PxEPA
           United St.-

           Age i
           Office of Radiation Pro
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                                                EPA-520/6-82-019
                                                November 1982
   EMISSIONS OF NATURALLY  XCURRING RADIOACTIVITY
        STAUFFER ELEMENTAL PHOSPHORUS PLANT
                 Vernon E. Andrews
         Office of Radiation Programs-LVF
       U.S. Environmental Protection Agency
             Las Vegas, Nevada  89114
                        and
                  Project Officer
                     Tom Bibb
    Emission Standards and Engineering Division
       U.S. Environmental Protection Agency
   Research Triangle Park, North Carolina  27711
This report was prepared with the technical  support
  of PEDCo Environmental Inc. contract 68-12-2811
 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  constitutes
neither endorsement nor recommendation for  their  use.
                                      n

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                                   FORWARD


    The  Office  of  Radiation   Programs   (ORP)   of  the   U.S.   Environmental
Protection Agency (EPA) conducts a national program for  evaluating  exposure  of
humans to ionizing and nonionizing radiation.  The  goal  of this  program  is  to
develop and promote  protective  controls  necessary to ensure the  public  health
and safety.

    In response  to  the 1977  amendments  to  the  Clean  Air Act  the Las  Vegas
Facility was  given  the responsibility to  collect field  data  on emissions  to
the  atmosphere  of   natural  radioactivity  from  operations  involved  in  the
mining, milling, and smelting  of minerals other  than  uranium and  coal.   This
report  is  one  of  a  series which  describes  an  individual  facility and  the
associated radioactivity emissions.

    ORP encourages readers of the report to  inform  the  Director,  ORP-Las Vegas
Facility, of any omissions or errors.  Comments or  requests for  further  infor-
mation are also invited.
                                       Wayne A. Bliss, Acting Director
                                       Office of Radiation Programs
                                       Las Vegas Facility

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                                   CONTENTS
                                                                          Page
Forward	iii
Figures	   vi
Tables	   vi

    1.  Background	    1
    2.  Introduction  	    3
    3.  Summary	    4
    4.  Plant Operations  	    5
            Product Flow	    5
            Emission Points 	    8
    5.  Sample Collection and Analysis	   10
            Sample Collection 	   10
            Sample Analysis 	   12
            Data Reporting	   12
    6.  Sample Results	   13
            Process Samples 	   13
            Ambient Air  Samples	   13
            Emission Samples  	   18
            Radon Emanation Results  	   21
    7.  Population Distribution  	   25
    8.  Discussion of Results	   26

References	   28

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                                    FIGURES

Number                                                                     Page
  1  Uranium and Thorium Radioactivity Decay Schemes 	    2
  2  Stauffer Chemical Plant Location  	    6
  3  Stauffer Chemical Plant Flow Diagram  	    7
  4  Sampling Sites for Radon Emanation from Soil, Ore, and Slag 	   11
                                    TABLES
Number                                                                     Page
  1  Process Materials Radioactivity Concentrations 	 14
  2  Ambient Radon-222 Concentrations 	 15
  3  Ambient and Stack Particulate Radioactivity Concentrations 	 16
  4  Radon-222 Stack  Emissions   	 19
  5  Particulate Radioactivity  Emission  Rates 	 20
  6  Particulate Radioactivity  Annual Emission Rates  	 22
  7  Scrubber Removal  of  Radionuclides  	 23
  8  Radon-222 Emanation  Rates  from Soil,  Ore, and Slag 	 24
                                      vi

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                                   SECTION 1


                                   BACKGROUND
     The Clean Air Act,  as  amended in August  1977,  required the  Administrator
 of the Environmental  Protection Agency (EPA) to determine whether  emissions  of
 radionuclides into ambient  air should be regulated under the Act.   In  December
 1979 the  Administrator  listed  radionuclides  as  a hazardous  pollutant  under
 Section 112 of the Clean Air Act.

     The naturally occurring radionuclides most likely to be  emitted  in signif-
 icant  quantities  are those  in the  uranium-238  and  thorium-232  decay  series
 (Figure 1).   These radionuclides  and their daughter  products occur  naturally
 in widely  varying amounts   in  the soils  and  rocks  that make  up the  earth's
 crust.  Average  values  for  uranium-238  and thorium-232  in  soils are  approx-
 imately 1.8 ppm (0.6 pCi/g)  and 9  ppm  (1 pCi/g)  respectively  (1).   The  radio-
 activity concentration of  each  of the  daughter products  in  the two series  is
 approximately equal to that of the uranium-238 or  thorium-232 parent.

     Almost all operations  involving  removal  and  processing of soils and rocks
 release some of  these  radionuclides  into  the   air.    These  releases  become
 potentially  important when the materials  being  handled contain  above-average
 radionuclide concentrations  or  when  processing concentrates the  radionuclides
 significantly above the average amounts  in soils  and  rocks.

     Because mining and milling operations  involve  large  quantities of  ore,  and
 because there  is  little information  about how these activities release  radio-
 active emissions, EPA, in 1978, began to  measure  airborne radioactive emissions
 from  various  mining, milling,  and  smelting  operations.   These  surveys  were
 screening  studies designed to  identify important sources of  airborne emissions
•of radionuclides at individual facilities.

     Operations were selected for study on the basis of  their potential  to emit
 significant quantities of naturally occurring  radionuclides  to  the atmosphere.
 Some of the  factors  in  the selection included typical  mine size, annual  U.S.
 production, measured  working levels of  radon daughters  in underground  mines
 and associated  ventilation rates, production  rate and  process  of  individual
 facilities, and  previous  association with  naturally occurring radionuclides.
 Usually, we chose to look  at  large facilities  in  order to  improve the chances
 of  obtaining  emission  samples  with   radioactivity   contents   significantly
 greater than background.

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              URANIUM - 238 DECAY SERIES
THORIUM - 232 DECAY SERIES
ro
238
U
4 BxlO'yr
a
234
Th
24 da


234
Pa
6 75 hr

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                                   SECTION  2


                                 INTRODUCTION
    As early  as  1908 it  was  recognized  that  phosphate rock  contained above-
normal concentrations of  uranium and  thorium  (2).  Those  concentrations  have
been  observed  in the United  States  to  range  from  8  to  399  ppm  (2.7  to 133
pCi/g) of uranium-238 and 2 to  19  ppm (0.22 to 2.1  pCi/g)  of  thorium-232  (3).
South  Carolina ores  had  the  highest  concentrations,  while  the  lowest  were
found in Tennessee.   During the 1950's uranium was recovered as a byproduct of
phosphate production.

    Since  1974  the EPA  has  studied  various  aspects of the  radioactivity
released to plant environs during  benefication and processing  of the phosphate
ores.  The EPA had  conducted  a comprehensive radiological  survey of a thermal
phosphate  (elemental  phosphorus)  plant   in  1975   (4).    However,  problems
associated with  the  analyses  for  lead-210 had greatly  reduced the accuracy of
the measurements of  both  lead-210 and polonium-210.  Under the added emphasis
provided by the  Clean  Air Act Amendments  the  decision  was made  to include at
least two elemental   phosphorus plants  in  this  series of surveys.  The first of
the  plants  surveyed was  the  Stauffer  Chemical  Company plant in  Silver  Bow,
Montana.

    PEDCo  Environmental,  under contract  with EPA,  conducted  the  survey and
collected samples  (5).   Before the survey,  representatives of  PEDCo Environ-
mental  and  EPA visited the  plant  to select  sampling  locations.   During the
period  October  15-31,   1979   PEDCo   Environmental, accompanied  by  an   EPA
representative,  conducted the  sampling  and  measurement   program,  collecting
particulate and  gas  samples  from  plant  effluents and  ambient air  as  well  as
information  on  plant  operations.    Stauffer   provided   meteorological  data
collected by one of their  meteorology stations.

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                                   SECTION 3


                                    SUMMARY
    PEDCo Environmental collected samples of  participate  and  gaseous emissions
from all  controlled  sources at  the  Stauffer  Chemical Company  plant.   Ambient
particulate and  gaseous samples were  collected  at a  site  1.6  km east of  the
plant.   Radon-222  emanation rates were measured  from soil around  the  plant,
from an ore storage pile, and the slag pile.

