WSRC-TR-2002-00077

55-Gallon Drum Attenuation Corrections
for Waste Assay Measurements

V. R. Casella
Westinghouse Savannah River Company
Aiken, SC 29808

This document was prepared in conjunction with work accomplished under Contract No. DE-AC09-96SR18500 with the U.S. Department of Energy.

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Abstract

The present study shows how the percent attenuation for low-level waste (LLW), carbon-steel 55-gallon drums (44 and 46 mil) and for transuranic (TRU) DOT Type 7A 55-gallon drums (~61 mil) changes with gamma energy from 60 keV to 1400 keV. Attenuation for these drums is in the range of 5 to 15% at energies from 400 to 1400 keV and from 15 to 35 % at energies from 120 to 400 keV. At 60 keV, these drums attenuate 70-80% of the gamma rays. Correction factors were determined in order to correct for gamma attenuation of a TRU drum if a calibration is performed with a LLW drum. These correction factors increase the activities of the TRU drum by from 10% to 2% in the energy range of 165 to 1400 keV, with an increase of about 50% at 60 keV.

In cases where waste is assayed without a drum, the measured drum attenuations can be used to correct the calibrations that were done for drum assays. Correction factors to determine nuclide activities of samples without the drum attenuation were also determined in this study. These correction factors decrease the measured activities by 70% at 60 keV, by 30% to 9% at energies from 100 to 500 keV, and by about 7% for energies from 500 to 1400 keV.

Correction factors for TRU drums and for analyses without a drum were used to adjust the %yield for frequently measured gamma rays, so that the assay libraries could be modified to provide the drum attenuation corrections.

Keywords: 55-gallon Drum, Attenuation, Gamma PHA

1. Introduction

Transuranic (TRU) and low-level waste (LLW) at the Savannah River Site (SRS), packaged in 55-gallon drums, are assayed using Canberra Q2 Waste Assay Systems. Standard drums, containing materials of varying density and National Institute of Standards and Technolgy (NIST) traceable radioactivity standards, are used to calibrate these waste assay systems.1 For these calibrations, the attenuation of the drum is included in the calibration. LLW is assayed in carbon-steel drums that are about the same thickness (~44 mil) as the calibration drums (~46 mil) purchased from Canberra. However, TRU waste is assayed in DOT 7A drums that are considerably thicker (~61 mil) than the drums used for the calibration. Therefore the assay values for TRU waste will be biased low because there is more attenuation from the TRU drums than from the calibration drums. The present study measures the attenuation for gamma ray energies from 59 keV to 1408 keV for a LLW drum, a TRU drum, and the Canberra calibration drum to evaluate the attenuation corrections needed for routine assays. This correction is particularly important for measuring lower energy gamma rays from Am-241 (60 keV) and other TRU nuclides, such as Pu-239 (129 keV) and Pu-238 (99 keV and 152 keV), that are frequently assayed in SRS solid waste.

Also, there are LLW waste items, such as HEPA (High Efficiency Particulate Air) filters, that do not fit into a 55-gallon drum, but can be assayed with the Canberra Q2. Measured activities for waste not in a drum are biased high because the calibration is done with a drum. The results from this study can be used to adjust the assay results for waste items not contained in a drum, so that the drum calibration can be used.

2. Experimental

The Canberra Q2 Waste Assay System is a very low-level, quantitative and qualitative gamma pulse-height-analysis system and is shown in Figure 1. It contains three intrinsic germanium detectors with 7.5-liter cryostats. A low-level or TRU waste sample, usually in a 55-gallon drum, is placed on a turntable mounted on the door of the shielding. The turntable rotates at a nominal 10 RPM. An electronic load cell mounted on the turntable weighs the sample and displays the result. A 4-inch thick, low-background-steel shield surrounds the sample and detectors in all directions. The data acquisition system contains a PC-based Canberra AccuSpec Multichannel Analyzer (MCA) system, appropriate high voltage power supplies and amplifiers. The three AccuSpec boards are controlled by Canberra's NDA-2000 software running in a Windows-NT environment. For this study, NIST traceable standards, contained in a specially designed plastic holder that was representative of the drum geometry, were assayed with the 773-A Canberra Q2 Waste Assay System for 600 seconds.

