In
Vivo Measurement Sensitivity and Occurrence of Radionuclides
in Residents of the Carlsbad,
New Mexico Area
Introduction
Citizen volunteers from the Carlsbad,
New Mexico area were monitored for internally deposited radionuclides through
a project entitled "Lie Down and Be Counted" (LDBC). This project is provided as an
outreach service to the public to support education about naturally occurring
and man-made radioactivity present in people and the environment prior
to the opening of the Waste Isolation Pilot Plant (WIPP). The data collected
prior to the opening of the WIPP facility will provide information for
future studies and serve as a baseline for operational monitoring. In addition,
information obtained from these measurements will be used to evaluate and
reduce the uncertainties associated with bioassay methodologies. It is
important to note that these data represent an interim summary of an ongoing
study.
Methods
Following the commissioning of the
Center's in vivo monitoring facility, 272 citizen volunteers were
assayed during July 1997 to September 1998. These volunteers were recruited
through presentations to local community groups and businesses. When a
citizen volunteer arrived at the Center for a bioassay, he or she viewed
a short video explaining the measurement protocol, and completed a lifestyle
questionnaire which included questions regarding age, sex, ethnicity, occupation,
foreign travel, wild game consumption, smoking habit and any nuclear medicine
procedures
(Table
12). In addition, the subject's height and weight were recorded.
Measurement
System
Lung and whole body counts were simultaneously
performed with the subject positioned horizontally using two arrays of
hyper-pure Ge detectors. Each array consisted of four detectors and represented
a specific detector design, low energy (LEGe) and coaxial (COAX). The primary
function of the LEGe detector array was lung counting (7 to 250 keV). Each
LEGe detector was fitted with a 0.6 mm thick carbon composite entrance
window. The active diameter, area, and thickness of each LEGe detectors
as 70 mm, 3800 mm2, and 20 mm, respectively. The function of
the second detector array (COAX detectors) was to measure higher energy
photons (100 to 2000 keV) emitted from radionuclides deposited in the whole
body. The active diameter, length, and relative efficiency of the COAX
detectors were 75 mm, 76 mm, and 80%, respectively. The high energy (1333
keV) resolution performance of the LEGe detectors was matched to that of
the COAX and was added, using additional signal processing electronics,
to the signal from the COAX detectors to increase the sensitivity of the
whole body count.
The counting shield consists of a large
shielded room measuring 2.7 m wide, 3.0 m long, and 2.7 m high. It is constructed
from 25 cm-thick cast iron obtained from pre-World War II iron. A graded-Z
liner (Z represents the charge of the liner element) consisting of 64 mm
of lead, 32 mm of tin, and 32 mm of stainless steel was added to the inside
of the iron walls of the shield to attenuate photons produced within the
shield walls.
Radionuclides analyzed for in lungs
included 232Th,
144Ce, natural U, 235U,
226Ra,
233U,
155Eu,
210Pb,
237Np,
Pu isotopes, 241Am,
244Cm, and
252Cf.
Radionuclides analyzed for in the whole body included
40K,
51Cr,
54Mn,
58Co,
59Fe,
60Co,
65Zn,
88Y,
95Zr,
103Ru,
106Ru,
125Sb,
131I,
133Ba,
133I,
134Cs,
137Cs,
140Ba,
141Ce,
152Eu,
154Eu
and 192Ir (Table
13). A 30-min count time was used for each subject.
Data Analysis
The proprietary software package ABACOS
Plus from Canberra Industries was used for routine calibration, operation,
data analysis, and data archival. This software was specially developed
for in vivo applications and is currently employed at in vivo
facilities located at General Electric Nuclear, Wilmington, North Carolina;
Savannah River Plant, Aiken, South Carolina; Rocky Flats Environmental
Technology Site, Golden, Colorado; Oak Ridge National Laboratory, Oak Ridge,
Tennessee; Mound Site, Mound, Ohio; Fernald Site, Fernald, Ohio; and Lawrence
Livermore National Laboratory, Livermore, California.