    The kiln stacks  emitted essentially all of  the  radioactivity emitted  from
controlled sources.  They accounted for  99  percent of the lead-210,  97 percent
of the polonium-210,  and  98 percent  of the radon-222.   Annual  emission  rates
of  the three  radionuclides from  all  stacks were  measured  at  280  mCi  for
lead-210, 200 mCi  for polonium-210,  and  8.2  Ci  for  radon-222.   An  additional
estimated release  of  1.2  Ci/y  of  radon-222  is produced  by  ore in  storage.
Annual emission  rates  of  uranium-238  and  -234,  thorium-230,  and  radium-226
were measured  at  an  average amount  of 0.22  mCi  for each radionuclide.   The
estimated release  of each  of  those radionuclides,  based on  measured  mass
emission  rates  and   assuming   that   the  radioactivity  concentration  in  the
emitted particulates  was  the same as  in  the  materials handled by the process
was 4.2 mCi/year.

    The  radon  emanation rate from the slag  pile,  with  an average  radium-226
concentration of 27  pCi/g was  3.5 ±  3.7 pCi/m^-min;  much  less than  the  soil
emanation rate  of 18 * 9  pCi/m^-min.   The  average  emanation  rate  from  the
ore pile was 117 ± 138

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                                  SECTION 4


                               PLANT OPERATIONS
PRODUCT FLOW


    The Stauffer Chemical Company Silver  Bow  Plant  is  located  in the community
of Silver Bow, approximately 11 km west  of Butte, Montana  (Figure  2).   Ore is
delivered  by rail  from a  mine  in   Idaho.   The  plant  product is  elemental
phosphorus.  A by-product is  ferrophosphorus (FeP), which  is  sold  as  a steel
alloying  additive.   The other  solid  product is  slag, which  can  be either  a
by-product or  a  waste product.   Stauffer sold  their  slag  for use  as  highway
aggregate  until  shortly  before  this   survey.    Pending   further  radiation
studies, Stauffer voluntarily withdrew their slag from the market.

    Figure 3  is  a schematic of the plant operation.   Ore  rail cars  are dumped
into  a  pit  from  which  ore  is  moved   to  one  of two  large  storage  piles
(Figure 4).   The process of ore  blending  begins  at  this point  as  the  ore
stockpile  is  built  up by layers.  One  pile  is  built  while ore  is  drawn from
the other  pile.   Because of the  severe  winter  weather, ore is  shipped during
the summer and stockpiled for year-round  use.

    The  ore  is  further  blended when it is  recovered  from the  stockpile  and
moved into a pit where it is transferred  by hoppers in the kiln feed building.

    It  is  necessary  to form  the  finely  divided ore  into   larger,  stable
agglomerates for  proper  operation of the reduction furnaces.   This is accom-
plished  by passing  the ore  through  two rotary kilns  at  about  1300°C.   The
temperature  of  the  ore  is  raised  to  its  incipient  melting  point  and  the
tumbling action  forms  the ore  into the  desired  nodular form.   The hot nodules
'pass through coolers and crushers before  being conveyed to storage silos.

    The furnace  feed  consists  of  a mix  of ore nodules, silica rock, and coke.
A  proper  fraction  of silica is required to form slag with  the  necessary flow
properties  to facilitate  removal from   the  furnace.   The  content  of silica
occurring naturally  in  the  ore must  be  augmented with added  silica.   Coke is
added  as a  carbon  source  to  reduce the calcium  phosphate ore  to elemental
phosphorus.  The approximate reaction is:

             2Ca3(P04)2 + 10 C  + 6 Si02 —»  P4  + 10 CO + 6  CaSi03

Nodules, coke, and silica are fed from storage  silos  by means  of a  proportion-
ing belt  and skip hoist  to  "burden   bins"  which provide a  continuous  feed to
the furnaces.

    Feed material enters the electric arc furnaces  from the top and progresses
downward until reaching the molten layer  on the bottom.  Phosphorus  and CO are

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1-90
                           Stauffer
                           Chemical
                           Plant
                 KILOMETERS
              0              1
           Figure 2.  Stauffer Chemical Plant Location

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                                       it Emission/Sampling Point
Figure 3.  Stauffer  Chemical  Plant  Flow Diagram

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driven off  as  gases and are  piped  off near the top of  the  furnace.   The slag
and  FeP  which  are  continually  collecting in  the furnace are  periodically
tapped off.   FeP  is tapped  for about 20  minutes  each  8-hour shift.  Slag  is
tapped (or flushed) in an 80  to  90  minute  operation  about  seven  or eight times
per 24-hour period.  FeP is  cooled  and crushed for shipment.  Slag is disposed
of on site.

    The  product gases  through an electrostatic  precipitator where particulate
contaminants  are  removed,  and  then  through a  spray tower  where  water  sprays
cool the phosphorus to  below the condensation  point.  The  molten phosphorus  is
filtered to  remove  any carry-over  particulates  and  piped  into  rail  tank cars
for shipment.  The  remainder of the gas stream, primarily CO, is  used as fuel
in  the kilns.   Sludge resulting  from the  phosphorus  filtering  operation  is
roasted  to recover any  residual  phosphorus.  Roaster  residue  is spread  in  a
6-inch layer  on the stockpile prepared for winter use to  prevent  the damp ore
from freezing  in  the pile and hampering recovery.


EMISSION POINTS


    Oust generated while conveying  ore to  the  kiln feed  building  hoppers  is
collected  by a hooding  system.   The  air is  discharged through a wet scrubber.

    Exhaust gases from the  rotary  kilns  are cleaned by multiple  air cleaning
devices  which  remove both particulates and  fluorine.

    Exhaust gases from the nodule coolers  are treated  by  two sets of multiple
air cleaning devices to  remove particulates.

    Emissions  occurring within  the  kiln  building from  materials  handling and
coke  drying  are  collected  by the  ventilator  collector  system.   This   system
exhausts through  two sets of multiple  air  cleaning devices.

    Emissions  arising  from  transfer  to   and  storage  in  the  burden bins  of
nodules,  coke, and  silica are  collected  by  a  hooding system  and  discharged
through  a  wet  scrubber.

    A  small  amount  of  phosphorus  is  released  during  slag and  FeP tapping.
Upon  oxidizing  in  air  the  phosphorus  forms  a  dense  white  cloud of Po05
fumes.   Collecting  hoods   intercept  most   of  the   P205   fumes   and  other
emissions  and  discharges them through  the  tap  hole fume  scrubber.

    With  the  installation  of  air  pollution  control  systems on  most  of the
sources  of particulate emissions,  the visible  emissions  during the period of
the survey originated  from two primary sources.   One  is a  periodic  release of
some  of  the fumes  produced during furnace  tapping.  The  other  source  is the
nodule storage silo  area.   Material  handling at the burden  bins generates con-
siderable  dust which  exits  the building  through roof  ridgeline ventilators.
No  satisfactory  method has  been  devised  to control these dust  emissons.  The
point of emission is also inaccessible to  sampling.
                                       8

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    Other  potential  sources of  airborne  radioactivity were  the ore  storage
piles and  slag  piles.   These were  considered as  possible sources  of  gaseous
radon-222.

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                                  SECTION 5


                        SAMPLE COLLECTION AND ANALYSIS
SAMPLE COLLECTION


    Most  samples  were  collected  using  EPA  reference  methods  (6).    Stack
sampling points were  selected  according  to EPA Method  1.   Stack gas velocity
and  volumetric  flow rate were  determined by  EPA  Method 2.   Gas  samples  for
radon analysis were collected using EPA Method 3.  (Radon in this report  means
radon-222).   Total  suspended particulates (TSP)  in  ducts  and exhaust stacks
were  determined  using  EPA  Method  5.   High  volume  ambient TSP  samples   were
collected  in  accordance with  the  Reference  Method  for  the   Determination  of
Suspended Particulates in the Atmosphere  (7).

