of liquid ammo-phos,
and crystalline ammonium sulfate are produced at the Wet Process
Plant.  These are 16-20-0, 18-46-0, and 11-54-0 for the solid
ammo-phos; 10-34-0 and 11-37-0 for the liquid ammo-phos; and
21-0-0 for the ammonium sulfate.  (The numbers represent the
percent nitrogen, ?2^l-> anc' P°tasn in the final product.)

     In the manufacture of the solid ammo-phos, the ammonia,
phosphoric acid, and sulfuric acid are mixed  in a reactor to form
a slurry.  This slurry is then mixed with recycle fine product  in

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a granulator, with the slurry coating the outside of the recycle
particlea to form a layer of fresh ammo-phos.  Ttie granulated
material is then dried and screened.   The oversized material is
crushed and recycled with the fine.  The intermediate fraction,
the ammo-phos product, is cooled and  conveyed to storage.

     The liquid fertilizer (10-34-0 and 11-37-0} is made by
reacting ammonia, water, and concentrated "superacid" (70 percent
P205) to form the liquid products.  (The superacid is produced by
evaporation of 52 percent PpO,-.)

     Ammonium sulfate is produced by  reacting ammonia and sulfuric
acid in a crystal 1izer,  under vacuum, which forms a crystalline
product.  The crystals are separated  from the liquid phase by
centrifuging.  The crystals are then  dried and conveyed to
storage and the liquid phase is returned to the crystallizer as a
"seed"  solution.

     Another product, triple superphosphate (0-45-0) was produced
by reacting the ground phosphate rock with phosphoric acid.  This
acidulated material is "cured" for a  period of about three to
four weeks and is then ground, granulated, dried, and screened.
This process is no longer utilized; instead, a patented process
is now  used which eliminates the need for "curing."  These various
processes are shown in Figure 1.

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                              \RAW  7
                               \ ROCK /
                                                    ~^3
                                     0 010
   SULFUR

  5O  I  OO
   SULFUR
  STORAGE
                      AIR
                  NATURAL GAS
                                                        Co
                          3>
          FLUOSOLIDS]
           REACTOR  |
                     AMMONIA PLANT
     I
SULFURIC ACID
    PLANT
  AMMONIUM
   SULFATE
                  |  AMMONIA  |
                  |  STORAGE  |
                  f
PHOSPHORIC
ACID PLANT
              AMMONIUM
              PHOSPHATE
                                    LJ
• ••••••••• ••••••••
GYPSUM
TAILINGS
                                                                TSP
                                                             PRODUCTION
                 18-46-0
21-0-0       16-20-0      11-54-0     10-34-0
                                                                     TSP
                                                                 GRANULATION
                                                   0-52-0
                                                                    0-45-0
                    Figure  1.   Flow diagram of  the wet  process

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       THE RADIOLOGICAL ASSESSMENT OF  THE  WET PROCESS  PLANT
     Radiological  surveys were completed at the J.  R.  Simplot's
Wet Process Plant  in Pocatello,  Idaho during the week  of April  28
to May 1, 1975.   Included among  these surveys were:   gamma
radiation measurements;  ambient  radon-222 concentrations;  radio-
logical  analyses of selected input, process and product samples;
airborne particulate sampling; and particle-size characterization.
Stack sampling of  representative effluent discharge  vents  was
also completed in  September 1975.   The following sections  of this
report discuss the results of these surveys.
GAMMA RADIATION SURVEYS

     In order to assess the external gamma radiation exposure
rates in the various working areas of the Wet Process Plant, a
survey was conducted using a portable gamma scintillator survey
meter.*  This instrument was calibrated with a radium-226 standard,
and measured the relative gamma radiation exposure rate in units
of microroentgens per hour (uR/h).  Measurements were made at a
height of three feet above an area surface and the results shown
in Table 1 represent average values for each location.  At the
time of these surveys, a pressurized ionization chamber (PIC) was
not available to complete radiation surveys for comparison to the
scintillator measurements.  Although the scintillator survey
meter's response is dependent on  the energy of the gamma
photon (Eadie et al., 1976), no instrument response correction
factor has been applied to the reported scintillator measurements.
   Baird-Atomic, Type NE148A-Gamma Scintillator Ratemeter.
                                  5

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  • -------
    Therefore,  the reported scintillator measurements  (Table  1)  are
    assumed to  be equivalent to the "true"  gamma exposure rate due to
                                                   *
    both the cosmic and the terrestrial  components.
    
    EXTERNAL DOSE ASSESSMENT
    
    Background  Radiation
    
         Gamma  exposure rate data for non-coastal plain regions of
    the United  States have been summarized  and indicate a mean value
    of 5.2 yrem/h (46 mrem/year) absorbed dose rate equivalent in air
    from terrestrial sources (NCRP, November 1975).   Specific surveys
    around the  National Reactor Testing Station near Idaho Falls,
    Idaho showed an average terrestrial dose equivalent rate of about
    6 yrem/h (Oakley, 1972).  Therefore, the natural terrestrial
    background  radiation annual dose equivalent for the Pocatello,
    Idaho area  should be approximately 53 mrem per year (i.e., con-
    tinuous exposure at 6 yrem/h x 24 h/day x 365 day/year).
    The scintillator instrument's response to cosmic radiation in the
    Pocatello area  has been estimated to be roughly 3 yR/h.  This
    value corresponds to an annual average cosmic dose equivalent
    rate of 28 mrem per year as summarized by NCRP  (November, 1975).
    Therefore,  a total natural  background radiation exposure rate of
    9 yR/h has been used to obtain the "net" exposure rates for the
    survey results  as reported  in Table 1.
    
    In-Plant Radiation Exposures
    
         Several areas of  background radiation  exposure rates were
    measured in  the Wet Process Plant  (Table 1).  The lowest net
    exposure rate  (measured minus background rate)  was 1 yR/h in  the
    
    *    The absorbed exposure  rates (mR/year)  have been converted  to
         dose equivalents  (mrem/year), assuming  the roentgen  is
         essentially equal  to  a rad and  using  a quality factor of
         one for gamma photons.  This  is consistent with the recom-
         mendations of the  National Council on  Radiation Protection
         (NCRP,  January 1971 ).
                                    8
    

    -------
    ammonium sulfate storage area and in the area of the 70 percent
    phosphoric acid tanks.   Therefore, for workers who spend the
    majority of their working periods in these areas, the maximum
    annual  dose equivalent  would be about 2 mrem per year (i.e.,
    1  yR/h  x 40 h/wk x 50 wk/year).  General working areas within the
    200 Phosphoric Acid Plant had net exposure rates ranging from
    background in the evaporator control room to 21 yR/h around the
    phosphoric acid tanks.   This corresponds to a maximum dose
    equivalent of 42 mrem per year.  The highest net exposure rate,
    111 yR/h, obtained in the Wet Process Plant was observed near a
    condensate pipe in the  200 Phosphoric Acid Plant.
    
         Background exposure rates were also measured in the phos-
    phoric  acid control room of the 300 Phosphoric Acid Plant.  Area
    surveys over the ore storage piles showed net exposure rates of
    about 61 yR/h for the low grade ores to 76 yR/h for the high
    grade ore. Surveys around the various plant product areas ranged
    from background in the  ammonium sulfate storage area to a high of
    26 yR/h on the triple super phosphate (green pile) storage area.
    
         In-plant radiation exposures are also summarized in Table 1.
    By assuming co tinuous  exposure during the entire work period
    (40 h/wk x 50 wk/year)  at the net gamma exposure rate levels, the
    reported dose equivalents are probably overestimated.  A more
    precise dose estimate could be obtained by fractioning the time
    spent in various work locations and using that particular exposure
    rate; however, such information has not been obtained in this
    study.   It should also  be emphasized that these in-plant external
    gamma dose estimates for the work year are in addition to the
    dose received by an individual due to natural background radiation
    exposure.  Furthermore, these estimates are based on free air
    measurements.  It is estimated that the dose to internal body
    organs  varies from 0.5  to about 0.7 of the free air measurement
    due to  the shielding effect of the body (O'Brien and Sanna,
    1976).
    

    -------
         Surveys conducted at a Thermal  Process  Plant in  Florida
    (Windham et al.,  1976) showed external  gamma dose rates  slightly
    higher than those measured in this study.   Total  measured  dose
    equivalent rates  (including background)  in the Florida plant
    ranged from 100  mrem per work year in general  plant areas  to  a
    maximum of 300  mrem per work year in the ferrophosphorus and  slag
    storage area.   For the Idaho Thermal Process Plant, the  general
    work areas averaged about 42 mrem per work year,  and  the maximum
    net dose equivalent rate (on the slag pile)  was 182 mrem per  work
    year, above a  background level of about 79 mrem per year.   For
    the Idaho Wet  Process Plant, the general work area averaged about
    42 mrem per work  year, and the maximum net dose equivalent rate
    on the ore piles  was 152 mrem per work year, above a  background
    level of about  79 mrem per year.
    
    AMBIENT RADON-222 CONCENTRATIONS
    
    Sampling System and Analytical Methods
    
         A continuous, low-volume sampling system was used to obtain
    samples of ambient air for analysis of radon content (U.S. Public
    Health Service,  1969).  This sampling technique consists of
    drawing filtered  air through a small, low-volume air pump (less
    than 10 ml/min  sampling rate) into a 30-liter Mylar bag.  The air
    intake was about one ireter above the ground surface.   Various
    sampling time periods were used for this  study.
    