Figure 1.  Canberra Q2 Waste Assay System
Figure 1. Canberra Q2 Waste Assay System

The standards, obtained from North American Scientific, Inc., are composed of an epoxy matrix cast in a 9.53 mm OD by 813 mm long aluminum tube. Subsequently, the plastic holder and standards were inserted into a 55-gallon drum and assayed again for 600 seconds.

Figure 2. Standards in Holder
Figure 2. Standards in Holder

 

Figure 3. Holder Placed in Drum
Figure 3. Holder Placed in Drum

 

Figure 4. Top View of Arrangement of Rod Standards in Positions 2, 3, 4, 5, 6 and 9 to Represent a Full Drum
Figure 4. Top View of Arrangement of Rod Standards in
Positions 2, 3, 4, 5, 6 and 9 to Represent a Full Drum

Figures 2 and 3 show how the plastic holder and standards were inserted into each drum, while Figure 4 shows the top view of the plastic holder and standards that were used in this study. The standards and holder were assayed inside a LLW drum (43 mil thickness), the Canberra standard drum (46 mil thickness) and a TRU drum (61 mil thickness) and the holder without a drum was assayed. The results of these assays were used to determine the attenuation of gamma rays over the energy range from 59 keV to 1408 keV for each drum.

3. Results

Peak counts for Am-241, Cs-137 and Eu-152 gamma rays (600-second count) are shown in Tables 1 through 3. In columns two and three, peak counts and uncertainties are listed for the standards and holder placed inside the drum, while columns four and five list the peak counts and uncertainties for just the standards inside the holder. From these data, the drum attenuations and uncertainties are calculated and listed in columns six and seven.

Table 1. Activities and Percent Attenuation for LLW Drum (44 mil)

Gamma

Energy
(keV)

Peak Counts

Drum+Holder+
Standards

Uncert.(2s)

Drum+Holder+
Standards

Peak

Counts
Holder+Stds


Uncert (2
s)
Holder+Stds

Drum

Att.
(%)

Drum

% Att.
Uncert. (2s)

59.5

9430

467

29800

570

68.4

3.6

121.8

122000

978

161000

1058

24.2

0.3

244.7

31400

578

35600

590

11.8

0.3

344.3

83600

664

93300

696

10.4

0.1

661.7

34300

381

37300

397

8.0

0.1

778.9

21500

350

22700

363

5.3

0.1

964.1

20300

322

21700

332

6.5

0.1

1112.1

16800

291

18200

300

7.7

0.2

1408.0

21500

297

23200

308

7.3

0.1

 

Table 2. Activities, Percent Attenuation and Correction Factors for Assay
without a Drum and Calibrated with the Canberra Drum (46 mil)

Gamma

Energy
(keV)

Peak Counts

Drum+Hldr+
Standards

Uncert.(2s)

Drum+Hldr+
Standards

Peak

Counts
Hldr+Stds

Uncert (2
s)
Hldr+Stds

Drum

Att.
(%)

Drum

% Att.
Uncert. (2s)

No Drum

% Att.
CF

Calc

CF
46 mil Fe

59.5

8980

504

30300

575

70.4

4.2

3.37

2.89

121.8

125000

984

164000

1069

23.8

0.2

1.31

1.30

244.7

31300

560

36100

415

13.3

0.3

1.15

1.12

344.3

84700

660

96000

693

11.8

0.1

1.13

1.09

661.7

34500

368

37800

385

8.7

0.1

1.10

1.07

778.9

21400

351

23500

367

8.9

0.2

1.10

1.06

964.1

20700

329

22000

340

5.9

0.1

1.06

1.06

1112.1

17100

294

18500

304

7.6

0.2

1.08

1.05

1408.0

22200

301

23500

311

5.5

0.1

1.06

1.05

Table 3. Activities, Percent Attenuation and Correction Factors for the
TRU Drum (61 mil) Calibrated with Canberra Drum (46 mil)