    PEDCo  collected  Method   5  TSP  samples on  7.6-cm  (3-inch) diameter  glass
fiber filters.  Ambient TSP  samples were  collected on  20.3- by 25.4-cm (8- by
10-inch) Microsorban  polystyrene fiber  filters.   Stack  gas  and ambient  whole
air samples for radon analysis were collected  in  30 liter Tedlar bags.

    PEDCo  sampled  each  of the emission  points described  on  page 8 except  the
silo  fugitive emissions.  They  collected  two  to four  samples  each  of TSP  and
gas samples from each  point.  These points are shown in Figure 3.  Where more
than  one  exhaust of  a given type existed, such  as  kiln  exhausts, they only
sampled one.  At two  locations  it  was possible to obtain simultaneous  samples
from  the inlet and outlet of an emission control  system.

    Radon  emanation  rates from the  surface  of  the  ore  pile   and  surrounding
soil  areas was measured at  the locations shown in Figure 4 by means of  char-
coal  canisters.   U.S.  Army  M-ll  gas canisters  containing  activated  charcoal
were  placed on the surface  to collect radon  gas  emitted.  The canisters were
left  in position for the duration  of the survey.   Radon emanation rates from
the  slag  pile  were  measured  using  inverted  tubs  sealed  to  the   surface
(Figure 4).   The tubs were  sealed to  the slag pile using  dry bentonite clay
powder moistened  in place.   A valve and gas  cock  in  the  bottom  of  the  tub
permitted the collection of  air samples  at the time  of  placement and  after an
elapsed time  of 2 to 3 hours.   The  change  of  radon concentration  in  the
53-liter  tub  made  it  possible to calculate  the  rate  of  emanation  from  the
surface beneath the tub.

    Samples  of  process  materials  were collected   to  relate  radionuclide
emission rates to  the radioactivity of  the material  handled  at each  emission
point and to permit a radionuclide balance through the process.
                                      10

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                                   ®
                       COUNTY ROAD
                                   PLANT
                                              ORE
                                              ORE
                                        SLAG
                                       'PILE
         PLANT BOUNDARY
              Approximate Scale
       LEGEND
(7) Soil Background
|T] Slag Pile Sample
       0    0.2   0.4  0.6   0.8   1.0
                 Kilometers
Figure 4.  Sampling Sites for Radon Emanation from Soil, Ore,  and Slag

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SAMPLE ANALYSIS


    PEDCo made  mass  determinations on  TSP  samples before  forwarding them to
Eberline Instrument  Corporation  (EIC)  for radiochemical  analysis.   Stack and
ambient  gas  samples  were  shipped  to  EIC  for  arrival  within   2   days  of
collection.

    EIC  analyzed  process   and  TSP  samples  by  dissolving  the  samples  and
separating  the  elements of  interest  by  chemical  techniques.   The  separated
uranium  and  thorium  fractions  were  counted  on  alpha   spectrometers  for
individual  isotopic quantitation.   An alpha scintillation counter measured the
polonium-210.  Lead was separated  and set aside for about 2  weeks to  allow for
ingrowth  of  bismuth-210  from  lead-210.   After  the   ingrowth   period  the
bismuth-210 was  separated from  the lead and was counted  on  a beta counter to
quantitate  lead-210.   Radium  was   separated  and enclosed  as a  solution  in  a
sealed tube to allow for ingrowth  of radon  from radium-226.  After 3  weeks of
ingrowth the  radon gas was  evolved and  collected in  an alpha scintillation
cell to  be  counted.   Stack  and  ambient gas  samples  were transferred  to  alpha
scintillation cells and counted  for radon.

    The  EPA's  project  officer collected  the  slag  pile radon samples  directly
into evacuated alpha scintillation cells and counted  for radon the  same day.

    PEDCo shipped  the  radon  emanation canisters  by  air express   to  the  EPA
Eastern  Environmental  Radiation Facility  in Montgomery, Alabama.   EPA analyzed
the canisters  on a gamma spectrometer and reported  the results as radon  flux
(emission rate per  unit area) from the surface.


DATA REPORTING


    The  radioactivity  reported for  each sample,  except for  charcoal canisters,
is the net radioactivity plus or minus  twice  the standard deviation (2s)  based
on  counting statistics.  The net  radioactivity is the  gross  sample radio-
activity minus counter background  and  (1) for  filter samples, minus an average
value for the  radioactivity content of  a  blank filter, or  (2)  for  stack  radon
samples, minus  the ambient  radon  concentration.  The  counting  variation,  plus
the variable  radioactivity  content of  individual  blank  filters,  occasionally
results  in   a  net  radioactivity   of  less  than 0.    Of  course,  there  is  no
negative radioactivity.  In these  cases,  as with all others, the net negative
results must be considered along with the 2s uncertainty.

    The  sample  standard  deviation  is based  only  on  the  random variations
inherent in  radioactivity counting and is propagated  only  in those situations
of  either duplicate  emission  samples  or  samples describing  process materials.
This  uncertainty  is  not  propagated when samples are collected  at  different
times  yet  are combined  to  describe a  source average.   In  these  cases  where
multiple samples are averaged,  the standard  deviation is calculated  from the
variance in the samples.   Since  there is  no adequate  way of  describing  the
variability  in  daily emissions   for  the   control   technology,   the  annual
emissions have no  associated error term.
                                      12

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                                  SECTION 6


                                SAMPLE  RESULTS
PROCESS SAMPLES


    The  average  concentration  in  ore  of  radionuclides  of  the  uranium-238
series was 32 pCi/g  (Table  1).   The apparent  departures from  secular  equilib-
rium reported for the individual nuclides of the uranium series  in  ore samples
are due primarily to  a  combination of  statistical  variations  in counting  and
analytical  biases.   Uranium  was  above  the normal  concentration  in  rock  by
about a factor of 50.  The thorium series was  at a  normal concentration level.

    Although a large  fraction  of  the ore was  removed as  elemental  phosphorus
and oxygen,  the  radionuclide concentrations in  slag are  similar to  those  in
ore due  to the  diluting  effect of  the added  silica.   The major  differences
between ore and slag concentrations are  for lead-210  and polonium-210, both of
which are  volatilized and driven  off during processing.   Radionuclide concen-
trations in the nodules show  that  about half  the lead-210  and essentially all
of  the  polonium-210  are  lost during  calcining.   The rest  of  the  lead-210  is
lost during the thermal  reduction process.  FeP contains significant concentra-
tions of  uranium-234  and  -238.   However, the  FeP  is produced in much smaller
quantity than slag and most of the  uranium  is  found  in  the slag.  Radionuclide
concentrations  in  the  four slag  pile  samples  are   in  very  close  agreement,
reflecting the uniformity of blended feedstock and  overall  operations.


AMBIENT AIR SAMPLES


    Radon-222 concentrations  measured at the  background station are  shown  in
Table 2.   The  samples collected from 1440  to  1758  hours on October 17  and on
October 18 were collected during periods when  the  wind  direction was primarily
from the plant to the sampling  site.  All other samples were  collected during
periods when the sampling site  was either upwind or  crosswind from the plant.
No  effect  of plant operation  is apparent from the  results  and all  samples are
considered to  represent ambient concentrations.  Ambient  radon  concentrations
vary from  less  than  0.1 to about  1  nCi/m3, depending on time of day, season,
and meteorology (1).