The identification of radionuclides
of interest was accomplished using a library-driven peak search and a library-driven
region of interest (ROI) analysis. The concept of 'library driven' means
that only the portions of the spectrum that would contain the photons of
interest (usually listed in a library) are examined.
Peak Search
Analysis
A peak search was the first analysis performed
on the spectral data. In simplified terms, a peak was identified by approximating,
through a correlation function, the second derivative of each channel in
the spectrum (Canberra, 1991, Nuclide Identification Algorithms and
Software Verification and Validation Manual, 07-0464). When the algorithm
is sampling a portion of the spectrum that contains no peaks, the second
derivative should approach zero. When a peak is encountered, the second
derivative will become positive and remain so until an inflection point
is reached. At the inflection point, the second derivative will become
negative and increase to a very large negative value just past the apex
or centroid of the peak. When these conditions occurred within the spectrum,
a peak was considered identified. The peak ROI, background and net counts
were determined for identified peaks as described below.
Region
of Interest Analysis
A region of interest, centered at a given
photon energy, was established for all radionuclides regardless of whether
or not a peak was identified as described above. For radionclides that
were not identified by the peak search, the width of the ROI was determined
by multiplying a constant by the calibrated resolution of the spectrometer
at the photon energies of interest. Constants of 2 and 3 were empirically
determined and verified for radionuclides deposited in lungs and whole
body, respectively. Typical ROI widths for radionuclides in lungs were
25 channels and for radionuclides in whole body were 13. For radionuclides
identified by the peak search, the ROI width was determined as the channels
on both sides of the centroid, where the second derivative returned to
zero.
Background and net counts for each
ROI were calculated using a step-background computation. This computation
calculates the background counts for each channel (i) in the ROI
of interest (Bi) using the following equation:
where Yj is the total counts in channel
j,
L is the left starting channel of the ROI, R is the right ending
channel of the ROI, Lavg is the average value of the
Compton continuum on the left side of the ROI determined from the sum of
four channels to the left of L, and Ravg is the
average value of the Compton continuum on the right side of the ROI determined
from the sum of four channels to the right of R.Next,the
total background counts for the region of interest (BT)
were calculated by summing
Bi from channels R
to L. Finally, the net count rate in the ROI was calculated by subtracting
BT
from the observed gross counts and dividing by the count time.
Decision
Level (Lc) and Minimum Detectable Amount (MDA)
To determine whether or not activity has
been detected in a particular person, the parameter, Decision Level (LC)
was used. The LC
represents the 95th percentile of a null distribution that results
from the differences of repeated, pair-wise background measurements. An
individual result (net count rate) was assumed to be statistically greater
than background if it was greater than LC.
It is important to recognize that the use of this criterion (LC)
will result in a statistically inherent 5% false positive error rate per
pair-wise comparison (5% of all measurements will be determined to be positive
when there is actually no activity in the person). Decision levels were
calculated using the following equation based on the recommendations of
HPS N13.30 (Performance Criteria for Radiobioassay, May 1996):

where Cgross is the total gross counts
in the region of interest and t is the count time in seconds.
The value of MDA indicates the ability
of a facility to detect a radionuclide in a person. The MDA represents
the amount of a radionuclide that, if present, would be detected 95% of
the time under routine operation of a facility. The MDA is used to measure
the efficacy of a facility, but it should not be used to decide if a specific
radiobioassay has or has not detected activity within a person. MDA was
calculated using the following equation (HPS N13.30, Performance Criteria
for Radiobioassay, May 1996):

where K0.05 is the calibration factor,
taking into consideration counting efficiency and self absorption, that
represents the 5th percentile in distribution of individual
specific calibration factors; U is a conversion factor taking into
account photon yield, radioactive decay during the counting interval and
unit conversion; t is the count time in seconds; SB1
is the standard deviation, including Poisson and other random error components
in the count of a subject, determined by the routine measurement procedure,
where the subject contains no actual analyte activity above that of the
appropriate blank; and SB0 is the standard deviation,
including Poisson and other random error components, in the unadjusted
count of an appropriate blank. The term SB1 was determined
from the measurement of 272 and 271 individuals for radionuclides deposited
in lungs and whole body, respectively (a single whole body count was invalidated
due to instrument malfunction). The term SB0 was determined
from 20 measurements of a bottle manikin absorption (BOMAB) phantom filled
with de-ionized water.