         Radon analysis was completed at the  Environmental Monitoring
    and Support Laboratory in Las Vegas, Nevada (EMSL-LV) using a
    radon concentration apparatus for sample  preparation (Johns,
    1975).  This apparatus permits the  isolation of radon from about
    a 5-liter ambient air sample by transferring the ambient air  from
    the Mylar bag into a container of known volume, followed by
    circulation through water and carbon dioxide traps.  Radon is
    collected on two charcoal traps maintained  at a temperature of
    about minus 80° C using dry  ice and acetone.  The  radon sample  is
                                   10
    

    -------
    then de-emanated into a Lucas scintillation cell  (125-ml  volume)
    using helium gas at 400° C.   The Lucas cell is held for four and
    one-half hours to allow for  the ingrowth of the radon daughters
    and then counted in a photomultiplier tube/sealer unit.  The
    radon activity is calculated to the mid-point of the sample
    collection period to account for the radioactive decay
    (T,  = 3.82 days) of radon from  the  time of sample collection to
    time of analysis.  The ambient  air  volume sampled is determined
    by correcting for air density differences based on the nearest
    1000-foot elevation increment,  and  the average ambient temperature
    during the sampling period.   The radon concentrations (in pCi/1)
    reported in Table 2 therefore represent the average ambient radon
    concentration for the sampling  period for each specific sampling
    site location.
    
    Radon Measurement Results
    
         Ambient radon-222 concentrations measured in the various
    indoor working areas ranged  from a  low of 0.14 pCi/1 near a dryer
    of the No. 100 Ammophos Plant to a  high of 1.9 pCi/1 outside the
    control room of the 300 Phosphoric  Acid Plant. Out-of-doors, the
    ambient radon "anged from 0.23  pCi/1 to 0.31  pCi/1 on the ore
    loading and unloading areas  and the gypsum pile, respectively.
    
         Harley (1975) estimated the average background concentration
    of radon in surface air of about 0.10 pCi/1 in the northern hemi-
    sphere.  Other authors (Pearson, 1967; United Nations, 1972) have
    reported radon concentrations in the general  environment ranging
    from 0.03 to 0.4 pCi/1.  Ambient outdoor radon concentrations
    measured in areas associated with inactive uranium mill tailings
    piles indicate average levels of 0.34 pCi/1 (Monticello, Utah),
    0.38 pCi/1 (Salt Lake City,  Utah),  0.51 pCi/1 (Durango, Colorado),
    and 0.83 pCI/1 (Grand Junction, Colorado), (U.S.  Public Health
    Service, 1969).
                                    11
    

    -------
         Indoors, the radon levels  are  typically from three to four
    times the outdoor levels due  to  the  entrapment within the structure
    of radon emanation from soils  beneath  the  structure and also from
    radon emanated from the building  materials,  supplemented by radon
    infiltration from outside air.   In  general,  radon levels inside
    structures are usually 0.6  to  1.2 pCi/1  for  ventilation rates
    below four air changes per  hour  (Johnson et  al. ,  1973).  As shown
    in Table 2, the ambient radon  concentrations measured in the Wet
    Process Plant are within expected ranges due to natural terrest-
    rial background sources alone.
    Radon Dosimetry
    
         The report by Swift  et  al.  (1976)  discusses various aspects
    of radon dosimetry including  the  degree of equilibrium between
    TABLE 2. AMBIENT RADON-222 CONCENTRATIONS
    Date Radon *
    Time Location Concentration
    On Off Description (pCi/1)
    4/28/75
    1155
    4/28/75
    1035
    4/29/75
    0940
    4/29/75
    1021
    4/30/75
    0904
    4/30/75
    0828
    5/1/75
    0930
    5/1/75
    0942
    Calciner Bldg.
    1542 No. 3 Calciner
    300 Phosphoric Acid P
    1603 Outside Control Room
    0.18 ± 0.036
    lant
    1.9 ±0.12
    100 Plant, Ground Floor
    1612 Near Ammophos Dryer 0.14 ± 0.033
    1530 TSP Storage Area
    Grinder Building
    1555 Mill #7
    TSP Dryer
    1500 Station 13
    Gypsum Pile-
    1332 North End
    Ore Loading and
    1320 Unloading Area
    0.55 ± 0.064
    0.22 ± 0.041
    0.32 ± 0.05
    0.31 ± 0.049
    0.23 ± 0.043
    *  Radon-222 concentration ± two-sigma counting error term.
       To convert to pCi/m3,  multiply the pCi/1 value in the table
       by  1000.
                                     12
    

    -------
    radon and its daughters,  the  fraction  of unattached daughter ions
    and certain assumptions  regarding  exposure modes to tissues
    within the lung.  For dose  estimates  in  this  study, a dose con-
    version factor of 4 mrem  per  year,  for continuous exposure to 1
    pCi/m3,  was used.  This  factor  represents radon-222:polonium-
    218:lead-214:bismuth-214  concentrations  of 1.0:0.90:0.51:0.35
    pCi/m3, respectively.  This  is equivalent to  an average daughter
    product equilibrium ratio of  50  percent  and an average ventilation
    rate of one air change per  hour, which is typical in living
    accommodations with adequate  ventilation.  This dose is delivered
    to the basal cell nuclei  of  segmental  bronchi  which are estimated
    to lie 60 ym below the surface where  the activity is deposited.
    A quality factor of 10 for  alpha particles has been used in the
    dose calculations.  Therefore, continuous exposure to an assumed
    average background radon  concentration of 100  pCi/m3 (0.10 pCi/1
    as estimated by Harley,  1975) would result in  a dose equivalent
    of 400 mrem per year.  For  a  worker exposed for an entire work
    year (40 h/wk x 50 wk/year)  to the  maximum ambient measured radon
    concentration of 1,900 pCi/m3, the  dose  equivalent would be about
                     *
    1.7 rem per year.
    WET PROCESS SAMPLES
         Appendix M discusses the radiochemical analytical techniques
    used for this study.  Since  the  completion of  the analyses of the
    following samples, a question has  arisen as to the validity of
    the lead-210 radiochemical  procedure.   Although the procedure as
    outlined in Appendix A for  the lead-210  analysis was fully tested
    and proved satisfactory  for  water  sample analysis, there now
    appears to be some difficulty in obtaining consistent lead-210
    recovery rates for solid  samples such  as the  ore, briquettes,
    
    *  4 mrem/year/(pCi/m3) x 8760 h Continuous x ]'90° pCi/m3 x 10~3 rem/mrem =
                                 Exposure                  1.7 rem/year
        The significance of this dose estimate is questionable, given the
        uncertainties in the determination of background and the "grab sample"
        nature of this particular measurement, plus the actual exposure condi-
        tions of the plant personnel.
    
                                   13
    

    -------
    slag,  and air filter samples.   The inaccuracies  of  the  lead-210
    results relate to analysis  of  samples  without the  benefit  of  a
    tracer or carrier yield.   Thus the assumed  yield,  which was
    assumed to be the same as  that for test  samples  (i.e.,  85  percent)
    was in error by up to a factor of five.   Comparison of  lead-210
    cross-check results, as reported for two EPA laboratories,
    indicates that the EMSL lead analyses  are roughly  a factor of
    five lower than the actual  lead-210 content (see Appendix  C  for
    data which limits the uncertainty for  individual results).  This
    error has also been noted  in recent cross-check  air sample results.
    Since the majority of samples  have been  consumed to obtain the
    results reported here, it  is impossible  to  re-analyze these
    samples to resolve this question.  Therefore, the  lead-210 results
    which have been obtained using the EMSL  procedure  (Appendix  A)
    have been reported here, but for solid samples,  these results
    probably underestimate the real sample lead-210  activity by  up  to
    about a factor of five.  Future lead-210 analyses  will  be  con-
    ducted with a revised technique.
    
         The problem of underestimating the  lead-210 content is  also
    reflected in the estimate  of a sample's  polonium-210 content, as
    discussed in Appendix A.  Results reported  in the  thermal  process
    report (ORP/LVF, 1977) for selected samples (e.g.  calcined ore
    and slag) indicate that the polonium-210 values  reported here may
    overestimate the actual polonium-210 content by  a  factor of  ten
    or more (ranging from 1 up to  about 20,  but could  be higher);
    i.e., if the reported EMSL lead-210 results are  actually a
    factor of five too low.  Recognizing these  difficulties encountered
    in obtaining valid lead-210 and polonium-210 results, the  following
    sections describe the radiological evaluations of the Wet  Process.
         The two-sigma (95 percent) statistical counting error is
    reported for all of the radiochemistry data presented in this
    report.  The techniques for calculating  the counting errors  are
    illustrated in Johns  (1975).  The error  terms for data  averages,
    the decay and ingrowth corrected polonium-210 results,  and for
    the net air sample results represent error  terms obtained  using
                                    14
    

    -------
    techniques for propagating error estimates as given  in Appendix A
    and by Eadie and Bernhardt (1976).
    
         It should be recognized that the statistical  counting error
    only includes the uncertainty from  the number of counts measured
    from the sample and instrument background.  It is  not an estimate
    of the total analytical  uncertainty nor uncertainties in sample
    collection, preparation  and/or aliquoting procedures.  Evaluation
    of soil sampling and analytical  techniques for plutonium by
    Bernhardt (1976) indicate that sampling and analytical variations
    of up to 50 percent and  more (95 percent confidence  level) are
    observable in many groups of data,  especially at levels within
    about an order of magnitude of the  analytical detection level.
    Thus, it should be recognized that  the uncertainty of the results
    is greater than the counting error.
    
         Table 3 presents the results of analyses of samples consid-
    ered to be typical of the raw materials input to the wet process.
    The average radium-226 content of the Idaho phosphate rock (ore)
    was 29 pCi/g, and the calcined ore  contained 38 pCi/g for the Wet
    Process Plant, but was 26 and 25 pCi/g, respectively, for the
    Thermal Proces* Plant  (ORP/LVF, 1977).  Radium-226  analysis
    of Florida ore average about 60 pCi/g (Guimond and Windham,
    1975).
    
         The results of limited analyses of phosphoric acid samples
    are shown in Table 4.  Radium-226 concentrations in  the various
    grades of phosphoric acid ranged from 5.7 ± 0.87 to  63 ± 3.3
    pCi/1.
    