    Three  filters from  the background  high volume samplers were analyzed for
ambient particulate radioactivity concentrations.  The results are in Table 3.
The measured concentrations of  the  uranium, thorium,  lead, and radium isotopes
are comparable to those found throughout the United States   (1).  The polonium-
210  concentrations   of   0.020  and  0.029  pCi/m3  in the  October  18-21  and
October 26-28 samples are an order of magnitude higher than the normal  back-


                                      13

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TABLE  1.   PRXESS MATERIALS RADIOACTIVITY CONCENTRATIONS
              Radioactivity Concentrations (pC1/g)a
Material
Phosphate Ore
Phosphate Ore
Average^
Nodules
Coke 0
Silica 0
Fresh Slag
Fresh Slag
Average*3
Ferrophosphorus
Ferrophosphorus
Averageb
Slag, Drum Site 1
Slag, Drum Site 2
Slag, Drum Site 3
SI ag, Drum Site 4
Average*3
U-238
29 * 3
24 * 2
27 ± 2
26 * 2
.24 * 0.10
.14 * 0.07
26 * 2
25 ± 4
26 * 2
11 * 3
10 * 3
11 * 2
20 ± 2
26 * 2
22 ± 2
26 * 2
24 * 1
a Picocuries (10~12 curies)
U-234
29 ± 3
23 * 2
26 * 2
26 * 2
0.31 * 0
0.24 * 0
26 ± 2
25 ± 4
26 ± 2
7.6 ± 2
9.6 * 3
8.6 * 1
20 * 2
26 ± 2
22 ± 2
26 * 2
24 * 1
per gram
Th-230
54 * 11
24 * 6
39 * 6
51 * 11
.12 0.31 * 0.29
.09 0.48 * 0.31
54 * 13
46 * 14
50 * 10
.1 0.56 * 0.44
.1 0.45 ± 0.38
.9 0.51 * 0.29
37 ± 8
58 * 18
46 ± 18
39 * 8
45 * 7
plus or minus the
b Counting statistic standard deviation propagated to
Ra-226
31 * 9
21 * 6
26 * 5
21 * 6
0.11 ± 0.
0.18 * 0.
31 ± 9
28 * 8
30 ± 6
0.35 * 0.
0.39 ± 0.
0.37 * 0.
24 ± 7
29 * 9
21 * 6
Pb-210
41 *
34 *
38 *
22 *
03 0.52 *
05 0.55 *
0.53 *
-1.4 *
-0.4 *
11 0.79 *
12 0.67 *
08 0.73 *
1.3 *
1.5 *
1.7 *
34 * 10 2.6 *
27 * 4
standard
1.8 ±
deviation
2
2
1
2
0.76
0.78
0.90
1.8
1.0
0.88
1.7
0.96
0.9
0.8
1.3
1.3
0.6
based
Po-210
33
38
36
2.7
0.3
-0.3
0.0
1.8
0.9
-0.9
0.6
-0.2
6.8
1.1
1.4
0.32
2.7
± 3
* 3
± 2
* 3.9
* 2.8
* 2.7
* 2.8
* 3.1
± 2.1
* 2.5
± 2.9
* 1.9
± 4.1
* 5.5
* 5.6
* 2.1
* 2.3
on counting
Th-232
0.20 * 0.23
0.32 * 0.30
0.26 * 0.19
0.06 * 0.13
0.06 * 0.13
0.04 * 0.09
0.76 ± 0.47
1.1 * 0.6
0.93 * 0.38
0.08 * 0.16
0.07 * 0.15
0.08 * 0.11
0.21 ± 0.21
0.36 ± 0.28
0.42 * 0.28
0.57 * 0.33
0.39 ± 0.14
statistics.
Th-228
0.20
0.84
0.52
0.06
0.06
0.04
0.43
0.07
0.25
0.08
0.07
0.08
0.21
0.95
0.73
0.58
0.62

± 0.23
± 0.50
± 0.28
* 0.13
± 0.13
* 0.09
± 0.21
* 0.14
± 0.13
* 0.16
± 0.15
* 0.11
* 0.21
* 0.71
* 0.59
* 0.41
± 0.26

average result.

-------
ground of  0.001  to  0.003 pCi/m3.  The  polonium-210 concentration of  0.0043  ±
0.0028  pCi/m3  is  in  the range  of  expected  background.    Using  the  hourly
average  wind speed  and  direction  data  provided  by  Stauffer  the  estimated
polonium-210 concentrations at the drive-in  theater  site  were calculated.   The
estimates  were  made  using a  Gaussian  plume diffusion  model  and  Pasquill's
diffusion categories (8).  The calculated concentrations for the three sampling
periods,  including   an  estimated  background of  0.001  pCi/m3,  were  0.027,
0.003,  and 0.001 pCi/m3.   Of the  first result,  0.021  pCi/m3  was  due to  a
1-hour observation with  an average wind speed of 0.8  km/h,  and  the  background
site was 1.6 km from the plant.  If that  1-hour  observation  is  not used in the
calculations  the predicted   concentration   becomes  0.006   pCi/m3.   From  the
calculations it  is  obvious  that  some  polonium-210  above background  would  be
expected  at the  drive-in theater  site  under  the  meteorological  conditions
observed  on October   19-20  and  27-28.   Considering  the  sensitivity  of  the
predictive  model  to  proper  selection  of stability factors and  precise  wind
direction  measurement,  the measured  values   for  polonium-210 concentration  are
believed to be valid.
                  TABLE 2.  AMBIENT RADON-222 CONCENTRATIONS
                                 Time                      Concentration

    Date                       On  -  Off                    (nCi/m3)a

   10/17                     0910  -  1418                   0.39 ± 0.10

   10/17                     1440  -  1758                   0.16 ±0.06

   10/18                     1032  -  1319                   0.32 ± 0.09

   10/18                     1320  -  1635                   0.20 ± 0.09

   10/22                     1058  -  1314                   0.13 ± 0.06


   10/22                     1315  -  1605                   0.12 ± 0.04b
   10/22                     1606  -  1859                   0.17 ± 0.05
a  Nanocuries (10~9 curies) per cubic meter plus or minus twice the
   standard deviation based on counting results only.

b  Derived from duplicate samples.
                                      15

-------
                     TABLE 3.   AMBIENT AND STACK PARTICULATE RADIOACTIVITY CONCENTRATIONS
                                                Radioactivity Concentrations (pCt/ni3)'
Time - Date
Source Collected
Ambient Air 2355 - 10/18
0022 - 10/21
Ambient Air 0026 - 10/26
0021 - 10/28
Ambient Air 0030 - 10/28
0049 - 10/30
Kiln Feed 0852 - 1032
Conveyor 10/30/79
Kiln Feed 1305 - 1510
Conveyor 10/30/79
Kiln 1 1324 - 1627
Scrubber Exhaust 10/25/79
Kiln 1 1718 - 1943
Scrubber Exhaust 10/25/79
Kiln 1 1046 - 1701
Scrubber Exhaust 10/26/79
Nodule Cooler 0940 - 1610
10/19/79
Nodule Cooler 0941 - 1612b
10/19/79
Nodule Cooler 0956 - 1225b
U-238
0.000049
0.00016
0.00014
-0.01
-0.01
0.34
0.32
0.19
0.36
0.05
-0.07
* 0.000076
* 0.00010
* 0.00010
* 0.22
* 0.21
« 0.20
« 0.20
» 0.20
* 0.26
* 0.18
* 0,18
U-234
0.00007
0.00014
0.00013
0.12
-0.02
0.45
0.17
0.10
0.28
0.05
-0.07
* 0.00013
* 0.00014
* 0.00014
* 0.30
» 0.28
* 0.26
* 0.24
* 0.25
* 0.31
* 0.24
* 0.24
Th-230
0.00008
0.00037
0.00010
-0.02
-0.03
0.26
0.42
-0.01
0.4
0.08
-0.02
* 0.00035
* 0.00039
* 0.00034
* 0.68
* 0.66
* 0.58
* 0.67
* 0.15
* 1.2
* 0.56
* 0.55
Ra-226
-0.00013
0.00001
-0.00006
0.03
0.10
0.45
0.39
0.40
0.63
0.06
0.20
* 0.00045
* 0.00043
* 0.00045
* 0.42
* 0.42
* 0.34
* 0.34
* 0.36
* 0.45
* 0.33
* 0.35
Pb-210
0.020
0.0074
0.0074
0.7
0.3
380
420
210
0.3
0.1
0-7
* 0.002
* 0.0023
* 0:0014
* 2.9
* 2.7
* 34
* 35
4 7
* 2.8
* 2.2
* 2.4
Po-210
0.020
0.029
0.0043
1.1
0.6
190
2bO
290
11
7.4
0.8
* 0.002
* 0.005
* 0.0028
* 1.4
* 1.3
* 27
* 28
* 14
* 3
* 1.8
* 1.1
Th-232
0.00007 *
0.00009 *
0.00008 *
-0.10 *
-0.12 *
-0.07 *
-0.06 *
-0.07 *
-0.08 *
0.02 *
-0.08 *
0.00024
0.00025
0.00025
0.44
0.42
0.33
0.35
0.36
0.45
0.39
0.36
Th-228
0.00008
0,00010
0.00009
-0.05
-0.05
-0.03
-0.02
-0.03
-0.03
0.06
-0.04
* 0.00018
* 0.00018
* 0.00018
* 0.42
* 0.40
* 0.32
* 0.34
* 0.35
* 0.43
* 0.38
* 0.34
(continued)