Gamma

Energy
(keV)

Peak Counts

Drum+Hldr+
Standards

Uncert.(2s)

Drum+Hldr+
Standards

Peak

Counts
Hldr+Stds


Uncert (2
s)

Hldr+Stds

Drum

Att.
(%)

Drum

% Att.
Uncert. (2s)

TRU Canberra % Att CF

Calc

CF
61 mil Fe

59.5

5880

440

30300

571

80.6

6.2

1.53

1.50

121.8

109000

947

159000

1059

31.4

0.3

1.11

1.11

244.7

29400

546

36500

572

19.5

0.5

1.08

1.04

344.3

79300

641

93700

684

15.4

0.2

1.04

1.04

661.7

33300

374

37400

397

11.0

0.2

1.03

1.03

778.9

20400

345

22900

364

10.9

0.3

1.02

1.02

964.1

19300

317

21900

339

11.9

0.3

1.07

1.02

1112.1

16600

289

18300

299

9.3

0.2

1.02

1.02

1408.0

21200

295

23200

308

8.6

0.2

1.03

1.02

The "No Drum" correction factor and the "TRU Drum/Canberra Drum" correction factor are given in column eight of Table 2 and Table 3, respectively. The "No Drum" correction factor referred to in Table 2 is calculated as follows:

CFND = (1 / (1 – AC))

where:

AC =the fractional attenuation for a given energy for the Canberra drum

while the "TRU Drum/Canberra Drum" correction factor in Table 3 is defined by the equation:

CFT/C = (1 / (1 – AT) / (1 / (1 – AC))

where:

AT= the fractional attenuation for a given energy for the TRU drum.

"No Drum" correction factors and the "TRU Drum/Canberra Drum" correction factors were calculated based on known mass attenuation coefficients2 for iron and are given in column 9 of Tables 2 and 3. As expected, the calculated correction factors for iron show good agreement with the measured correction factors for the steel drums.

4. Analysis of Results

Plots of the gamma ray attenuation versus gamma ray energy for the Canberra drum, the LLW drum and the TRU drum are given in Figure 5 and plots of the "No Drum" and the "TRU Drum/Canberra Drum" correction factors are given in Figure 6.

Figure 5. Gamma Ray Attenuation Versus Gamma Ray Energy for 55-Gallon Drums. 
  (The Green (Top), Blue and Red Curves (Bottom) are for the TRU Drum, Canberra Drum and LLW Drum, 
  Respectively.)
Figure 5. Gamma Ray Attenuation Versus Gamma Ray Energy for 55-Gallon Drums. (The Green (Top),
Blue and Red Curves (Bottom) are for the TRU Drum, Canberra Drum and LLW Drum, Respectively.)

 

Figure 6. No Drum (Green; Top) and TRU Drum/Canberra Drum (Blue; Bottom) Correction Factors Versus Gamma Ray Energy
Figure 6. "No Drum" (Green; Top) and "TRU Drum/Canberra Drum"
(Blue; Bottom) Correction Factors Versus Gamma Ray Energy

By using the known shape of the attenuation corrections for iron and the data shown in Figure 6, the "No Drum" and "TRU Drum/Canberra Drum" correction factors for the 60 keV to 1400keV energy range were determined and are given in Table 4 and shown in Figure 7.

The "No Drum" correction factors vary from 3.37 at 60 keV to 1.07 from 1000 to 1400 keV. For assays done without a drum, the measured activity would be divided by the "No Drum" correction factor for activities at a given energy.

"TRU Drum/Canberra Drum" correction factors are smaller than the "No Drum" correction factors because they represent a ratio of attenuation corrections. These correction factors vary from 1.53 to 1.03 and are less than 5% above 400 keV. "TRU Drum/Canberra Drum" corrections become especially important below 200 keV. The actual measured activities would be multiplied by "TRU Drum/Canberra Drum" correction factor for a given energy to obtain the correct measured concentrations for waste assay in a TRU drum.