It is important to note that the use
of K0.05
applies to lung counting where individual-specific
calibration factors vary with subject chest wall thickness. For example,
in this study individual-specific calibration factors for 238Pu
ranged from 4E-5 to 4E-7. For radionclides deposited in the whole body,
a single calibration factor per photon energy is applied to all individuals
regardless of anthropomorphic characteristics. Historically, the variability
associated with K in lung counting has been ignored, resulting in
unrealistically low estimates of MDA for radionuclides deposited in lungs.
Calibration factors for lung counting
were determined as a function of photon energy and muscle equivalent chest
wall thickness (MCWT) using the humanoid torso phantom developed
by Lawrence Livermore National Laboratory, 100% muscle equivalent chest
plates, and 238Pu and 241Am/152Eu lung
sets. Calibration factors for whole body counting were determined using
a BOMAB phantom filled with a muscle equivalent epoxy containing 152Eu
and 40K.
For plutonium isotopes, 244Cm
and 252Cf, the MCWT was determined from the subject's
height, weight and age using Equation 4 (Sumerlin, T. J. and S. P. Quant,
1982, Radiation Protection Dosimetry, 3, 203):
where Wa is the subject's weight (kg),
Ha
is the subject's height (m) and A is the subject's age. The total
thickness of tissue composing the chest wall (CWT) was determined for the
remaining radionuclides in lungs using Equation 5, which represents a composite
of the work performed by Fry (Fry, F. A., 1980, Health Physics,
39, 89), Garg (Garg, S. P., 1977, Health Physics 32, 54) and Dean
(Dean, P. N., 1973, Health Physics, 24, 439):
where Wb is the subject's weight (lb)
and Hb is the subject's height (inch). It is important
to note that this predictive equation is not normalized to muscle equivalent
thickness and will result in a conservative estimate of calibration factors
(Vickers, L. R., 1996, Health Physics, 70, 346). The calibration
factors selected for the MDA calculation for plutonium isotopes, 244Cm
and 252Cf (photon energies less than 20 keV) corresponded to
the 95th percentile of the MCWT (K is inversely
proportional to MCWT) determined from Equation 4. The calibration
factors selected in the calculation of MDA for the remaining radionuclides
in lungs (photon energies greater than 20 keV) corresponded to the 95th
percentile of CWT determined from Equation 5. This value of CWT was then
converted into muscle equivalent chestwall thicknesses for each photon
energy greater than 20 keV (MCWT>20 keV) using Equation
6 (Krammer, G. H., et. al. 1998, Health Physics, 74, 594):
where mmsc,i
is the linear attenuation coefficient at photon energy i for muscle
(cm-1), madp,iis
the linear attenuation coefficient at photon energy i for adipose
(cm-1) and AMF is the adipose mass fraction. The AMF
for
male and females were assumed to be 0.34 and 0.64, respectively (Vickers,
L. R., 1996, Health Physics, 70, 346). A single value of AMF,
weighted
by the proportion of males and females in the cohort, was used for the
calculation of MCWT>20 keV.