-------
  TABLE   3.    (Continued)
                                                                   Radioactivity Concentrations (pC1/m3)a
Source
Kiln Building
Ventilator
Kiln Building
Ventilator
Kiln Building
Ventilator
Silo System
Exhaust
51 lo System
Exhaust
Tap Hole
Fume Scrubber
Tap Hole
Fume Scrubber
Tap Hole
Fume Scrubber
Collected
1305 - 1553
10/19/70
0955 - 1225
10/24/79
1000 - 1224
10/24/79
1015 - 1221
10/29/79
1421 - 1624
10/29/79
1550 - 1805
10/16/79
0935 - 1145
10/17/79
1435 - 1637
10/17/79
I
0.37

0.36

0.29

0.23

-0.06

0.01

-0.04

-0.01

J-238
* 0.29

* 0.32

* 0.20

* 0.21

* 0.14

* 0.14

* 0.14

* 0.14

U-
0.37

0.51

0.29

0.32

-0.06

0.04

-0.06

-0.01

-234
* 0.32

* 0.41

* 0.23

* 0.26

* 0.18

* 0.18

* 0.18

* 0.18

	 Th-230
0.51

1.3

0.29

0.39

-0.03

-0.01

-0.02

-0.02

* 0.77

* 1.1

* 0.44

* 0.68

* 0.43

* 0.41

* 0.41

* 0.43

Ra-226
0.57 *

0.77 *

0.42 *

0.77 *

-0.11 *

-0.10 *

-0.04 *

-0.18 *

0.37

0.51

0.29

0.39

0.26

0.25

0.25

0.26

Pb 210
1.3

0.02

0.5

1.2

0.7

0.6

7.9

4.2

* 2.2

* 3.2

* 1.7

* 2.0

* 1.8

* 1.7

* 1.1

* 0.8

Po-210
0.19 * 0.94

-0.4 * 1.4

-0.14 * 0.69

0 * 1.5

0 * 1.2

0 * 0.75

15 * 5.4

3.1 * 3.9

Th-
-0.02

-0.11

-0.06

0.05

-0.08

-0.06

-0.07

-0.06

•?32
* 0.34

* 0.49

* 0.25

* 0.35

t 0.26

* 0.26

i 0.26

* 0.27

Th-
0.01

0.06

-0.03

0.08

-0.05

-0.03

-0.04

-0.03

228
* 0.33

* 0.47

* 0.24

* 0.34

* 0.25

* 0.25

* 0.25

i 0.26

a Picocuries  (10~^ curies) per cubic meter plus or minus twice the  standard deviation based on counting results only.




  Results derived from duplicate samples.

-------
EMISSION SAMPLES


    Radon sampling results are shown in Table 4.   Gross concentrations measured
in  the  stacks,  net  concentrations  above the  measured ambient  concentrations
and  average  concentrations are  given  along with  the  derived annual  emission
rates.  Annual emission  rates  were  calculated assuming full-time operation  of
the  process  and annual  average  concentrations equal  to  the  average  obtained
from the samples.

    Two sources, the kilns and the  silo  system exhaust, had average concentra-
tions which  were  significantly  different  from  ambient.    Net  average  radon
concentrations  were  12   ± 11   and  0.12  ±  0.17  nCi/m^  respectively.    The
associated annual  releases were  8.2 and 0.034 curies.   Thus, the  kilns  were
responsible for  essentially all the  radon emitted from the plant  stacks.

    Particulate  radioactivity  concentrations measured  in  stack  emissions  are
given in Table  3.   These concentrations are calculated using  the  radionuclide
activity  on  the  filter  media  and  the  sample  volume  corrected  to  stack
conditions.   Using  these  values,   the  stack  emission  rates   (pCi/sec)  were
determined and  summarized in  Table 5.  These rates  are  calculated  from  the
ratio of the  stack flow rate  (in  standard ft^/hr,  dry)  to the sample volume
(standard  ft^,   dry).    Specific   stack  test   and  sample  parameters   are
contained in the emission  test report  (5).   PEDCo Environmental  has calculated
and summarized these ratios or "scaling factors."

    Radioanalytical  results for  the kiln  feed conveyor  exhaust samples  were
not  significantly  different   from  zero.    PEDCo  reported  an   average  mass
emission rate from this  source  of  0.98 pounds per  hour  (0.12  g/sec).   Using
the  measured  radioactivity in  ore, each  of  the uranium  chain radionuclides
should have been emitted at the  rate of 4  pCi/sec from the  kiln feed conveyor
exhaust.

    The emission rates of  uranium-238  and -234,  thorium-230, and radium-226 in
the  kiln  scrubber  exhaust averaged   about  3.6  pCi/sec.    Emission rates  of
lead-210 and  polonium-210 from  the kiln scrubber  exhaust  were 4,500 pCi/sec
and 3,200 pCi/sec, respectively.

    Measured  concentrations  and  emission  rates  of  uranium-238  and  -234,
thorium-230, radium-226,  and  lead-210  from  the  nodule cooler did  not differ
significantly from zero.   Based  on  the  measured mass emission  rates and radio-
activity of  the nodules  the  best   estimate  of the  release rates  of  each  of
those radionuclides  would be  2.7 pCi/sec.   Only polonium-210 was  measured  at
concentrations  significantly  above  zero.   The  average  emission  rate  was
50 pCi/sec.

    The kiln  building ventilator  is  the major  controlled   source  of particu-
lates.  As a consequence it was  also the major source  of  uranium-238 and -234,
thorium-230, and  radium-226.   Emissions of  each  of those  radionuclides  plus
lead-210 averaged 15 pCi/sec.
                                      18

-------
                  TABLE 4.  RADON-222 STACK EMISSIONS
                                     Concentration  (nCi/m3)3
                                                                 Annual
Source
Kiln Feed
Conveyor


Kiln



Time
1106 -
1320 -
1041 -

0930 -
1328 -
1025 -

1320
1623
1309

1328
1555
1358

Date
10/18
10/18
10/22d
Source
10/18
10/18
10/22d
Source
Gross
0.36 ±
0.23 ±
0.22 ±
Average
14 ±
0.35 ±
22 ±
Average
0.13
0.11
0.04

1
0.14
1

Total for 2
Nodule
Cooler


1005 -

1627 -

1420

1829

10/18

10/22d
Source
0.33 ±

0.30 *
Average
0.09

0.05

Total for 2
Kiln
Building
Ventilator
1153 -
1623 -

1345
1823

10/18J
10/22d
Source
0.45 ±
0.16 ±
Average
0.13
0.04
0.
0.
0.
0.

0.


kilns
0.