Table 4. "No Drum" and "TRU Drum/Canberra Drum" Correction Factors using the
Predicted Curve Shape of Fe to Obtain Values from 60 to 1400 keV

Gamma

Energy (keV)

No Drum

Corr. Factor

TRU/Canberra

Corr. Factor

Gamma

Energy (keV)

No Drum

Corr. Factor

TRU/Canberra

Corr. Factor

60

3.37

1.53

200

1.16

1.06

70

2.51

1.38

300

1.12

1.05

80

1.86

1.24

400

1.11

1.04

90

1.63

1.19

500

1.10

1.04

100

1.44

1.14

600

1.09

1.04

110

1.37

1.13

700

1.09

1.03

120

1.33

1.12

800

1.08

1.03

130

1.29

1.11

900

1.08

1.03

140

1.26

1.10

1000

1.07

1.03

150

1.23

1.08

1100

1.07

1.03

160

1.21

1.07

1200

1.07

1.03

170

1.19

1.07

1250

1.07

1.03

180

1.18

1.07

1300

1.07

1.03

190

1.17

1.07

1400

1.07

1.03

 

Figure 7. No Drum (Green; Top) and TRU Drum/Canberra Drum
  (Blue; Bottom) Correction Factors Versus Gamma Ray Energy using the Predicted Curve Shape of Fe to Obtain Values over the Energy Range of 60keV to 1400 keV.
Figure 7. "No Drum" (Green; Top) and "TRU Drum/Canberra Drum" (Blue; Bottom)
Correction Factors Versus Gamma Ray Energy using the Predicted Curve Shape
of Fe to Obtain Values over the Energy Range of 60keV to 1400 keV

Anytime a TRU drum is analyzed the correction factors must be applied to preclude reporting erroneously low results. Rather than multiplying the TRU drum measured activities by the correction factors, the TRU library for the 773-A Canberra Q2 has been adjusted so that the correction factors are included in the %yield values for all TRU waste assays. The library was adjusted because the 773-A Canberra Q2 software does not have another way to include this correction.

As stated, if waste is analyzed without a drum, then the "No Drum" correction factors may be applied. This would be the case if the waste item were too large to fit into the drum. However, in this case, the correction factor lowers the measured activity. Since the actual result is conservatively high, the Cognizant Technical Function for waste assay may not deem it necessary to make this correction, especially if the assay yields very low nuclide activities.

The correction factors given in Table 4 would be applied for most nuclides determined at the 773-A Solid Waste Assay Facility.3 These correction factors are used to modify the analysis libraries that are used for different waste streams.

Table 5. "No Drum" and "TRU Drum/Canberra Drum" Gamma Ray Correction Factors and
Corrected % Yields for Analyses done at the 773-A Solid Waste Assay Facility


Nuclide

Gamma

Energy (keV)

No Drum

Corr. Factor

TRU/Canberra

Corr. Factor

Gamma

% Yield

No Drum

(%Yield X CF)

TRU/Canberra

(%Yield/CF)