Results and Discussion
Cohort
Demographics
Demographic characteristics (Table
12) of the LDBC cohort are generally consistent with the survey published
by CERMC in 1998 entitled "Survey
of Factors Related to Radiation Exposure and Perception of Environmental
Risks in Carlsbad, Loving, Malaga, and Hobbs" and the 1990 Census
for citizens living in Carlsbad. With respect to gender, ethnicity, and
lifestyle, the current LDBC cohort is reasonably representative of the
citizens living in the vicinity of the WIPP. The largest deviations of
the LDBC demographics from those of the 1990 census were the over-sampling
of males and under-sampling of Hispanics by 12.7 and 19.4 %, respectively.
Interestingly, the 1998 CEMRC survey study (cited above) also under-sampled
Hispanics, to an even greater degree, relative to the 1990 Census. The
LDBC project is ongoing, and future recruitment efforts will focus on enrolling
additional females and Hispanics. However, the 1998 CEMRC survey and current
study results suggest that the recruitment of Hispanics, in proportion
to the 1990 Census, will be difficult. In addition, it is important to
note that if the presence of a radionuclide is dependent on a subclass
of interest (gender, ethnicity,etc.), valid population estimates can still
be made by correcting for the proportion of under- or over-sampling for
the particular subclass.
Background
Rates and Variability
The variance in background count rates
generally decreased with photon energy for each count type (e.g. lung or
whole body count) and source of background (e.g. human subjects or BOMAB
phantom, Fig. 39
and 40). This
is expected, since the counting efficiency of the instrument decreases
with photon energy. Background rates of a whole body count were generally
greater than that of a lung count. This also would be expected, since whole
body counts were performed with eight detectors compared with four for
lung counts, and the primary whole body counting detectors (COAX) are massive
relative to the lung counting detectors, resulting in greater background
due to increased intrinsic efficiency and photon/cosmic ray interaction
cross sections.
The difference in background rates
between the human subjects and the BOMAB phantom were greater for lung
counts than whole body counts, where the BOMAB phantom provided a reasonable
estimate of human subject background at energies less than 700 keV. The
energy response or shape of the background spectrum was well approximated
by the BOMAB phantom, especially for a lung count (Fig.
39). For both lung and whole body counts, repeated measures of the
BOMAB phantom underestimated the variance in human subject background (Fig
40).
The variance to mean ratio (Fig.
41) in human subject background for a lung and whole body count was
consistently greater than one. This has important implications to whole
body and nuclear counting, since it is often assumed that background is
characterized by a Poisson distribution. With a Poisson distribution, the
variance to mean ratio is one, and the best estimate of the mean response
is that observed (Knoll, G. F., 1989, Radiation Detection and Measurement,
John Wiley & Sons Inc., New York). If there are no other sources of
variability, then the mean, variance and standard deviation of a count
result (e.g. background) can be estimated from a single measurement. For
these data, if the Poisson assumption is applied and the human background
was estimated from the measurement of single subject or phantom (often
the case), the variability in background would have been underestimated
by as much as a factor of 10, but in all cases at least a factor of 2.
Underestimating the variability of background will result in an unrealistically
low estimate of measurement sensitivity.
Minimum
Detectable Amount
The range, mean and 95th percentile
of MCWT
(Equation
4) for plutonium isotopes, 244Cm and 252Cf were
1.7 to 4.9, 2.7 and 3.6 cm, respectively. The range, mean and 95th
percentile of CWT (Equation
5) were 1.0 to 6.8, 3.1 and 5.0 cm, respectively. The 95th
percentile of CWT when converted to MCWT>20 keV (Equation
6) ranged from 3.6 cm at 47 keV to 4.7 cm at 440 keV (Table
13).
MDAs calculated as described herein
for radionuclides in lungs ranged from 6.2E+00 Bq for 235U to
3.1E+04 Bq for 239Pu
(Table
13). MDAs for radionuclides in the whole body ranged from 1.4E+01 Bq
for 88Y to 1.9E+02 for 40K. Values of MDA reported
herein are a factor of 2 to 12 greater than those reported in the CEMRC
1997 Report. The reasons for the increases are threefold. First, values
of MDA reported in 1997 were based on repeated measures of a BOMAB phantom
filled with 140 g of K (reference man level). Although this is standard
practice in bioassay programs throughout the U.S., the data reported herein
demonstrated that such methodology underestimates the variability in human
background (Fig.