         The results of analyses of several gypsum samples are shown
    in Table 5.  The radium-226 content of a composite sample from
    the gypsum pile was 23 ± 0.87 pCi/g.  For the samples from the
    phosphoric acid reactor  and the thickner, the suspended matter
    was allowed to "settle-out" of solution and hence  a  suspended and
    liquid fraction of the sample were  analyzed.  For  both samples,
                                    15
    

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    appreciably more radioactivity was contained in the suspended
    versus the liquid fraction,  perhaps reflecting the water insolu-
    bility of these radionuclides.  Total  water samples, i.e.,
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         The results of analyses of the various product fertilizers
    are shown in Table 6.  The highest radium-226 activity content of
    14 ± 0.68 pCi/g was measured in the triple superphosphate (TSP).
    The liquid fertilizer (10-34-0) had a radium-226 content of
    25 ± 1.8 pCi/1.
    
    ENVIRONMENTAL SAMPLES
    
         Grab water samples were obtained from the Portneuf River at
    locations both upstream and  downstream from the liquid waste
    effluent discharge from both the Thermal  Process and the Wet
    Process Plants.  Prior to  analysis, the suspended solids were
    allowed to "settle-out" and  hence, both a liquid (soluble compon-
    ent) and a suspended (insoluble component) fraction of each water
    sample was processed.  The water samples  collected during this
    study are non-potable, and human ingestion of such water is
    improbable.
    
         The radiochemical results for the Portneuf River samples are
    shown in Table 7.  For the liquid fraction, the results of the
    upstream and downstream samples are essentially identical since
    they are within the two-sigma counting error term for each
    respective analysis.  Similar analytical  agreement was not
    obtained from the results  of the suspended fraction analyses.
    Although the measured radium-226 content  was lower in the down-
    stream sample, the uranium and thorium contents were about an
    order of magnitude greater in the downstream versus the upstream
    sample.  The higher radioactivity content in the suspended
    fraction may indicate the  insolubility of waste-product effluents,
    It must be emphasized  here  that  these  results  are  based on
    
                                    19
    

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    analysis of only one grab sample from both the upstream and  the
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    of both the liquid and suspended fractions of both of these  river
    water samples are well within the typical  background range for
    naturally-occurring radioactivity (Holtzman,  1964).   The slightly
    elevated activity in the suspended sediments  indicate that any
    future efforts to resolve whether there is any contribution  of
    radioactivity to the stream should include sediment sampling.
    
         Additional  water sample results are shown in Table 8.  The
    incoming water (Well #5) and the discharge water from the West
    Plant Outfall are at typical background radioactivity concentra-
    tions.  The cold pit water sample, however, shows an elevated
    radioactivity content of the suspended fraction, again reflecting
    the water insolubility of these natural radionucl ides.  The  cold
    pit water is recycled water within the plant which is not dis-
    charged to the uncontrolled environment.
    
    SCRUBBER DISCHARGE SAMPLES
    
         Results of the suspended and liquid fractions of various
    scrubber discharge samples are presented in Table 9.  Again, the
    suspended fraction contains the greater radioactivity content.
    The lowest radium-226 concentration of 2.5 ± 1.1 pCi/g was
    measured in the suspended fraction of the 200 Plant-phosphoric
    acid scrubber discharge sample.  The highest radium-226 content
    of 33 ± 1.1 pCi/g was obtained from the suspended fraction of the
    calciner scrubber discharge.  These results are  similar to those
    obtained from the calciner scrubber discharges from the Thermal
    Process Plant (ORP/LVF, 1977).
    
    AIRBORNE PARTICIPATE RADIOACTIVITY
    
    Background Airborne Radioactivity Concentrations
    
         Poet et al.  (1972) reported the average polom'um-210 and
    lead-210 concentrations; in ground level air to be 0.001 and 0.01
                                    22
    

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    pCi/m3,  respectively.   NCRP  (.November,  1975)  summarizes  reports
    by geographic areas of the normal  polom'um-210 and lead-210 air
    concentrations.   In Colorado,  the  reported polonium-210  concen-
    trations ranged  from 0.00005 to 0.003 pCi/m3,  whereas the lead-
    210 ranged from  0.001  to 0.021  pCi/m3.   The highest reported
    lead-210 concentrations were 0.026 pCi/m3  for  several locations
    in Illinois and  Utah.
    
         NCRP (November, 1975) also discusses  the  background level  of
    airborne concentrations of the  other naturally-occurring radio-
    nuclides.  Natural  uranium concentrations  ranged from 120 aCi/m3
    (one attocurie is 10-18 curie  or 10~6 pCi) near Chicago, Illinois,
    to a reported high  of  about  400 aCi/m3  for several sites in New
    York State.  Typical radium-226 concentrations are usually less
    than 100 aCi/m3.   Sedlet et  al. (1973)  reported thorium-232 and
    thorium-230 concentrations of  30 and 45 aCi/m3, respectively,
    near Chicago, Illinois.
    
    In-Plant Air Sampler
    
         Air samples  were  obtained  in  the in-plant areas using a
    portable air sampling  unit.*  This unit has a  carbon vane vacuum
    pump with a regulator  which  permits constant air flow sampling.
    Usually, sample  collections  were made at two cubic feet  per
    minute (CFM) using  a 47-millimeter diameter, Type E glass fiber
    filter.   This corresponds to a  linear flow rate of about 106 feet
    per minute.  The  air sample  dust load was  determined by  measuring
    the mass of material collected  on  each  filter.
    
         Airborne particulate sampling was  conducted in several
    working  areas within the Wet Process Plant using the portable air
    sampler.  The radioactivity  concentrations of  the naturally-
    occurring radionuclides are  usually expressed  as picocuries per
    *  Regulated Air Sampler, Model  RAS-1,  Eberline Instrument
       Corporation, Santa Fe, New Mexico
                                   25
    

    -------
    cubic meter of sampled air (pCi/m3).   Dust loading  of  the  air
    filter samples was also determined and the specific activity of
    the dust,  expressed as pCi/g,  is  also  given.   The  solubility of
    airborne particulate matter was not determined in  this study.
    
    Gross Versus Net Results
    
         Eadie and Bernhardt (1976) have reported that  radiochemical
    analyses of blank glass fiber  filters  (4-inch diameter)  indicate
    appreciable quantities of naturally-occurring radioactivity.
    Such activity may be due to the composition of the  filter  media
    itself, or due to contaminants in reagents, glassware, or  other
    analytical equipment.  The analytical  sensitivity  of the radio-
    chemical techniques may also mask the  identification of the true
    source of such low levels of radioactivity.
    
         Table 10 presents data on the radioactivity content of blank
    glass fiber filters (4-inch diameter)  and the extrapolated
    activity content for the 47-mm diameter filters which were used
    in this study.  In order to account for this radioactivity
    content associated with blank filter analyses, the appropriate
    blank filter activity  (Table 10)  has been subtracted from  the
    measured gross analytical result to obtain a "net"  result.  No
    blank subtractions have been made for  the three radionuclides
    (radium-228, polonium-210, and lead-210) which are at the
    analytical minimum detectable activity (MDA) levels.  Gross
    analytical results for all of the in-plant air samples are  shown
    in Appendix B.
                                   26
    

    -------
       TABLE 10.   RADIOACTIVITY CONTENT OF BLANK GLASS FIBER FILTERS
                              (pCi  per filter)
              ***
       Radi onucli de
    Ra-226
    Po-210
     U-234
     U-235
     U-238
    Th-230
    Th-232
    Pb-210
    Ra-228
    4-inch Diameter
    
       0.35 ± 0.09
             <0.17
       0.10 ± 0.03
    (0.0035 ± 0.0010)
       0.08 ± 0.02
       0.20 ± 0.08
       0.13 ± 0.02
             <0.32
             <1 .6
                    **
      47-mm Diameter
    
       0.07 ±  0.019
             <0.036
       0.021*  0.0064
    (0.00075±  0.00021)
       0.017*  0.0043
       0.043±  0.017
       0.028±  0.0043
             <0.068
             <0.34
    +  Average pCi  per filter with standard error term about this
       mean based on the t-distribution at the 95 percent confidence
       1 eve! .
    *  Taken  from Eadie and Bernhardt, 1976.
    ** Extrapolated value based on the area ratio between 47-mm and
       4-inch  diameter filters of  0.214 times the 4-inch diameter
       activity content.  Average  47-mm filter mass ± two standard
       deviations was 0.1249 ± 0.0013  grams.
    
    ***Calculated U-235 content based  on U-235 to U-238 natural
       activity ratio of 1:21.45 (0.0466).
                                    27
    

    -------
    In-Plant Air Sampler Net  Results
    
         Tables 11  to 16 present  the  net  radionuclide  concentrations
    obtained for the various  in-plant sampling  locations.   As  pre-
    viously noted,  the leacl-210 results  are  underestimated  by  up  to  a
    factor of five,  which results in  a  potential  overestimate  of
    about a factor  of ten or  more for the polonium-210 results.   Data
    which narrows this uncertainty for  specific samples are given in
    Appendix C.
    
         Of all the  in-plarit  samples, the highest airborne  radio-
    activity was measured in  the  area of  the No.  3 Calciner (Table
    12).  There, the measured airborne  concentrations  were  orders of
    magnitude greater than results obtained  in  the Technical  Building
    Library (Table  16).  Although the library had the  lowest airborne
    radioactivity measured in this study, even  these levels were
    slightly elevated compared to reported background  levels as
    discussed above.
    
    Specific Activity of Airborne Particulate Matter
    
         The specific activity of airborne particulate matter
    (reported in units of pCi/g)  was  also determined for the portable
    air sampler filters.  The highest polonium-210 activity was  371  ±
    146 pCi/g in the control  room of  the Calciner Building  (Table 12)
    with roughly one-half of  the sampling locations having  essentially
    a non-detectable polonium-210 level  (Tables 11, 13, 14, 15,  and
    16).  The highest radium-226 activity of 41 ± 11 pCi/g  was also
    obtained in the Calciner  Building (Table 12) and the lowest
    activity was less than 2.1 pCi/g  in the Technical  Building
    Library (Table 16).  These results for the Calciner Building  also
    show possible disequilibrium between the individual radionuclides
    of  the uranium-238 decay  series,  the most noticeable being the
    polonium-210 and thorium-230 contents compared to the other decay
    chain members.   (Thorium-232 and  radium-228 are members of a
    different decay series.)   It should be recognized that  the
    
                                   28
    

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    apparent disequilibrium can be  partially  accounted for by the
    errors in the polonium and  lead-210  data  and  analytical uncertain-
    ties (see Appendix C).  The results  for  #3  calciner do indicate
    the strong liklihood of excess  polonium-210 (see Appendix C).
    