0.
0.
Net1-
04
03
09
Ob
14
15
22
12

01

13
07
±
±
±
±
±
±
±
±

±

±
±
Release (Ci)
0.16
0.14
0.07
0.03
1

0.013

0.15
1

11



4.1
O"
0.13



0.07
0
.08
coolers
0.
-0.
13
01
0.06
Total for 2
Silo System
Exhaust

Tap Hole
Fume
Scrubber
1400 -
1646 -

0933 -
1413 -

1643
1846

1410
1740

10/22
10/22
Source
10/17
10/17
Source
0.12 ±
0.41 ±
Average
0.28 ±
0.23 ±
Average
0.09
0.04
venti
±
±
±
0
0
0
.16
.07
.10
lators
0.00
0.24
0.12
0.10
0.08
-0.11
0.07
-0.02
a Nanocuries (10~9 curies) per cubic meter.
b Radon-222 concentration in sample as collected plus
±
±
±
±
±
±
or
0
0
0
0
0
0
.10
.06
.!/
.14
.10
.13
minus
0.020

-------
                                     TABLE  5.   PARTICIPATE  RADIOACTIVITY  EMISSION  RATES
                                                           Radioactivity Emission Bates (pCl/sec)
Source
Kiln Feed
Conveyor
Ki In Feed


Kiln 1,
Scrubber Exhaust
Kiln 1,
Scrubber Exhaust
Kiln 1,


ro
o
Nodule Cooler

Nodule Cooler

Kiln Building
Ventilator
Ki IT Building
Venti lator

Silo System
Exhaust
Si lo System
Exhaust

Tap Hole
Fume Scrubber
Tap Hole
Fume Scrubber
Tap Hole
Fume Scrubber
Time - Date
Collected U-238
0852 - 1032 -0.13
10/30/79
1305 - 1510 -0.9
10/30/79
Average -0.11 * 1.6
1324 - 1627 4.6 * 2.7
10/25/79
1718 - 1943 4.3 « 2.7
10/25/79
1046 - 1701 2.5 * 2.6
10/26/79
Average 3.8 * 1.5

0940 - 1610b 1.9 * 1.5
10/19/79
0956 - 1225 -1.3 * 3.2
10/24/79
Source Average 0.30 * 1.8
1305 - 1553 7.6 * 5.9
10/19/79
0955 - 1225h 12 * 6.6
10/24/79
Source Average 9.8 * 4.5
1015 - 1221 2.5 * 2.2
10/29/79
1421 - 1624 -0.72 * 1.7
10/29/79
Average 0.89 * 1.4
1550 - 1305 0.2 * 2.6
10/16/79
0935 - 1145 -0.83 * 2.6
10/17/79
1435 - 1637 -0.15 * 2.5
10/17/79
U-?34 O!-230
1.2

-0.22

0.5
6.0

2.3

1.3

3.2

1.0

-1.3
-0.15
7.6

15

11
3.4

-0.72

1.3
0.70

-1.1

-0.15

* 3.0

* 2.8

4 2.1
* 3.5

* 3.3

* 3.2

* 1.9

* 1.8

* 4.3
* 2.3
* 6.6

* 8.6

* 5.4
* 2.8

* 2.2

* 1.8
* 3.4

* 3.4

» 3.3

-0.2R

-0.30

-0.26
3.5

5.7

-0.13

1.9

2.0

-0.33
0.84
10

28

19
4.1

0.41

2.3
0.25

-0.42

-0.35

* 6.7

* 6.5

* 4.7
4 7.8

4 9.0

* 1.8

* 4.0

4 5.8

4 9.9
4 5.7
4 16

4 21

4 14
4 6.1

4 5.1

4 4.0
4 7.7

4 7.9

4 7.7

Time-Weighted Averagec
Ra-226 Pb-210
0.27 * 4.2 7.2

1.0 4 4.2 2.7

0.64 4 3.0 5.0
6.0 * 4.7 5000

5.2 4 4.7 5800

5.2 4 4.5 2700

5.5 4 2.7 4500

3.0 4 2.6 1.9

3.6 4 6.2 13
3.3 4 3.4 7.5
12 » 7.6 27

21 4 n 9.0

17 * 6.7 18
8.2 4 4.1 12

1.3 4 3.2 7.9

4.8 4 2.6 10
1.9 * 4.6 12

-0.73 4 4.8 150

-3.3 4 4.7 75

43
4 28

4 27

4 19
4 470

4 480

4 100

4 230

4 17

4 43
4 23
4 44

4 63

4 38
4 22

4 22

4 16
4 32

4 21

4 15

4 13
Po-210
11 * 13

5.7 4 13

8.4 * 9.2
2500 * 14

3300 * 380

3800 4 180

3200 4 140

85 * 16

14 4 20
50 4 13
4.0 4 19

-9.0 4 28

-2.5 * 17
0 4 16

0 4 14

0 4 11
0 4 14

290 4 100

55 4 70
_
85 4 33
Th-232
-0.93 * 4.3

-1.2 4 4.2

-1.1 4 3.0
-0.97 4 4.5

-0.80 4 4.8

-0.88 4 4.7

-0.88 4 2.7

-0.24 * ?.8

-1.4 4 6.4
-0.82 4 3.5
-0.48 * 7,0

-3.1 4 9.7

-1.8 * 6.0
0.51 4 3.7

-0.96 4 3.2

-0.23 4 7.4
-1.1 4 4.g

-1.2 4 5.0

-1.2 * 4.9


rn-228
-0.45 4

-0.52 4

-0.49 4
-0.47 4

-0.28 4

-0.37 4

-0.37 4

0.45 4

-0.66 *
-0.11 4
0.28 4

0.45 '

0.37 4
0.88

-0.58

-0.15
-0.5

-0.68

-0.61


4.2

4.0

2.9
4.3

4.7

4.5

2.6

2.7

6.1
3.3
6.7

: 9.6

5.9
4 3.6

4 3.0

4 2.3
4 4.7

4 4. a

* 4.7


a Picocuries (10-'? curies) per cubic meter.
b Results derived from duplicate sample
c Emission rates of nuclides other than Pb-210 and Po-210 were insignificant.

-------
    The  average  emission  rates  of  the  uranium  chain  radionuclides,   less
polonium-210,  from  the  silo  system  exhaust  was  measured  at  3.8  pCi/sec.
Assuming that the particulate material  sampled  was  due to nodule handling and
that the radioactivity concentration  of the  particulates  was  the same as the
nodules, the average  emission rate  of each,  based  on  the mass emission  rate,
would be 3.1 pCi/sec, very close to  the measured radioactivity  emission rate.

    The collection period of each tap hole  fume scrubber  sample  included  times
when a  furnace  was being flushed  or  tapped.  Analysis  of  the data showed  that
the  primary source  of  lead-210 and  polonium-210  from  the  source  was FeP
tapping.  As shown  in Table 3,  the  concentrations  of  other radionuclides did
not differ significantly from zero and lead-210 and  polonium-210 concentrations
varied  widely between samples.   The  time-weighted average emission rates  based
on 2-days tap  and flush  records and the  three  sample  results  were  43 pCi/sec
for lead-210 and 85 pCi/sec for polonium-210.

    Table 6 shows  the  annual  emission  rates  calculated for  each  operation.
These  emission  rates include  the sum  of  two  kiln  stacks,  two  nodule  cooler
stacks,  and  two kiln building ventilator stacks.   Approximately  99  percent  of
the  lead-210 and  97 percent  of polonium-210  emissions   occur  from  the  kiln
stacks.  The process  sample  results  show that  essentially all of the  lead-210
and polonium-210  is  driven  off  in the kiln  and furnace.   The  observed differ-
ence  in kiln  annual  emissions  of 280  mCi   and 200 mCi,  may  be real, due  to
different removal  rates  in  pollution control equipment,   or may  be  an  artifact
of analysis.   The kilns also emit  several  tenths  of  a  curie  per year of the
other  uranium  chain radionuclides,  but  most of them -  about  1  Ci  per year  -
are released from the kiln building ventillator systems.