Co-60

1173.24

1.07

1.03

9.9974E+01

1.07E+02

9.71E+01

Co-60

1332.50

1.07

1.03

9.9986E+01

1.07E+02

9.71E+01

Cs-137

661.65

1.10

1.03

8.51E+01

9.36E+01

8.26E+01

Eu-154

123.07

1.32

1.11

4.079E+01

5.38E+01

3.68E+01

Eu-154

723.30

1.09

1.03

2.022E+01

2.20E+01

1.96E+01

Eu-154

873.19

1.08

1.03

1.227E+01

1.33E+01

1.19E+01

Eu-154

996.26

1.07

1.03

1.059E+01

1.13E+01

1.03E+01

Eu-154

1004.73

1.07

1.03

1.801E+01

1.93E+01

1.75E+01

Eu-154

1274.44

1.07

1.03

3.519E+01

3.77E+01

3.42E+01

U-235

143.76

1.25

1.09

1.096E+01

1.37E+01

1.01E+01

U-235

185.72

1.18

1.07

5.72E+01

6.75E+01

5.35E+01

Np-237

86.48

1.12

1.05

1.24E+01

1.39E+01

1.18E+01

Np-237

103.97

1.42

1.14

8.7E-01

1.24E+00

7.60E-01

Np-237

300.34

1.12

1.05

6.62E+00

7.41E+00

6.30E+00

Np-237

312.17

1.12

1.05

3.86E+01

4.32E+01

3.68E+01

Np-237

340.81

1.12

1.05

4.47E+00

5.01E+00

4.26E+00

Np-237

375.45

1.11

1.04

6.79E-01

7.54E-01

6.53E-01

Np-237

398.62

1.11

1.04

1.39E+00

1.54E+00

1.34E+00

Np-237

415.76

1.11

1.04

1.745E+00

1.94E+00

1.68E+00

U-237

59.536

3.37

1.53

3.45E+01

1.16E+02

2.25E+01

U-237

97.066

1.50

1.16

1.60E+01

2.40E+01

1.38E+01

U-237

101.059

1.43

1.14

2.60E+01

3.72E+01

2.28E+01

U-237

164.610

1.20

1.07

1.852E+00

2.22E+00

1.73E+00

U-237

208.000

1.16

1.06

2.114E+01

2.45E+01

1.99E+01

Pu-238

99.853

1.44

1.14

7.35E-03

1.06E-02

6.45E-03

Pu-238

152.72

1.23

1.08

9.37E-04

1.15E-03

8.68E-04

Pu-239

77.59

2.02

1.28

4.1E-04

8.3E-04

3.2E-04

Pu-239

98.78

1.46

1.14

1.22E-03

1.78E-03

1.07E-03

Pu-239

103.06

1.42

1.14

2.3E-04

3.3E-04

2.0E-04

Pu-239

115.38

1.40

1.14

4.62E-04

6.47E-04

4.05E-04

Pu-239

116.26

1.40

1.14

5.97E-04

8.36E-04

5.24E-04

Pu-239

129.30

1.29

1.11

6.31E-03

8.14E-03

5.68E-03

Pu-239

144.2

1.25

1.09

2.83E-04

3.54E-04

2.60E-04

Pu-239

146.09

1.25

1.09

1.19E-04

1.49E-04

1.09E-04

Pu-239

161.45

1.21

1.07

1.23E-04

1.49E-04

1.15E-04

Pu-239

171.39

1.19

1.07

1.1E-04

1.3E-04

1.0E-04

Pu-239

195.68

1.17

1.07

1.07E-04

1.25E-04

1.00E-04

Pu-239

203.55

1.16

1.06

5.69E-04

6.60E-04

5.37E-04

Pu-239

332.85

1.12

1.05

4.94E-04

5.53E-04

4.70E-04

Pu-239

336.11

1.12

1.05

1.12E-04

1.25E-04

1.07E-04

Pu-239

345.01

1.12

1.05

5.56E-04

6.23E-04

5.30E-04

Pu-239

375.05

1.11

1.04

1.554E-03

1.73E-03

1.49E-03

Pu-239

380.19

1.11

1.04

3.05E-04

3.39E-04

2.93E-04

Pu-239

382.75

1.11

1.04

2.59E-04

2.87E-04

2.49E-04

Pu-239

392.91

1.11

1.04

5.53E-04

6.14E-04

5.32E-04

Pu-239

413.71

1.11

1.04

1.466E-03

1.63E-03

1.41E-03

Pu-239

422.60

1.11

1.04

1.22E-04

1.35E-04

1.17E-04

Pu-239

451.48

1.10

1.04

1.894E-04

2.08E-04

1.82E-04

Pu-240

104.23

1.41

1.14

7.08E-03

9.98E-03

6.21E-03

Pu-240

160.31

1.21

1.07

4.02E-04

4.86E-04

3.76E-04

Am-241

59.5

3.37

1.53

3.59E+01

1.21E+02

2.35E+01

Am-241

98.97

1.46

1.14

2.03E-02

2.96E-02

1.78E-02