         Specific activity determinations  of  the  airborne particulate
    matter may also be compared to  the  results  of analyses of the raw
    material input to the wet  process  (Table  3).   The highest polonium-
    210 content of the input ore  was  48  ±  5.9 pCi/g (Conda Mine-low
    grade ore).  The specific  activity  determinations of the airborne
    particulate samples from the  Calciner  Building indicate potentially
    higher polonium-210 than the  input  ore concentration.  The specific
    activity concentrations for the other  radionuclides in the input
    products are generally comparable  to the  airborne particulate
    sample results for all locations  sampled.
    
    PARTICLE SIZE CHARACTERIZATION
    
    Cascade Impactor Sampling
                                       *
         High volume cascade impactors   were  used to measure the size
    distribution of airborne particulate matter for both the indoor
    and outdoor environments.   The  impactor  filter stages attach to a
                           **                                    ***
    high volume air sampler    which is  electronically controlled
    to operate at a flow rate  of  40 cubic  feet  per minute  (CFM).
    This corresponds to a linear  air  velocity of  about 72 feet per
    minute through the final 8  x  10-inch filter stage.
    
         Whatman #41 paper filters  were  used  for  each impaction
    stage. Glass fiber (Type E) was used for  the  final 8 x 10-inch
    filter.  Typical particle  size  ranges  for each filter stage, as
    reported by the manufacturer, are:
    *  Model  252 Series, six stage, cascade impactor from Tech Ecology, Inc.
       (Now produced and marketed by Sierra Instruments, Inc.)
    ** Model  GMWL-2000, High Volume Air Sampling System from General Metal Works,  Inc.
    ***Model  310/310A, High Volume Constant Flow Controller from Sierra Instruments,
       Inc.
    
                                    35
    

    -------
                             Equivalent Aerodynamic  Diameter at 50
        Stage No.              Percent Collection Efficiency  (micrometer)
    
           1                  Greater than 7.2 ym
           2                        3.0 - 7.2
           3                        1.5 - 3.0
           4                        0.95- 1.5
           5                        0.49- 0.95
        Final Filter           Less than   0.49
    
         "Equivalent aerodynamic diameter" is  defined  as  the  size  of
    a spherical particle of unit density which has  the same  terminal
    settling velocity as the sampled particle.   Radioactivity analysis
    of each impactor stage provides an indication of the  activity
    content for the various particle size ranges.
    
    Gross Results of Impactor Sampling
    
         The cascade impactor sampler was used at four locations  in
    the Wet Process Plant - the Calciner, the  ore unloading  and
    storage area, the 200 Ammophos Plant (18-46-0 storage area),  and
    at the gypsum p-'le.  Gross analytical results for  these  samples
    are presented in Tables 17 to 20. Tables  21  and 22 show  the
    results of radiochemical analyses of blank impactor filters  -  the
    slotted Whatman #41 paper and the 8 x 10-inch glass fiber filters,
    respectively.  Since most of the blank slotted  paper  filters
    contained  radioactivity concentrations at  the minimum detectable
    activity (MDA) levels for the analysis, a  blank filter subtraction
    has not been performed for all the radionuclides for  the impactor
    samples.   As noted  in subsequent discussions, tabulations of  net
    results have been used in some of the data plots.   The previously
    noted reservations  concerning the lead-210 and  polonium-210  data
    also apply to these results (i.e., lead-210  may be low by a
    factor of  five or more and polonium-210 high by a  factor of  ten).
    Data for narrowing  the uncertainty on specific  samples are given
    in Appendix C.
                                    36
    

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         Table 23 provides a summary of the gross  results  of  the
    cascade Impactor sampling for the four sampling  locations.  Except
    for the results from the 200 Ammophos Plant the  majority  of
    radioactivity (ranging from 32 to 77 percent of  the arithmetic
    total) was measured in the particle size fraction less than
    0.49 ym.   The average of all four sampling locations indicates
    that roughly 52 percent of the arithmetic total  airborne  radio-
    activity was in the sub-micron particle size range.
    
    Comparison of Air Sampling Results
    
         The activity summation for all filters of the cascade
    impactor may be compared to the activity concentrations determined
    from the portable air sampler for the same sampling location.
    Good agreement has been obtained between the results of the
    radioactivity determinations using these two different sampling
    systems,  even though the samples were not necessarily  obtained
    during simultaneous time periods.
    
         For the Ore Unloading and Storage Area, impactor  results
    (Table 17) are roughly two to three times the activity concen-
    trations as measured using the portable air sampler (third  column
    of Table 11).  In both cases, decay chain members appear  to be  in
    equi1ibrium.
    
         In the Calciner Building, the cascade impactor results
    (Table 18) are about one-third of the activity measured using  the
    portable air sampler (third column of Table 12), except for the
    radium-226 which was one-seventh of the portable air sampler
    result.  Of the four locations sampled for airborne radioactivity
    using both sampling systems, only the Calciner Building impactor
    results (Table 18) showed less airborne radioactivity  than  did
    the results obtained using the portable air sampler (Table  12).
    Of all the sampling locations, the highest airborne radioactivity
    measurements were obtained in the Calciner Building, regardless
    of the air sampling system used.  (This conclusion recognizes  the
    previously denoted uncertainties for the lead-210 and  polonium-
    210 results.)
                                   43
    

    -------
    
    
    
    
    
    
    
    
    
    
    
    
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    -------
         Impactor sampling in the 18-46-0 storage area  of  the  200
    Ammophos Plant (Table 19) showed  about three  times  the airborne
    radioactivity as obtained using  the portable  air sampler  (third
    column of Table 16).   Excellent  agreement was obtained for the
    results from both sampling systems  at the Gypsum Pile  (Tables  20
    and the fifth column  of Table 11).
    
    Particle Size Distribution
    
         Figures 2, 3,  4  and 5 present  the log-normal  probability
    plots of data from  the cascade impactor sampling.   The plotted
    points are based on both the gross  activity and in  some cases,
    the net activity (i.e., gross minus the appropriate activity
    associated with a blank filter).   Only total  uranium,  thorium-
    230, and radium-226 data have been  plotted.  Data  for  the other
    remaining radionuclides were not  plotted because of inadequate
    blank filter results  or because  the gross results  were so low
    that meaningful net results could not be calculated.  The actual
    points were calculated by allocating all the  activity  in  all the
    stages subsequent to  and including  that particular  stage  to the
    specified size cut  off for that  stage (Elder  et al. , 1974).  The
    manufacturer sppcified size cutoffs for the impactor at 40 cfm
    are 7.2, 3.0, 1.5,  0.95, and 0.49 micrometers (equivalent aero-
    dynamic diameter).   These are partially based on a  study  by
    Willeke (1975).  Thus, in the actual calculations,  the percent  of
    the total activity  on the 3.0, 1.5, 0.95, and 0.49  and final
    filter stages was designated as  less than 7.2 micrometers.  The
    percent of the total  activity on  the final filter was  ascribed  to
    the 0.49 micrometer stage, etc.   The lines are based on hand-
    drawn estimates and not based on  regression analysis.
    
         The plotted distributions (Figures 2, 3, 4 and 5) have not
    been statistically  tested to demonstrate the  appropriateness of
    describing the data with a log-normal distribution.  The  log-
    probability plots are used as a  tool to summarize the  data and
    describe its central  tendency.
    
                                    45
    

    -------
    10'
    5.0-
    2.0-
    UJ
    N
    35
    UJ
    _i
    u
    H
    1.0-
    0.5'
    0.2-
    0.1
                                   D U-Total (Gross)
    
                                   • Th-230 (Gross)
    
                                      Xg = 0.2 um
    
                                      Sg = M = 19
                                          0.2
    A Ra-226 (Net)
    
       Xg = 0.23 um
    
       Sg = °^I§ = 3.4
        a  0.23
    
    
    • Ra-226 (Gross)
    
       Xg = 0.2 um
    
       Sg = L2 = 6
        M  0.2
      0.01    0.1      125   10   20  30 40 50 60 70  80   90  95  98 99
                       ACCUMULATED PERCENT LESS THAN INDICATED SIZE
                                                                                99.9   99.99
     Figure 2.   Ore unloading and storage  area log-probability plot  of the
    
                        particle size  distribution (Table 17).
                                          46
    

    -------
       10-
    5.0-
      2.0-
    N
    V)
    Ul
    u
    1.0-
      0.5-
      0.2-
      0.1-
                             O U-Total (Gross)
                             • Th-230 (Gross)
                               Xg = 0.9jum
                                                          Ra-226 (Gross)
                                                          Yg = 0.4pm
      0.01   0.1       12   5   10   20  30 40 50 60  70  80  90  95   98 99
                       ACCUMULATED PERCENT LESS THAN INDICATED SIZE
                Figure  3.   Calciner building log-probability  plot of  the
    
                        particle  size distribution   (Table 18).
                                                                               99.9   99.99
                                             47
    

    -------
       10-
      5.0-
      2.0-
    S
    UJ
    N
    55
    UJ
    U
    1.0-
      0.5-
      0.2-
      0.1-
                  A U-Total (Net)
                  D  U-Total (Gross)
                  •  Th-230 (Gross)
                     Xg = 6 urn
                                      AD
                                                       Ra-226 (Gross)
                                                       Xg - 0.7 um
                                                       Sg = I? = 6
                                                           0.7
        0.01    0.1       12   5  10   20 30 40 50 60 70  80   90  95  98 99
                          ACCUMULATED PERCENT LESS THAN INDICATED SIZE
                                                                             99.9   99.99
                  Figure 4.   200 Ammophos plant  log-probability plot
    
                     of  the particle size  distribution (Table  19).
                                             48
    