    The removal of  radionuclides by emission control systems  was determined  on
the number  1 kiln scrubber  and  the  tap hole  fume scrubber.  As  is  common with
kilns,  Stauffer uses  an  effluent control system of  multiple control  devices  in
series.  It was possible to obtain  simultaneous samples  on the  inlet  and out-
let of the  final stage  scrubber.   Simultaneous samples  were  also  obtained  at
the inlet and  outlet of  the tap hole fume  scrubber.   The results are  shown  in
Table  7.  The  kiln scrubber removed 75 percent  of  the total mass entering it.
The average removal  for  uranium, thorium, and  radium was  essentially  identical
at  78  percent.   Both  lead-210  and   polonium-210  showed   a 54  percent  removal.
Only   lead-210  and  polonium-210 could be  evaluated  in  the  tap  hole  fume
scrubber.   The fume  scrubber  removed  an  average  of   86  percent  of  those
nuclides, compared  to 91 percent of the mass.   Lead and polonium,  presumed  to
be  present  as  fumes after condensing from  vapors,  are apparently more readily
removed in  the tap  hole  fume  scrubber  than  in  the  kiln  scrubber  which  is
designed to remove  particulates.


RADON  EMANATION RESULTS


    Radon  emanation rates from soil around the plant  generally ranged from 12
to  31  pCi/m2-min with an average of 21 ±  6  (Table 8).   If  two low results of
2.0 and 4.2 pCi/m2-min  are included the  average   is 18  ± 9.   Radon  emanation
from  the top  of the  ore  pile  covered  with roaster  residue  average   53  ±  35
pCi/m2-min. Considerable difference was found  between the emanation rates


                                       21

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ro
                                  TABLE 6.   PARTICIPATE RADIOACTIVITY  ANNUAL  EMISSION  RATES
                                                         Annual Emissjon Rate (ff*C_i_/y)a
Source
Kil'i Fei'd
Conveyor
Kiln 1 plus
Ki'ln ?
Nodule Cooler 1
plus Nodule Cooler 2
Kiln Buildinq
Vent i 1 dtor
jl l;i Syilwi
F.xhaust
r,ip Hale
Fume Scrubber^
a ,, , ,3
h i •••isoruis of nuclidvs
U-2.W U-?34 Th-23U Ra-226 Pb-210
-0.003 * 0.050 0.016 » 0.066 -0.008 * 0.15 0.020 « 0.095 0.16 * 0.60
0.?4 » 0.09 U.20 * 0.12 U.12 * 0.25 0.35 * 0.17 280 * 15
0.02 « 0.11 -0.009 * 0.15 0.05 « 0.36 0.21 * 0.21 0.47 * 1.5
0.62 * 0.2(1 0.70 * 0.34 1.2 * 0.9 1.1 * 0.4 1.1 « 2.4
0.0?H « '1.04.1 U.0-11 * 0.057 0.07 » 0.13 0.!5 * 0.08 0.32 * 0.50
1.4 * 0.4


Po-210 Th-232
0.26 * 0.29 0.035 * 0.095
200 * 7 -0.06 * 0.17
3.2 * 0.8 -0.05 * 0.22
-0.16 * 1.1 -0.12 * 0,311
0 * 0.35 -0.007 t 0.076
-'.7 * l.fj


Th-22S
-0.015 * 0.091
-0.02 * tj.lfi
O.U07 i fj.21
U.02 * ll.yt
-o.uns * ''j.nn




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measured from  the east  berm of the  ore pile  and  the west  berm.   The  three
measurements from the east  berm averaged  310 ±  140  pCi/m2-min  while  those
from  the  west  berm  averaged  36 ±  20  pCi/m2-min.   No  explanation  has  been
found  to  explain  the  difference between  the  two  berms.   The  average  radon
emanation  rate  from  the ore  pile  was  110  ±  70  pCi/m2-min.    The  radon
emanation rate  from  the  ore pile in  use should have  been about equal  to  the
berm  average,  or  170  ±  140 pCi/m2-min.   Radon  emanation  rates  measured  on
the slag pile averaged 3.5 ± 3.7 pCi/m2-min.

    Radon emanation rates from soil were comparable  to those measured  at other
locations  in  the  United  States as  part of  this  survey, but  were below  the
reported National average value of 35 pCi/m2-min (9).

    It is estimated that the covered ore pile emits  radon at the rate  of 1.2 ±
0.8 pCi/min.  The uncovered  ore  pile  is  estimated to release radon  at  the rate
of 1.9 ± 1.5  pCi/min.  The  radon which would have been released from  the soil
beneath the ore piles was about  0.2 uCi/min.   The net radon  emanation  rate for
the two piles  would  be 1.0  ± 0.8 pCi/min or 0.53 Ci/year  for  the  covered pile
and 1.7 ± 1.5 yCi/min or 0.89  Ci/year for the pile in use.

    Radon  emanated from  the slag pile at  the rate  of 0.8 uCi/min  compared to
an emission  rate from the  soil beneath of  0.4 uCi/min.   The  radon  reduction
provided by the slag cover is  estimated  to be 0.32 yCi/min or 0.17 Ci/year.

    The net radon  emanation  rate from the  ore and  slag piles during the survey
was estimated at  1.2 Ci/year.   However,  during  part  of the year only a portion
of one ore pile would be  in  existence and  snow and  ice cover during the winter
would reduce the  radon emanation rate.
                  TABLE 7.  SCRUBBER REMOVAL OF RADIONUCLIDES
                                  Fraction  Removed  (Percent)	

                                           U,Th,Ra                    Pb,Po
Kiln 1
Kiln 1
Kiln 1
Average
71
85
69
75
59
93
87
80
76
85
100
87
59
81
69
70
66
86
81
78
37
68
57
54
58
66
38
54
48
67
48
54
75
74
76_
75
 Tape Hole Fume Scrubber

 Tape Hole Fume Scrubber

 Average
95     100

73      75_

84      88
98

74

86
100
 91
                                        23

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TABLE 8.   RADON-222 EMANATION RATES FROM SOIL,  ORE, AND SLAG


Site
1
2
3
4
5
6
7
8
9
10
11
12
Average





Soil
Emanation
Rate (pCi/m2^nin
18
17
22
18
4.2
12
24
28
13
25
2.0
31
18 * 9





Ore

Pile Slag Pile
Emanation Emanation
Site Rate (pCi/m2-min Site Rate (pCi/m2-min)
Top
1
2
3
4
5
Average

East Berm
6
7
8
Average
West Berm
9
10
11
Average

75 1 1.8
100 2 8.6
22 3 3.3
30 4 0.1
35 Average 3.5 ± 3.7
53 ± 34


150
390
380
310 ± 140

13
48
47
36 ± 20
                             24

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                                   SECTION 7


                            POPULATION  DISTRIBUTION
    The  Stauffer  Chemical Company  plant is  located in  a sparsely  populated
area.  The  processing facility is  situated,  as  shown  in Figure  4,  near  the
east center portion of a company-owned site about 1  mile  (1.6  km)  square  which
is fenced to restrict access.   Several ranches  are  located west of the plant,
with  the nearest  residence  in that  direction  being about  2 km away.    One
family  lives  at  the drive-in  theater  1.6  km  east of   the  plant.    Several
residences  are  occupied  in  Silver Bow  about 2.5  km northeast  and  about  50
people live in Ramsey, about  the same  distance to the north-northwest.
                                      25

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                                   SECTION 8


                             DISCUSSION  OF RESULTS
    As  mentioned   earlier,   analytical  biases   can   result   in   consistent
differences  in  activity  levels  between radionuclides  of  a  decay chain  that
would normally have very nearly the same radioactivity.   This can be  seen  in
the process sample  results of  Table 1  and kiln building  ventilator results  in
Tables 3, 5, and 6.   Radionuclides  of  the uranium decay  chain through  radium-
226 in ore, modules,  and slag and  probably in  ventilator exhaust particulates
should be at nearly equilbrium values.

    Other results reported by  EIC on known  activity  samples have shown  similar
biases with thorium-230  being  about twice  the  activity of the  other  samples.
Evaluation of those results  has shown that thorium  analyses by  EIC have  been
more accurate than  the others.  Therefore,  it  is  believed that the thorium-230
results  reported  for  the samples  mentioned  are more  representative  of  the
uranium chain  activities than  the  other radionuclides.   However, no  attempt
has  been  made  in  this  report  to  apply  any  correction  to  the data.   More
important than  the specific radioactivities  are the  fractions  of the  radio-
activity  in  the  process which  are  emitted  from  the  stack.  Since the  biases
are probably consistent, the fractional values are considered to be valid.