40
and 41). Based
on a priori assumptions, a CWT value of 2.4 was used for calculations
in the CEMRC 1997 Report to determine
K0.05for MDA calculation of radionuclides
in lungs. Finally, the previous calibration for radionuclides in lungs
was based on phantom overlays consisting of 50% muscle and 50% adipose
equivalent materials. A calibration based on 50% muscle/50% fat overlays
has less photon attenuation because of the adipose content than that used
for the current data (100% muscle overlays).
Values of MDA reported herein are more
realistic than the MDAs as typically calculated, because the variability
and magnitude of human subject background and population based calibration
factors (K0.05) have been considered. It is important
to note that most facilities, especially those for lung counting, do not
calculate MDA in this manner. Typically, an average or more ideal value
of CWT (corresponding to K) is selected for the MDA calculation.
However, such methodology can be quite misleading when applied to a population
of individuals whose body shapes and sizes are unknown a priori.
For example, the reported MDA applies only to those individuals with a
CWT
less than or equal to that assumed in the MDA calculation. If the assumed
value of CWT was the average of a population, then 50% of the individuals
in the population would have a CWT greater than the assumed value,
resulting in a non-detect lung count for a lung burden equal to the reported
MDA. In contrast, for this study only 5% of the population would be expected
to have a CWT thickness greater than that assumed for the MDA calculation
(in this case
MCWT). Thus, the MDA reported herein would result
in only 5% of the population having a non-detect lung count for a lung
burden equal to the reported MDA at the 95% confidence level.
Results
Greater Than LC
As previously discussed, the criterion,
LC,
was used to evaluate whether a result was in excess of background, and
the use of this criterion will result in statistically inherent 5% false
positive error rate per pair-wise comparison (5% of all measurements will
be determined to be positive when there is no activity present in the person).
For a particular radionuclide, to evaluate whether the frequency of results
greater than LC
was consistent with a false positive error rate, a binomial statistical
approach was applied. For example, if a radionuclide was not present in
the sample population, the frequency of results greater than LC
should fall within the distribution-free confidence interval for a proportion
equal to the error rate. The width of the confidence interval is dependent
on the sample size (in this case, 272 and 271 for lung and whole body counts,
respectively), the proportion of interest (5%) and level of confidence
(95%). A frequency of results greater than the distribution-free confidence
interval, for a radionuclide not present in the shielded room background
(defined as a 24-hour count of the BOMAB phantom), would suggest a low
frequency baseline of occurrence in the local population. The term ‘distribution-free’
refers to the idea that the derived statistical interval does not require
any distributional assumptions with regards to the data being evaluated
(Hahn, J. and W.Q. Meeker, 1991, Statistical Intervals A Guide for Practitioners,
John
Wiley & Sons, Inc. New York).
Using the ROI methodology, the percentage
of results greater than LC
were consistent with a 5% random false positive error rate, at the 95%
confidence level, for all radionuclides except 232Th via 212Pb,
235U
/ 226Ra, 60Co, 137Cs,
40K,
54Mn,
103Ru,
232Th
via
228Ac and 65Zn (Table
14). Five of these (232Th via 212Pb,
60Co,
40K,
54Mn
(228Ac interference), and 232Th via
228Ac)
are part of the shield-room background and positive detection would be
expected at low frequency. The percentage of results greater than
LC
for 103Ru and 65Zn were below the 95% confidence
interval for the random false positive error rate and may be statistical
anomalies (38 comparisons to the confidence interval were made). 40K
is a naturally occurring isotope of an essential biological element, so
detection in all individuals is expected. 137Cs and 235U
/ 226Ra are not components of the shielded room background and
were observed at frequency greater than the 95% confidence interval for
the false positive error rate (discussed in more detail later). In addition
to false positive rates, the ROI methodology appeared to be effective with
respect to false negative error rates (Table
15). For example, 24-hour measurements of the BOMAB phantom were used
to determine an equivalent human body burden for shield contamination from
the Th series and 60Co. Theoretically, if a subject had a body
burden equal to LC,
the detection of that radionuclide at LC
would be missed, when actually present (false negative), 50% of the time.