    -------
       10'
      5.0-
      2.0
    S
    ui
    N
    55
    UJ
    u
    1.0'
      0.5'
      0.2-
      0.1-
        0.01
                                D U-Total (Gross)
                                • Th-230 (Gross)
                                   Xg = 0.1 um
                                A Ra-226 (Net)
                                   Xg = 0.03 um
        0.03
    
    
    Ra-226 (Gross)
    Xg = 0.04 um
    Sg = 0.57 = 14
        0.04
             0.1      12    5   10   20 30 40 50 60 70  80   90   95   98 99
                       ACCUMULATED PERCENT LESS THAN INDICATED SIZE
                                               99.9   99.99
                  Figure 5.   Gypsum  pile log-probability plot  of
    
                       particle size distribution  (Table 20).
                                            49
    

    -------
         The geometric  mean  (X  )  is  given  by  the  fiftieth  cumulative
    percent intercept.  The  geometric standard deviation  (S  )  is
    indicated by the slope  of  the line  and  is usually  calculated  by
    dividing the particle diameter at the  84  percentile  by  the  diam-
    eter at the 50 percentile.   Due  to  the  limited  data  and  the
    uncertainty of analytical  results,  there  is  considerable  uncer-
    tainty in the log-normal  probability values.   Many of  the values
    have been rounded to one  significant digit,  and those  that  have
    not are not accurate to  more than one  significant  digit.
    
         In order to present  as much inforamtion  as possible, size
    distribution plots  of the  gross  activity  are  given in  Figures 2
    to 5.   When the measured  sample  activity  was  sufficient to  allow
    calculation of reasonably  accurate quantities of net activity for
    most of the impactor stages, the size  distribution of  the net
    activity results were also  plotted (Figures  2,  4,  and  5).  The
    significance of the quantity of  blank  activity compared to  the
    net sample activity is  illustrated in  Figure  2.  Subtraction  of
    the blank radium-226 activity resulted in a  slightly different
    particle size distribution  plot  with essentially the same geo-
    metric mean value (X"  of 0.20 versus 0.23 ym) but  an apparently
    different standard  deviation (S   of 6.0 versus 3.4).  The thorium-
    230 sample activity was sufficiently greater than  the  appropriate
    blank activity such that the resulting "net"  values are essen-
    tially identical to the gross distribution therefore the net
    values were not shown.
    
         The data for the Ore Unloading and Storage Area,  the Calciner
    Building, and the Gypsum Pile (Figures 2, 3,  and 5, respectively)
    indicate geometric  means of less than one micrometer.   These
    results are within  expected values for atmospheric and industrial
    dusts (Lee, 1972; Elder et  al. ,  1974;  and Willeke, 1975).
    Relatively large geometric  means, indicating rather coarse
    particulate matter, was obtained in the 200 Ammophos Plant
    (Figure 4).
                                    50
    

    -------
         Geometric standard deviations  (S  )  ranged  from  3.4  to  19.
    These values are similar to,  but slightly higher than  reported
    values for ambient data (generally  less  than  S   of 10;  Lee,
    1972).  These relatively high geometric  standard deviations
    probably reflect the composite of several size  distributions.
    That is, there may be several particle size distributions  from
    the plant in conjunction with ambient  dust.  The results for the
    Ore Unloading and Storage Area (Figure 2) and the Calciner  Build-
    ing (Figure 3) show concentrations  above ambient levels.
    
         Knuth (1976), in his evaluation of  the impactor,  indicated
    that it tended to underestimate the size distribution  and  over-
    estimate the geometric standard deviation.   Thus, it is  possible
    that this is also reflected in the  data.  Although Knuth's
    results indicated that this appeared to  be  more of a problem for
    the larger size distributions (X  of 7 micrometers)  but  was  less
    of a problem for distributions around  4  micrometers.
    
         Results from Lee (1972)  indicate  average geometric  standard
    deviations of up to 20 for ambient  air.   Elder  et al. ,  (1974)
    indicate geometric standard deviations in the thirties  for
    processes using plutonium; thus, the values noted in this  study
    appear to be realistic.
    
         As shown in Figures 2 to 5, two different  particle  size
    distributions are implied by  the data  for total-uranium  and
    thorium-230 data versus the radium-226 data.   The geometric  mean
    of the uranium and thorium data for the  Calciner and the Gypsum
    Pile (Figures 3 and 5) are about twice that of  the radium  data
    and about a factor of 10 higher for the  200 Ammophos Plant
    (Figure 4).  The geometric means are similar  for the Ore Area
    (Figure 2), but the thorium and uranium  data  have a  higher
    geometric standard deviation  than the  radium  data.
                                    51
    

    -------
    STACK SAMPLING
         Stack sampling  was  conducted  in  late  September  1975  using
    the RAC Train Stacksamplr* and  methods  specified  in  the  Federal
    Register, Volume 36, No.  247  (December  23,  1971).   Representative
    samples were obtained from each process-type  discharge stack;
    however, every plant discharge  stack  was  not  sampled.
    
         Particulate matter  was collected on  a  glass  fiber filter
    (2.5-inch diameter)  which was subsequently  analyzed  for  natural
    radioactivity content.   To determine  the  blank filter natural
    radioactivity content,  two sets of unused  filters  were analyzed
    and these results are shown in  Table  24.   Also shown is  the
    extrapolated filter  content based  on  the  area ratio  between the
    2.5-inch and the 4-inch  diameter filters  of 0.391  times  the 4-
    inch diameter activity  content  as  reported  by Eadie  and  Bern-
    hardt, (1976).  These results show fairly  good agreement between
    the measured and the extrapolated  activity contents.  The extra-
    polated filter content  (last  column of Table  24)  has been used  as
    a blank filter activity  content which has  been subtracted from
    the gross analytical result to  obtain the  reported "net  result".
    No blank subtractions have been made  for  the  three radionuclides
    (radium-228, pol onium-2!l 0, and  lead-210)  which are at the analyti-
    cal minimum detectable  activity (MDA) level.   The net results  for
    the stack effluent discharge  radioactivity concentrations are
    reported in Table 25.
    
         The 100 Calciner Scrubber  and the 100 Ammophos  Reactor
    stacks were sampled, but the  sampling was  not done under iso-
    kinetic conditions.   Thus, these results  have not been reported.
    Assuming the results were not grossly in  error (sampling was 25
    and 35 percent outside  of isokinetic), the concentrations of
    activity in these stacks (uranium-238 chain)  were around 1  pCi/m3
    The flow rates for these stacks were  similar  to those given for
    the data in Table 25, indicating that a large proportion of the
    *Research Appliance Corporation  (RAC),  Gibsonia, PA.
                                    52
    

    -------
    effluent  was  not missed.   That is, more radioactivity is accounted
    for by  the  Mill Stacks  and TSP Dryer  than by the  Calciner Scrubber
    and Ammophos  Reactor.
    
    TABLE 24.  RADIOACTIVE CONTENT OF BLANK GLASS FIBER  FILTER (2.5-INCH DIAMETER)*
                       (pCi/filter ±  two-sigma counting error term)
    5- Filter
    Radionuclide Composite
    Ra-226
    Po-210
    U-234
    **
    U-235
    U-238
    Th-230
    Th-232
    Pb-210
    Ra-228
    0.52 ± 0.14
    0.29 ± 0.11
    0.060 ± 0.038
    <0.0012
    <0.026
    <0.075
    <0.080
    No data
    <0.81
    0.
    0.
    0.
    0.
    0.
    0.
    0.
    <0.
    
    6- Filter
    Composite
    42
    058
    022
    001
    025
    089
    029
    088
    No
    +
    +
    +
    2±
    +
    +
    +
    
    0.
    0.
    0.
    0.
    0.
    0.
    0.
    
    16
    015
    018
    00079
    017
    040
    023
    
    data
    Average Blank Extrapolated ++
    Filter Content Filter Content
    0.47 ± 0.21
    0.17 ± 0.11
    <0.041
    <0.0012
    <0.026
    <0.082
    <0.055
    <0.088
    <0.81
    0.
    <0.
    0.
    0.
    0.
    0.
    0.
    <0.
    <0.
    14 ±
    066
    039 ±
    001 4±
    031 ±
    078 ±
    051 ±
    13
    62
    0.
    
    0.
    0.
    0.
    0.
    0.
    
    
    035
    
    012
    00039
    0078
    031
    0078
    
    
    ''Average 2.5-inch filter mass ± two standard deviations of 0.2159 ± 0.0050 grams.
    **U-235 calculated based on natural U-235 to U-238 activity ratio of
      1:21.45 (0.0466).
    + Average of the 5-filter and 6-filter composite results.
    ++Extrapolated value based on area ratio between 2.5-inch and 4-inch diameter
      filters of 0.391 times the 4-inch diameter activity content (Eadie and
      Bernhardt, 1976).
         Table  25 presents  the stack  results in units  of picocuries
    per cubic meter.  These can be converted to discharge rates  by
    multiplying by the stack flow rates  given in  the  footnote.   These
    values  can  then be related to the  total  plant  process by multiply-
    ing by  the  number of  similar stacks.   It has  been  assumed  that the
    various  stacks have similar discharge parameters  (i.e., there
    were  four  200 Mill Stacks but only  one  such  stack was sampled).
                                       53
    

    -------
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    -------
         It is emphasized that there are considerable uncertainties
    in estimating releases,  especially annual  releases,  from single
    short-term samples.   Such estimates  are only a general  indication
    and are impacted by  variations between stacks, analytical  uncer-
    tainties,  daily variations in the operations of the  plant,  etc.
    Thus, without additional  verification, release estimates probably
    have at least an order of magnitude uncertainty.   Based  on  the
    reported data, the annual releases are estimated  to  be about 5 to
    10 mCi  for the uranium-238 chain nuclides  (uranium-238 through
    lead-210).  The lead-210  estimates could be somewhat higher than
    this, based on the previously mentioned uncertainties in the
    lead-210 data.  The  higher levels of lead-210 may be related to
    its volatility in the calcining and other  heating processes.  The
    low levels (compared to  lead-210) of polonium-210 in the stack
    effluents  are not readily explainable, given the  volatility of
    polonium.   It is possible a discharge point for polonium-210 was
    overlooked.
    