    A major environmental protection problem  associated with  thermal  process-
ing of  phosphate  is the  emission of fluorides to  the atmosphere.  To  combat
that  problem  and  control particulate  emissions  Stauffer  uses  multiple  air
cleaning  systems  in series  on its  kilns,  nodule coolers,  and  kiln  building
ventilators.  Although radioactive  emissions were not  a  consideration when  the
pollution control   system  was  installed,  it removed  large  fractions  of  the
particulate radionuclides and  smaller, but  still  significant,  fractions  of  the
more volatile lead-210 and polonium-210.

    Each  exhaust stack  emits a portion of  the  particulate material  controlled
by the exhaust system.   Due  to the above-average concentrations  of  naturally-
occurring radioactivity in  the process  materials  the   particulate  emissions
result  in  radioactive   emissions.   Most   of   the   radioactive  particulate
emissions from  controlled  sources  come  from  the  kiln   building  ventilator.
Next  in  importance is  the  kiln.   The  kiln  probably  generates  more  airborne
particulates,   but  because  of  the  more  complex  pollution  control   system
actually emits less than the ventilator.

    The average measured emissions  of  uranium-234  and -238,  thorium-230,  and
radium-226 from all controlled sources were  1.3  mCi/year.  A better  estimate
is probably derived  from the measured  mass emission rates.  Assuming  that  the
particulate material,  except for the  tap hole  fumes,  are  similar  to  ore  in
radionuclide concentration the calculated  total emissions of  each of the  four
radionuclides is 4.2 mCi/year.
                                      26

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    The nodule cooler and tap hole fume scrubber are  small  sources  of  lead-210
and polonium-210.  The kilns, however,  are the major source, releasing 99  and
97 percent, respectively, of the total  plant emissions of those  nuclides.

    As with lead-210 and polonium-210, the  kilns are  the  major  source  of  radon
emissions.  The average measured emission rate of 8.2 Ci/year may be low  since
it is based on results from four samples, one  of which  was  extremely low.   The
estimate of 1.5 Ci/year of radon from the ore  pile  is probably  an upper  limit,
considering the  actual  area of  the  ore  piles averaged  over  the year  and  the
effect of winter rain, snow, and ice on reducing emanation rates.

    Comparison of radioactivity removed by  the kiln scrubber  and tap hole fume
scrubber demonstrated that the fume scrubber removed the larger  fraction of  the
lead-210 and polonium-210 from the exhaust gases.  Within the limits  of  sampling
and  analytical  accuracy,  the  kiln  scrubber  removes  the  other,   nonvolatile
radionuclides in the same proportion as total suspended  particulates.   As  would
be expected for  a noble gas, no removal   of radon  was  exhibited  by  the  kiln
scrubber.

    Although  slag  was   found  to  contain  about  as  much  radium-226   as  the
original ore  it  was found  to not  be a source of  radon, as  is the ore.   The
physical form of the slag, even when somewhat  frothy  in appearance  reduces  the
rate at which  radon  gas  is able to escape.   Slag  pile sites sampled  included
slag which has been  in  place  for a few days to  several weeks so that at  some
sites the radon would have been  in  equilibrium with  radium-226.   Gamma  exposure
rates were significant on the slag pile,  averaging  0.15 milliroentgen  per hour
(mR/h).  Ambient background gamma exposure rates were  about 0.01 mR/h.
                                      27

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                                  REFERENCES
1.  National  Council  on  Radiation  Protection   and   Measurements.    Natural
    Background  Radiation  in  the  United  States,  NCRP  Report  No.  45,  1975,
    Washington, D.C.

2.  Habashi,  Fathi.   Uranium  in  Phosphate   Rock.   Special  Publication  52,
    Montana  Bureau  of Mines  and  Geology,  Montana  College of  Mineral  Science
    and Technology, Butte, Montana, December 1970.

3.  Menzel, F. G.   Uranium, Radium, and  Thorium Content in Phosphate  Rocks and
    their  Possible  Radiation  Hazards,  Journal  of   Agriculture   and  Food
    Chemistry, Vol. 16, No. 2, 1968, pp 231-234.

4.  Eadie, Gregory  G.,  and David  E. Bernhardt.   Radiological  Surveys  of Idaho
    Phosphate Ore  Processing  -  the Thermal Process Plant.   U.S. Environmental
    Protection   Agency,   Technical  Note   ORP/LV-77-3,  Las   Vegas,   Nevada,
    November 1977.

5.  PEOCo  Environmental,   Inc.  Emission test  report:  Collection of  Airborne
    Radon   and   Radioactive  Particulates  at   Stauffer  Chemical   Company,
    Silver Bow, Montana.   Cincinnati, Ohio, December 1979.

6.  Code of Federal Regulations, Title 40,  Chapter 1, Part 50, Appendix B.

7.  Code of Federal Regulations, Title 40,  Chapter 1, Part 60, Appendix A.

8.  Slade, David H.,  editor.  Meteorology  and  Atomic  Energy 1968.  U.S. Atomic
    Energy Commission, Oak Ridge,  Tennessee, July 1968.

9.  Turekian,  Karl  K.,  Y. Noyaki, and  Larry  K.  Benninger.   Geochemistry of
    Atmospheric  Radon   and   Radon  Products.    Annual   Review  of  Earth  and
    Planetary Sciences, 5:227-225, 1977.  Palo Alto, California.
                                      28

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                                   TECHNICAL REPORT DATA
                            (Please read Instructions on the reverse before completing)
1. REPORT NO.
    EPA-520/6-82-019
                              2.
                                                            3. RECIPIENT'S ACCESSION NO.
4. TITLE AND SUBTITLE
  Emissions of  Naturally Occurring  Radioactivity:
  Stauffer Elemental  Phosphorus Plant
             5. REPORT DATE
                 November 1982
             6. PERFORMING ORGANIZATION CODE
7. AUTHOR(S)
                                                            8. PERFORMING ORGANIZATION REPORT NO.
  Vernon E. Andrews
9. PERFORMING ORGANIZATION NAME AND ADDRESS
                                                            10. PROGRAM ELEMENT NO.
  U.S. Environmental  Protection Agency
  Office of Radiation Programs-Las Vegas  Facility
  P.O. Box 18416
  Las Vegas, Nevada   89114
              11. CONTRACT/GRANT NO.
12. SPONSORING AGENCY NAME AND ADDRESS
                                                            13. TYPE OF REPORT AND PERIOD COVERED
    Same as above
             14. SPONSORING AGENCY CODE
15. SUPPLEMENTARY NOTES
                      This is the third  in  a series of reports  covering work performed
  in response to  the  1977 Clean Air Act Amendments
16. ABSTRACT
     Naturally occurring radioactivity was  measured in the  atmospheric emissions  and
  process materials  of a thermal phosphate  (elemental phosphorus)  plant.  Represent-
  ative exhaust stack  samples were collected from each process  in  the plant.  The
  phosphate ore contained about 120 parts per million uranium.   The radioactivity
  emitted in greatest  quantity was radon-222 with an annual  release from the plant
  of  8.3 curies.  Emissions of lead-210  and polonium-210 were measured at 280 and
  200 mi Hi curies per  year.  Annual emissions of each of the other radionucl ides  of
  the uranium decay  chain were estimated to be 4.2 millicuries.  The slag pile was
  determined not to  be a source of radon.
 7.
                                KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
                                              b.lDENTIFIERS/OPEN ENDED TERMS
                           c. COSATI Field/Group
 Natural  radioactivity
 Airborne wastes
 Exhaust  gases
  Technologically
  enhanced
  radioactivity
   1808
   1302
   2102
18. DISTRIBUTION STATEMENT

  Release  to public
19. SECURITY CLASS (TIlis Report)
  Unclassified	
21. NO. OF PAGES
     28
                                               20. SECURITY CLASS (This page)

                                                Unclassified	
                                                                          22. PRICE
EPA Form 2220—1 (R«v. 4-77)   PREVIOUS EDITION is OBSOLETE

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