Am-241

102.98

1.42

1.14

1.95E-02

2.77E-02

1.71E-02

Am-241

125.30

1.31

1.11

4.08E-03

5.34E-03

3.68E-03

Am-241

208.01

1.16

1.06

7.91E-04

9.18E-04

7.46E-04

Am-241

335.37

1.12

1.05

4.96E-04

5.56E-04

4.72E-04

Pu-241

103.68

1.41

1.14

1.017E-04

1.43E-04

8.92E-05

Pu-241

148.57

1.23

1.08

1.855E-04

2.28E-04

1.72E-04

Pu-242

158.80

1.21

1.07

4.536E-04

5.49E-04

4.24E-04

Am-243

74.66

2.21

1.32

6.82E+01

1.51E+02

5.17E+01

Am-243

99.52

1.44

1.14

1.50E+01

2.16E+01

1.32E+01

Am-243

103.73

1.42

1.14

2.39E+01

3.39E+01

2.10E+01

Am-243

106.12

1.40

1.13

2.72E+01

3.81E+01

2.41E+01

Am-243

209.75

1.16

1.06

3.42E+00

3.97E+00

3.23E+00

Am-243

228.18

1.15

1.06

1.076E+01

1.24E+01

1.02E+01

Am-243

277.60

1.13

1.05

1.438E+01

1.63E+01

1.37E+01

Cm-243

99.52

1.44

1.14

1.44E+01

2.07E+01

1.26E+01

Cm-243

103.73

1.42

1.14

2.30E+01

3.27E+01

2.02E+01

Cm-243

209.75

1.16

1.06

3.29E+00

3.82E+00

3.10E+00

Cm-243

228.18

1.15

1.06

1.0569E+01

1.22E+01

9.97E+00

Cm-243

277.60

1.13

1.05

1.3959E+01

1.58E+01

1.33E+01


5. Conclusions

The present study shows how the attenuation for low-level waste (LLW), carbon-steel 55-gallon drums (44 and 46 mil) and for transuranic (TRU) DOT Type 7A 55-gallon drums (~61 mil) changes with gamma energy from 60 keV to 1400 keV. Attenuation for these drums is quite significant (5-15%) at energies from 400 to 1400 keV, and becomes very significant at energies from 120 to 400 keV (15-35%). At 60 keV, these drums attenuate 70-80% of the gamma rays. Correction factors were determined in order to correct for gamma attenuation of a TRU drum if a calibration is performed with a LLW drum. The correction factors require an increase in the activities of the TRU drum of from 10% to 2% in the energy range of 165 to 1400 keV, while an increase of about 50% is required at 60 keV.

In cases where waste is assayed without a drum, the measured drum attenuations can be used to correct the calibrations that were done for drum assays. Correction factors to determine nuclide activities of samples without the drum attenuation were also determined in this study. These correction factors decrease the measured activities by 70% at 60 keV, by 30% to 9% at energies from 100 to 500 keV, and by about 7% for energies from 500 to 1400 keV.

Correction factors for TRU drums and for analyses without a drum were calculated for gamma rays of most nuclides determined at the 773-A Solid Waste Assay Facility. These correction factors were used to adjust the branching intensities for the gamma rays, so that the assay libraries could be modified to make the drum attenuation corrections.

6. References

  1. WSRC L7.13 Manual, Procedure 006, "Calibration of the 773-A Q2 Waste Assay System," May 1999.
  2. B. S. Shleien, L. A. Slaback and B. K. Birky, Handbook of Health Physics and Radiological Health, Third Edition, ISBN 0-683-18334-6, 1998.
  3. P. E. Filpus-Luyckx, WSRC-TR-96-0344, January, 1997.