         The stack sampling  data for the 200 Mill and the 200 Phos-
    phoric  Acid Scrubber indicate somewhat higher concentrations of
    lead-210 and radium-226  than for the other nuclides.  Uranium-234
    and -238 and thurium-230  appear to be present in  similar quanti-
    ties as the radium-226 and lead-210 for the TSP Dryer stack
    sample.
    
         The estimated stack  discharges of uranium, thorium-230,
    radium-226, and lead-210  for the wet process plant are of the
    same order of magnitude  (millicuries per year), but  generally a
    bit lower  than those estimated for a thermal phosphate plant
    (ORP/LVF,  1977).  The two plants processed similar volumes  of ore
    (1 to 2 million tons per  year), but produced different products
    (i.e.,  fertilizer for the wet process plant and elemental  phos-
    phorus  for the thermal process plant).
                                   55
    

    -------
         The highest stack discharges from this plant,  both pCt/m3
    and pCi/sec, were for the TSP Dryer.   Since this study, the air
    pollution control equipment for this  process has been upgraded
    (additional cyclone and scrubber), resulting fn significant
    decreases in the particulate and fluoride effluents and, undoubt-
    edly an associated reduction in the quantities of radioactivity
    discharged to the environs.
                                   56
    

    -------
                                 SUMMARY
    
         External gamma radiation measurements conducted in various
    working areas of the J.  R.  Simplot's Wet Process Plant near
    Pocatello, Idaho ranged  from background to 120 yR/h, including an
    estimated background level  of about 9 yR/h.   Ambient radon-222
    concentrations in several  buildings ranged from 0.14 to a high of
    1.9 pCi'/l. which was measured outside the Control  Room of the 300
    Phosphoric Acid Plant.   Out-of-doors, the ambient radon concentra-
    tion ranged from 0.23 to 0.31 pCi/1 in the Ore Loading and
    Unloading Area and the  Gypsum Pile, respectively.   These ambient
    radon concentrations are within expected ranges due to natural
    terrestrial background  sources alone.
    
         The highest airborne  particulate radioactivity was measured
    in the area of the #3 Calciner Building.  There the radium-226
    was 1.6 pCi/m3, and total  uranium was about 2.1 pCi/m3.  These
    airborne concentrations  are orders of magnitude greater than
    results obtained in the  Technical Building Library.
    
         Particle size characterization (of selected cascade impactor
    results) indicates geometric means of equivalent aerodynamic
    diameters of less than  one  micrometer, except for one value of
    six micrometers (values  ranged from 0.03 to 6.0 ym).  These
    values are within the expected ranges for atmospheric and indust-
    trial dusts.  The average  of all  cascade impactor sampling results
    indicated that roughly  52  percent of the arithmetic total airborne
    radioactivity was contained in the particle size fraction less
    than one micrometer.
    
         Difficulties in the radiochemfcal analysis of samples for
    lead-210, discovered subsequent to the completion of analysis of
    the reported samples, indicates up to an order of magnitude
    
                                    57
    

    -------
    uncertainty in many of the  reported  lead-210  and  polonium-210
    results.
    
         Stack sampling of representative effluent discharge  points
    showed radium-226 release concentrations  ranging  from 0.74±  0.29
    to 9.5 ±  1.6 pCf/m3.   Natural  uranium and lead-210 concentrations
    ranged up to about 15 pCi/m3.   Estimates  based on these results,
    the number of similar stacks,  and associated  stack flow rates
    indicate  annual discharges  of  about  5 to  10 mCi/year of lead-210,
    radium-226, and uranium-234 and -238, with lower  values for
    thorium-230 and polonium-210.
                                   58
    

    -------
                                REFERENCES
    
    
    BERNHARDT, David E.  (May 1976),  Evaluation of Sample Collection
    and Analysis Techniques for Environmental  Plutonium.  U.S.
    Environmental Protection Agency,  Technical Note ORP/LV-76-5.
    
    EADIE,  Gregory G,  R.F.  KAUFMANN,  D.O.  MARKLEY, R.  WILLIAMS  (June
    1976),  Report of Ambient Outdoor  Radon and Indoor  Radon Progeny
    Concentrations During November 1975 at Selected Locations in  the
    Grants  Mineral Belt,  New Mexico.   U.S. Environmental Protection
    Agency, Technical  Note  ORP/LV-76-4.
    
    EADIE,  Gregory G.  and D. E. BERNHARDT  (December 1976), Sampling
    and Data Reporting Considerations for  Airborne Particulate
    Radioactivity.  U.S.  Environmental  Protection Agency, Technical
    Note ORP/LV-76-9.
    
    EISENBUD, M. (1963),  Environmental  Radioactivity.  McGraw-Hill
    Book Company, New York.
    
    ELDER,  J.C., M.  GONZALES, and H.J.  ETTINGER (1974),  Plutonium
    Aerosol Size Characteristics.  Health  Physics. 27:45-53.
    
    (EPA, February 1977)  -  U.S. ENVIRONMENTAL  PROTECTION AGENCY
    (February 3-5, 1977), Report of  the Workshop on Issues Pertinent
    to the  Development of Environmental Protection Criteria for
    Radioactive Wastes.   Washington,  D. C.
    
    FEDERAL REGISTER.  Volume 36, No.  247 (December 23, 1971),
    "Standards of Performance for New Stationary Sources."  Also,
    Volume  41, No. Ill (June 8, 1976),  "Proposed Amendments to
    Reference Methods."
    
    GUIMOND, R.J. and S.T.  WINDHAM (August 1975), Radioactivity
    Distribution in  Phosphate Products, By-Products, Effluents, and
    Wastes.  U.S. Environmental Protection Agency, Technical  Note
    ORP/CSD-75-3.
    
    HARLEY, J.H. (1975),  "Environmental Radon," in The Noble  Gases,
    R.E. STANLEY and A.A. MOGHISSI,  eds.,  U.S. Government Printing
    Office, Washington,  D.C. pp. 109-114.
    
    HOLTZMAN, R.B. (1964),  "Lead-210  (RaD) and Polonium-210 (RaF)  in
    Potable Waters in Illinois," in  The Natural Radiation Environment
    J. A.S. ADAMS and W.M.  LOWDER, eds., The University of Chicago
    Press,  Chicago,  pp 227-237.
                                   59
    

    -------
    JOHNS, F.B.,  ed.  (February 1975),  Handbook of  Radiochemical
    Analytical  Methods.   U.S.  Environmental  Protection  Agency,
    EPA-680/4-75-001.
    
    JOHNSON,  Raymond  H.,  Jr.,  D.E.  BERNHARDT,  N.S.  NELSON and
    H.W. GALLEY,  Jr.  (November 1973),  Assessment of Potential  Radio-
    logical Health Effects for Radon in Natural  Gas.
    U.S. Environmental  Protection Agency,  EPA-520/1-73-004.
    
    KAPLAN, Irving (1958), Nuclear  Physics.  Addison-Wesley Publishing
    Company,  Inc.  Reading, Massachusetts,  U.S.A.
    
    KNUTH, R.  H.  (1976),  Calibration of the  Sierra  High Volume Slotted
    Cascade Impactor.   HASL-Technical  Memo 76-6.
    
    LEE, R. E.  JR. (1972), The Size of Suspended Particulate Matter
    in Air:  Science.  178:567-575.
    
    (NCRP, January 1971)  - NATIONAL COUNCIL  ON RADIATION PROTECTION
    AND MEASUREMENTS,  NCRP Report No.  39 - Basic Radiation Protection
    Criteria.   Washington, D.C., p. 135.
    
    (NCRP, November 1975) - NATIONAL COUNCIL ON RADIATION PROTECTION
    AND MEASUREMENTS,NCRP Report No. 45 -  Natural  Background Radiation
    in the United States. Washington,  D.C.,  p. 163.
    
    OAKLEY, D.T.  (1972),  Natural Radiation Exposure in  the United
    States.  U.S.  Environmental Protection Agency,  ORP/SID 72-1.
    
    O'BRIEN,  K. and R.  SANNA (1976), Absorbed Dose-Rates in Humans
    from Exposure to  Gamma Rays.  Health Physics 30:71-78.
    
    (ORP/LVF,  1977),  Radiological Surveys  of  Idaho  Phosphate Ore
    Processing - The  Thermal Process Plant,  ORP/LV-77-3  (November,
    1977).  U.S.  Environmental Protection  Agency,  Office of Radiation
    Programs  - Las Vegas  Facility.
    
    PEARSON,  J.E.  (May 1967),  "Natural Environmental  Radioactivity
    from Radon-222."   Environmental Health Series,  U.S.  Public Health
    Service Publication No. 999-RH-26.
    
    POET, S.E., H.E.  MOORE and E.A. MARTELL  (1972), "Lead-210,
    Bismuth-210 and Polonium-210 in the Atmosphere."   J. Geophys Res.
    77, 6515.
    
    SEDLET, J., N.W.  60LCHERT  and T.L. DUFFY  (1973),  Environmental
    Monitoring at Argonne National  Laboratory - 1972, USAEC Report
    ANL-8007,  Argonne,  Illinois.
    
    STATE OF IDAHO (June  1, 1977),  Technical  Policy Memorandum No. 7-
    Concerning the Use of Radium-Contaminated Phosphate  Slag in
    Idaho.
                                    60
    

    -------
    SWIFT, J.J., J.M.  HARDIN and H.W.  GALLEY (January 1976),  Potential
    Radiological Impact of Airborne Releases and Direct Gamma Radia-
    tion to Individuals Living near Inactive Uranium Mill  Tailings
    Piles   U.S. Environmental Protection Agency, EPA-520/1-76-001.
    