The false negative error rate would then increase as the body burden becomes
smaller relative to LC
until eventually no activity would be detected. In all cases, shield contamination
was equivalent to body burdens at levels below LC
and false negative error rates consistent with theory were observed.
In contrast, the peak search methodology
did not perform as well as the ROI methodology with respect to false positive
and false negative error rates and low activity radionuclide detection
(Table
14). While valuable to the practice of bioassay, this observation has
little impact on this study because the ROI methodology was used for the
detection and quantification of radionuclide activity.
40K results were positive
for all individuals, ranging from 2308 to 6513 Bq with an overall mean
(±SE) of 3293 (±784)
Bq. Such results are expected since K is an essential biological element
contained primarily in muscle, and a constant fraction of all naturally
occurring K is the radioactive isotope 40K. The mean 40K
value for males (±SE), was 4730
(± 46) Bq, which was significantly greater (P
< 0.0001) than that of females, which were 3507 ± 39 Bq (mean
± SE). This result was also expected since, in general, males tend
to have larger body sizes and greater muscle content than females.
In 27.8% of individual measurements,
the value for 137Cs was greater than LC
ranging from 6 to 25 Bq. This percentage was significantly higher than
the distribution-free confident interval for a 5% random false positive
error rate (2.2 to 7.4%), suggesting a low frequency baseline occurrence
of 137Cs in the local population. From these data, detectable
137Cs
is present in 22% to 33% (95% confidence level) of citizens living in the
Carlsbad area. These results are consistent with preliminary conclusions
that were reported in the CEMRC 1997 Report and not unexpected, since 137Cs
is an abundant, long-lived fission product. Because of its abundance, mobility,
and physiological properties, 137Cs is widely distributed throughout
the biosphere and has been detected previously in many organisms including
humans (Whicker, F.W. and V. Schultz, 1982,
Radioecology: Nuclear Energy
and the Environment 1, CRC Press, Inc., Florida).
Individual 137Cs results
were then compared to two sources of demographic data to determine whether
the presence of
137Cs was dependent on a particular demographic
or lifestyle parameter using a Chi-square test of independence (L. Ott,
1988, An Introduction to Statistical Methods and Data Analysis,
PWS-Kent Publishing Company, Boston, MA; Table 16). The presence of 137Cs
was independent of gender, ethnicity, age, radiation work history, consumption
of wild game, nuclear medical treatments and European travel. Occurrence
of detectable
137Cs was slightly associated (p = 0.032) with
smoking habit, where smokers had a higher prevalence of 137Cs
relative to non-smokers (21.3 to 11.2%, respectively). These data are interesting
because 137Cs is often assumed to be correlated to the consumption
of wild game, but this pattern did not appear in these data. The association
of 137Cs with smoking habit is also interesting, and could be
related to the presence of fallout 137Cs in tobacco. However,
the statistical significance of this dependence was weak, and further study
is warranted.
The percentage of results greater than
LC
for 235U/226Ra (9.9%) was significantly (although
slightly) higher than the distribution-free confidence interval for a 5%
random false positive error rate (2.2 to 7.4%). These data are not nearly
as suggestive, when compared to 137Cs, of low frequency baseline
occurrence of 235U/226Ra. It is important to note
that 235U and 226Ra are naturally occurring and these
two radionuclides cannot be distinguished via gamma spectroscopy. Therefore,
any positive signal could be the result of either or both radionuclides.
This effect was not apparent in the initial data reported in the CEMRC
1997 Report and requires a larger sample size to support or reject
the apparent pattern.
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