    UNITED NATIONS (1972), Ionizing Radiation:   Levels and Effects,
    Vol. 1: Levels.   (A report of the  United Nations Scientific
    Committee on the Effects of Atomic Radiation for the General
    Assembly.)   New York.
    
    U.S. PUBLIC HEALTH SERVICE (1969), Evaluation of Radon-222 Near
    Uranium Tailings Piles, DER 69-1.   U.S.  Department of Health,
    Education,  and Welfare, Rockville, Maryland.
    
    WILLEKE, K. (1975) Performance of  the Slotted Impactor.   Presented
    at 15th American Industrial Hygiene Conference, Minneapolis,
    Minn., June 1975.   Mechanical Engineering Department, University
    of Minn.,  Minneapolis, Minn.
    
    WINDHAM, S., J.  PARTRIDGE and T. HORTON  (December 1976),  Radiation
    Dose Estimates to  Phosphate Industry Personnel. U.S. Environmental
    Protection  Agency, EPA-520/5-76-014.
                                    61
    

    -------
               APPENDIX-A
    RADIOCHEMICAL ANALYTICAL METHODS
    

    -------
                                APPENDIX-A
    
    RADIOCHEMICAL ANALYTICAL METHODS
         All  analyses were completed at the Environmental  Monitoring
    and Support Laboratory in Las Vegas, Nevada (EMSL-LV).  The
    following sections present brief descriptions of the analytical
    methods employed for this study.  Specific details of the pro-
    cedures are contained in the Handbook of Radiochemical Analytical
    Methods.  F. B. Johns, ed. (1975).
    
    Analysis  of Radium-226, Radium-228 and Lead-210
    
         A sequential method for the determination of radium-226,
    radium-228, and lead-210 in environmental  samples has been
    developed by the EMSL-LV.  This method is  initiated by the
    precipitation of radium from the sample aliquot using barium
    sulfate.   Barium-radium-sulfate is then dissolved in a diethylene-
    triaminepentaacetate disodium solution and transferred to an
    emanation tube and the radon allowed to come to equilibrium,
    approximately 30 days ingrowth with its parent - radium.
    Radium-226 (Tij = 1602 years) decays by alpha emission to radon-
    222 (Tij = 3.8 days).  Radon-222, a noble gas, is then collected
    from the  liquid by a de-emanation technique.  Radon-222 is
    usually counted for 30 minutes by alpha scintillation at four and
    one-half  hours after the de-emanation step to allow for the
    build-up  of the daughters.
    
         The  solution from the radium-226 determination is saved and
    the total radium is reprecipitated.  Radium-228 (Tj, = 6.1 years)
    is a beta emitter and decays to actinium-228 (Ti, = 6.13 hours).
    The actinium is allowed to ingrow for three days and is extracted
    with diethylhexylphosphoric acid and back  extracted with nitric
    acid.   The actinium-228 is beta counted for 30 minutes in a low-
    level  beta counter.
    
         Lead is also precipitated with the radium sulfate in the
    original  solution.  Advantage is taken of  the 30-day storage, for
                                    63
    

    -------
    radon-222 ingrowth,  to allow the bismuth-210  to  grow  in.   Lead-
    210 (Tjj = 20.4 years)  decays by beta  emision  to  bismuth-210
    (Tjj = 5.01  days).   The bismuth-210 is precipitated  from the
    supernatant liquid in  the radium-228  separation  step.   Bismuth is
    converted to an oxide, dissolved in nitric acid, mounted  on a
    two-inch planchet  and  beta counted for 30 minutes.
    
         As noted in the text of this report, subsequent  to the
    analysis of the samples reported in this report, it was found
    that the lead-210  recovery was less than expected.   This  is
    discussed in Appendix  C .
    
    Analysis of Isotopic Uranium and Thorium
    
         Samples are decomposed utilizing techniques of nitric-
    hydrofluoric acid  digestion, potassium fluoride  fusion or igni-
    tion.  The residues are dissolved in  dilute nitric  acid and
    successive sodium  and  ammonium hydroxide precipitations are
    performed in the presence of boric acid to remove fluoride and
    soluble salts.  The hydroxide precipitate is  dissolved, the
    solution is adjusted to 9N. in hydrochloric acid, and uranium is
    absorbed on an cnion exchange column, separating it from thorium.
    Iron is removed from the column by washing with  hydrochloric acid
    and the uranium is eluted with dilute hydrochloric  acid.   The
    thorium is converted to a nitrate form and absorbed on the same
    anion exchange column  separating it from calcium and other inter-
    ferences.  The thorium is then eluted with 9J1 hydrochloric acid.
    The uranium is electrodeposited on stainless  steel  discs from an
    ammonium sulfate solution and subsequently counted  by alpha
    spectrometry.  Usually 1000-minute counting times are used for
    analysis.  Chemical yields are normally determined  by the recovery
    of internal tracer standards (e.g., uranium-232  and thorium-234)
    added at the beginning of the analysis.
                                     64
    

    -------
    Analysis of Polonium-210
    
         Samples are decomposed by digestion with hydrofluoric acid
    and nitric acid in the presence of lead carrier and a polonium-
    208 tracer.  Polonium is co-precipitated with lead sulfide from a
    dilute acid solution separating it from calcium, iron, and other
    interferences.   The sulfide precipitate is dissolved in dilute
    hydrochloric acid and polonium is spontaneously deposited on a
    nickel disk.  Polonium-210 and polonium-208 tracer are measured
    by alpha spectrometry.  Usually, 1000-minute counting times are
    used for analysis.
    
    Polonium-210 Activity Estimations
    
         Due to the time delay between sample collection and radio-
    chemical analysis for poloniurti-21 0,  the following considerations
    have been utilized to estimate the polonium-210 activity in a
    sample.
    
         1.    Polonium-210 decays with a radiological half-life of
              138 days.  Therefore, a decay correction factor should
              be considered for samples  which are held for a rela-
              tively long period  between collection and analysis.
    
         2.    Concurrently, there will be some polonium-210 ingrowth
              from  lead-210 and bismuth-210 contents of the original
              sample during the elapsed  time between collection and
              analysis.
    
              The consideration of radioactive series transformations
              is discussed in  detail in  Kaplan (1958)   For the
              specific case of lead-210, the decay scheme is as shown
              in Figure A-l.  The solution of the system of differen-
              tial  equations,  which describe this lead-210 decay
              series, was derived by Bateman and is summarized here.
                                   65
    

    -------
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                             66
    

    -------
    a.   For polonium-210 ingrowth from lead-210. in  the original  sample:
    
         APb «
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         Where
    
         APo = P°lonium~210 activity at time  of  measurement  due
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         Apb = lead-210 activity at time of  sample  collection
           t = Elapsed time (in days) between sample
               collection and analysis
         Since the bismuth term is negligible and allowing for typical
         values of t, the following simplification  of the  above
         expression results:
    
         apb - A°  M m    i nc Q-0.00501tN
         ApQ = Apb (1.01  - 1.06 e         )
    b.   For polonium-210 ingrowth from bismuth-210 in the original
         sample:
    
         A^ = 0.0377 A° e-°-00501t- 0.0377  A° e'0-1381
          rO           Dl                    bl
         Where
    
          Ri
         Apo = polonium-210 activity at time  of  measurement  due  to
               ingrowth from bismuth-210 in  sample.
         An- = bismuth-210 activity at  time  of sample collection
    
         This term is insignificant for typical  values of  t  and  even  in
         the case of the complete decay of bismuth-210,  the  polonium-210
         ingrowth factor would be less  than  four percent  (i.e.,  decay
         constant for polonium-210 divided by the decay  constant for
         bismuth-210 equals 0.036).
                                67
    

    -------
    c.    The polonium-210 decay correction  term:
    
         «Po   .0  -0.005QK
         APo " MPoe
         Where
          Po
         ApQ = polonium-210 activity at time of measurement due to decay
               of original polonium-210 in  sample.
         ApQ = Original  polonium-210 activity in the sample at time of
               collection.
         Therefore, the polonium-210 activity at the time of measurement
         (Ap ) is the summation of the two  source terms (i.e. due to the
          ingrowth from lead-210 and due to the decay of the original
         polonium-210 in the sample).
    
         A   = APb + APo
         MPo   MPo   MPo
         or
         a   - a°  n m   i n* 0-0.00501tx .  flO  -0.00501t
          Po    Pb ''   ' "                '   "Po
    
    d.    Due to the relatively long half-life of lead-210 (T^ = 20.4
         yea1"*), the lead-210 activity at the time of measurement (Apb)
         is essentially equivalent to the original Pb-210 activity in
         the sample (Ap. ).  Solving the above expression for the original
         polonium-210 activity in the sample at the time of collection
         (A°Q) yields:
         All reported polonium-21Q analytical results are calculated
         values obtained from the above equation.  Whenever the apparent
         polonium-210 content from its ingrowth from lead-210 exceeds
         the measured polonium-210 activity, a non-detectable (ND) value
         has been reported.
                                68
    

    -------
    e.   The estimated counting error term associated with thts calcu-
         lated polonium-210 activity is simply the sum of squares of the
         individual  counting error terms, or:
                                            .
            MPo               APo    MPb
    
         Where
    
         aflo  = Estimated counting error term of the calculated
           Po
                polonium-210 activity in the sample at the time of
    
                collection.
    
         a.   = Counting error term of the measured polonium-210 activity.
          APo
    
         a.   = Counting error term of the measured lead-210 activity.
          APb
    
         In the tables, the estimated counting error terms at the 95
    
         percent confidence level (i.e., twice a.o  ) have been included
                                                 Po
         for the calculated polonium-210 activities.
    
         Throughout this report, the symbol for less than (<) has been
    
         used to indicate the equivalence of the error term (at the 95
    
         percent confidence level) to the reported result.
                                69
    

    -------
                   APPENDIX-B
          AIRBORNE PARTICULATE SAMPLING
    
    
    
    
    
    GROSS RADIONUCLIDE CONCENTRATION RESULTS
                       70
    

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                     APPENDIX C
    
    
    
    
    
    
    
    
    UNCERTAINTIES IN LEAD-210 AND POLONIUM-210
    
    
    
    
    
                   AIR SAMPLE DATA
                        77
    

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                                APPENDIX  C
    
       UNCERTAINTIES IN LEAD-210 AND  POLONIUM-210  AIR  SAMPLE  DATA
    
         Tables C-l  and C-2  present  a tabulation of  the  polonium-210
    concentrations,  as of time of analysis,  and  lead-210 concentra-
    tions, as of the time of collection,  for air samples listed  in
    Tables 11 to 20  of the text.  This tabulation  can  be used to
    assess the uncertainty associated with  individual  lead-210
    results and to estimate  the correct value.
    
         Comparison  of lead-210 interlaboratory  duplicate results
    (ORP/ LVF, 1977) and special method evaluation samples indicates
    that the EMSL lead-210 results for solids and  air  samples may  be
    underestimated by up to  a factor of five or  more.   Due to the
    delay of about 280 days  between  sample  collection  and analysis
    for polonium-210, the polonium-210 values are  generally indicative
    of the lead-210  collected in the sample.  That is, while  the
    polonium-210 collected in the sample would  have  decayed to 25
    percent of its level 31:  time of  collection  prior to  analysis,  the
    ingrowth of pol oni um-2"i 0 from lead-210  collected in  the sample
    would have reached about 75 percent of  the  lead-210  value.  Thus,
    the polonium-210 at time of analysis would  be  indicative  of the
    lead-210 (within 50 percent) under the  range of  extreme conditions
    of a polonium-210:lead-210 ratio of one-tenth  (normal ambient,
    NCRP, 1975) to three.
    
         Therefore,  the true lead-210 concentrations should fall
    between the reported lead-210 values and the polonium-210 values
    of time of collection (Tables C-l and C-2).   Furthermore, with
    minor exceptions, the lead-210 values should be  near the  high
    side of the range indicated.
                                    78
    

    -------
         The notable exceptions  are cases  where  the  polonium-210
    concentrations are excessively above the  reported  lead-210  values
    (e.g.,  about an order of magnitude).  Specifically,  the  sample
    from the #3 Calciner Area (from Table  12)  indicates  that the
    polonium-210:  lead-210 ratio was probably  greater  than  three and
    thus,  especially  for this Calciner sample,  it  appears  the
    polonium-210 in this sample  at time of analysis  was  primarily due
    to polonium-210 collection,  and not due to ingrowth.   For this
    sample  the best estimate for lead-210  is  about  0.70  pCi/m3  or
    less (up to about five times the reported  lead  value).   For the
    remaining air sample results,  although there is  some  evidence of
    elevated polonium-210, the individual  sampling  results  are
    insufficient to clearly denote even the positive presence of
    polonium-210 (beyond that ingrown from the lead-210).   That is,  a
    polonium-210:1ead-210 ratio  of up to four  at time  of  analysis for
    these  data (if analysis is at  280 days after collection) can be
    solely  due to a factor of five error in the  lead-210  analysis and
    75 percent ingrowth of polonium-210 from  the lead.   Although such
    a situation of elevated lead-210 with  no  polonium-210  is not
    likely,  much of the data are insufficient  to demonstrate that it
    could  not occur.
    
         In  summary, the best estimates for the  lead-210  values are
    the polonium-210 values at time of analysis, except  for  the value
    denoted  above.  The polonium-210 values can  only be  approximated
    as discussed above.
                                   79
    

    -------
           TABLE C-l.   ESTIMATED UNCERTAINTY FOR LEAD-210 IN  AIR FILTERS*"1"
     Referenced Table/               Reported Lead-210       Polonium-210 at  Time
    Location Description                (pCi/m3)           of Analysis  (pCi/m3)
    Table 11
    Grinder Mill No. 7                0.19  ± 0.068             0.30  ±  0.041
    Ore Unloading and Storage         0.24  ± 0.071             0.11  ±  0.033
    Gypsum Pile                       0.076 ± 0.006             0.11  ±  0.015
    Table 12 - Calciner Area
    Control Room                      0.077 ± 0.065             0.20  ±  0.04
    #3 Calciner                      <0.14                      2.5   ±  0.27
    Table 13 - 300 Phosphoric Plant
    Above Digester                    0.82  ± 0.40              0.53  ±  0.13
    Outside Control Room              0.36  ± 0.13              0.24  ±  0.047
    Continuous Filter                 0.18  ± 0.14              0.16  ±  0.052
    Control Room                      0.16  ± 0.12              0.22  ±  0.088
    Table 14
    TSP Storage Area                  0.12  ± 0.079             0.13  ±  0.029
    TSP Dryer                         0.68  ± 0.12              0.83  ±  0.084
    Acidulation TSP Discharge         0.14  ± 0.094             0.094 ±  0.026
    Table 15
    200 Ammophos Plant   Dryer        0.34  ±0.014             0.15  ±0.068
    100 Ammophos Plant - Dryer        0.16  ± 0.14              0.16  ± 0.14
    Table 16
    Library                           0.048 ± 0.014             0.025 ± 0.0063
    200 Ammophos Plant-Storage        0.17  ± 0.091             0.12  ± 0.0063
    100 Ammophos Plant-Storage        0.14  ± 0.094             0.093 ± 0.056
         These data are gross results prior to blank filter activity subtraction.
         The statistical uncertainty of values as expressed by the two-sigma
         counting error must be considered in comparing values.  For example,
         5 ± 2 is not statistically greater than 3 ± 1.  Furthermore, counting
         error does not include other analytical and sample collection uncertain-
         ties.
                                           80
    

    -------
           TABLE C-2.   ESTIMATED UNCERTAINTY FOR LEAD-210 IN  AIR  FILTERS*"1"
    
    Referenced Table/                Reported Lead-210      Polonium-210  at  Time
    Location Description                (pC1/m3)           of Analysis  (pCi/m3)
    Table 17. Ore Unloading Area
    Filter 1
    2
    3
    4
    5
    Final filter
    Table 18. Calciner Building
    Filter 1
    2
    3
    4
    5
    Final filter
    Table 19. 200 Ammophos Plant
    Filter 1
    2
    3
    4
    5
    Final filter
    Table 20. Gypsum Pile
    Filter 1
    2
    3
    4
    5
    Final filter
    
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         These data are gross  results  prior to blank filter activity subtraction.
    
         The statistical  uncertainty of values as  expressed by the two-sigma
         counting error must be considered  in  comparing  values.   For example,
         5 ± 2 is not statistically greater than 3 ± 1.   Furthermore,  counting
         error does not include other  analytical and sample collection uncertain-
         ties.
                                          81
    

    -------
    TECHNICAL REPORT DATA
    (Please read Instructions on the reverse before completing)
    1. REPORT NO.
    ORP/LV-78-1
    4. TITLE AND SUBTITLE
    Radiological Surveys
    Processing - The Wet
    2.
    of Idaho Phosphate Ore
    Process Plant
    7. AUTHOR(S)
    9. PERFORMING ORGANIZATION NAME AND ADDRESS
    Office of Radiation Programs - Las Vegas Facility
    U.S. Environmental Protection Agency
    P. 0. Box 15027
    Las Vegas, NV 89114
    12. SPONSORING AGENCY NAME
    Same as above
    AND ADDRESS
    3. RECIPIENT'S ACCESSION NO.
    5. REPORT DATE
    April 1978
    6. PERFORMING ORGANIZATION CODE
    8. PERFORMING ORGANIZATION REPORT NO.
    10. PROGRAM ELEMENT NO.
    11. CONTRACT/GRANT NO.
    13. TYPE OF REPORT AND PERIOD COVERED
    Final
    14. SPONSORING AGENCY CODE
    15. SUPPLEMENTARY NOTES
    16. ABSTRACT
          Radiological  surveys conducted  at the J.  R.  Simplot's Wet Process Plant in
     Pocatello,  Idaho indicate slightly elevated ambient levels of natural  radio-
     activity.   Compared to an estimated  natural background annual dose equivalent rate
     of about 79 mrem,  net gamma dose rates ranged  from 42 mrem in general  plant areas to
     152 mrem per work  year (2000 hours)  on the ore piles.  Ambient radon-222 concentra-
     tions,  ranging from 0.14 to 1.9 pCi/1, were measured in various indoor locations.
     Elevated airborne  radioactivity concentrations were measured in several work areas,
     with polonium-210  and radium-226 being the most predominant radionuclides of the
     natural  uranium decay series.   Particle size characterization indicates roughly 52
     percent of  the arithmetic total radioactivity  is associated with the particle size
     fraction less than one micrometer equivalent aerodynamic diameter.  Stack sampling
     results also show  thau appreciable concentrations of the naturally-occurring
     radionuclides are  being discharged into the local environs.  In general, the dose
     estimates and the  interpretation of results have been oriented toward evaluating
     the maximum potential impact of the plant on the environment; however, no attempt
     has been made to determine the annual  average  dose to workers within the plant from
     all exposure pathways.
    17.
    KEY WORDS AND DOCUMENT ANALYSIS
    a. DESCRIPTORS
    Phosphate, Natural Radioactivity
    Radium, Radon
    Gamma Radiation
    Particle Size
    Airborne Radioactivity
    18. DISTRIBUTION STATEMENT
    Release to public
    b. IDENTIFIERS/OPEN ENDED TERMS
    Phosphate Industry
    Environmental Surveys
    Radiation Surveys
    19. SECURITY CLASS (This Report/'
    Unclassified
    20. SECURITY CLASS (This page)
    Unclassified
    c. COSATl Field/Group
    1806
    1807
    1808
    21. NO. OF PAGES
    92
    22. PRICE
    EPA Form 2220-1 (Rev. 4-77)   PREVIOUS EDITION is OBSOLETE
    

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