Standard Test Method for Atom Percent Fission in Uranium and Plutonium Fuel (Neodymium-148 Method)

SCOPE
1.1 This test method covers the determination of stable fission product  148Nd in irradiated uranium (U) fuel (with initial plutonium (Pu) content from 0 to 50 %) as a measure of fuel burnup (1-3).  
1.2 It is possible to obtain additional information about the uranium and plutonium concentrations and isotopic abundances on the same sample taken for burnup analysis. If this additional information is desired, it can be obtained by precisely measuring the spike and sample volumes and following the instructions in Test Method E267.
1.3 This standard does not purport to address all of the safety concerns, if any, associated with its use. It is the responsibility of the user of this standard to establish appropriate safety and health practices and determine the applicability of regulatory limitations prior to use.

General Information

Status
Historical
Publication Date
31-Dec-2004
Technical Committee
Drafting Committee
Current Stage
Ref Project

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ASTM E321-96(2005) - Standard Test Method for Atom Percent Fission in Uranium and Plutonium Fuel (Neodymium-148 Method)
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NOTICE: This standard has either been superseded and replaced by a new version or withdrawn.
Contact ASTM International (www.astm.org) for the latest information
Designation:E321–96(Reapproved2005)
Standard Test Method for
Atom Percent Fission in Uranium and Plutonium Fuel
(Neodymium-148 Method)
This standard is issued under the fixed designation E321; the number immediately following the designation indicates the year of
original adoption or, in the case of revision, the year of last revision. A number in parentheses indicates the year of last reapproval. A
superscript epsilon (´) indicates an editorial change since the last revision or reapproval.
1. Scope E267 Test Method for Uranium and Plutonium Concentra-
tions and Isotopic Abundances
1.1 This test method covers the determination of stable
fission product Nd in irradiated uranium (U) fuel (with
3. Summary of Test Method
initial plutonium (Pu) content from 0 to 50 %) as a measure of
2 3.1 Fission product neodymium (Nd) is chemically sepa-
fuel burnup (1-3).
rated from irradiated fuel and determined by isotopic dilution
1.2 It is possible to obtain additional information about the
mass spectrometry. Enriched Nd is selected as the Nd
uranium and plutonium concentrations and isotopic abun-
isotope diluent, and the mass-142 position is used to monitor
dances on the same sample taken for burnup analysis. If this
for natural Nd contamination. The two rare earths immediately
additional information is desired, it can be obtained by pre-
adjacent to Nd do not interfere. Interference from other rare
cisely measuring the spike and sample volumes and following
142 148
earths,suchasnaturalorfissionproduct Ceornatural Sm
the instructions in Test Method E267.
and Sm is avoided by removing them in the chemical
1.3 This standard does not purport to address all of the
purification (4 and 5).
safety concerns, if any, associated with its use. It is the
150 233 242
3.2 After addition of a blended Nd, U, and Pu spike
responsibility of the user of this standard to establish appro-
to the sample, the Nd, U, and Pu fractions are separated from
priate safety and health practices and determine the applica-
eachotherbyionexchange.Eachfractionisfurtherpurifiedfor
bility of regulatory limitations prior to use.
mass analysis. Two alternative separation procedures are pro-
2. Referenced Documents vided.
3.3 The gross alpha, beta, and gamma decontamination
2.1 ASTM Standards:
factors are in excess of 10 and are normally limited to that
D1193 Specification for Reagent Water
242 147 241
value by traces of Cm, Pm, and Am, respectively (and
E180 Practice for Determining the Precision of ASTM
sometimes Ru),noneofwhichinterferesintheanalysis.The
Methods for Analysis and Testing of Industrial and Spe-
70 ng Nd minimum sample size recommended in the
cialty Chemicals
procedure is large enough to exceed by 100-fold a typical
E244 TestMethodforAtomPercentFissioninUraniumand
natural Nd blank of 0.7 6 0.7 ng Nd (for which a correction
Plutonium Fuel (Mass Spectrometric Method) (Discontin-
4 is made) without exceeding radiation dose rates of 20 µ Sv/h
ued 2001)
(20 mR/h) at 1 m. Since a constant amount of fission products
is taken for each analysis, the radiation dose from each sample
is similar for all burnup values and depends principally upon
This test method is under the jurisdiction ofASTM Committee C26 on Nuclear
cooling time. Gamma dose rates vary from 200 µ Sv/h (20
Fuel Cycle and is the direct responsibility of Subcommittee C26.05 on Methods of
mR/h) at 1 m for 60-day cooled fuel to 20 µ Sv/h (2 mR/h) at
Test.
1 m for 1-year cooled fuel. Beta dose rates are an order of
Current edition approved Jan. 1, 2005. Published March 2005. Originally
approved in 1967 . Last previous edition approved in 1996 as E321 – 96. DOI:
magnitude greater, but can be shielded out with a ⁄2-in.
10.1520/E0321-96R05.
(12.7-mm) thick plastic sheet. By use of such simple local
The boldface numbers in parentheses refer to the list of references appended to
shielding, dilute solutions of irradiated nuclear fuel dissolver
this test method.
solutions can be analyzed for burnup without an elaborate
For referenced ASTM standards, visit the ASTM website, www.astm.org, or
contact ASTM Customer Service at service@astm.org. For Annual Book of ASTM
shielded analytical facility. The decontaminated Nd fraction is
Standards volume information, refer to the standard’s Document Summary page on
mounted on a rhenium (Re) filament for mass analysis.
the ASTM website.
Samples from 20 ng to 20 µg run well in the mass spectrometer
Withdrawn. The last approved version of this historical standard is referenced
+ +
on www.astm.org. with both NdO and Nd ion beams present. The metal ion is
Copyright © ASTM International, 100 Barr Harbor Drive, PO Box C700, West Conshohocken, PA 19428-2959, United States.
E321–96 (2005)
enhanced by deposition of carbonaceous material on the used, provided it is first ascertained that the reagent is of
filament as oxygen getter. (Double and triple filament designs sufficiently high purity to permit its use without lessening the
do not require an oxygen getter.) accuracy of the determination.
5.2 Purity of Water— Unless otherwise indicated, refer-
4. Significance and Use
ences to water shall be understood to mean reagent water as
4.1 The burnup of an irradiated nuclear fuel can be deter-
defined in Specification D1193.
148 239 238
mined from the amount of a fission product formed during 5.3 Blended Nd, Pu, and U Calibration Standard—
148 148
irradiation. Among the fission products, Nd has the follow-
Prepare a solution containing about 0.0400 mg Nd/litre, 50
238 239
ingpropertiestorecommenditasanidealburnupindicator:(1) mg U/litre, and 2.5 mg Pu/litre, in nitric acid (HNO ,
It is not volatile, does not migrate in solid fuels below their
1 + 1) with 0.01 M hydrofluoric acid (HF) as follows. With a
recrystallization temperature, and has no volatile precursors. new calibrated, clean, Kirk-type micropipet, add 0.500 mL of
(2) It is nonradioactive and requires no decay corrections. ( 3)
239Pu known solution (see 5.11) to a calibrated 1-litre volu-
It has a low destruction cross section and formation from metric flask. Rinse the micropipet into the flask three times
adjacent mass chains can be corrected for. (4) It has good
with HNO (1 + 1). In a similar manner, add 0.500 mLof U
emission characteristics for mass analysis. (5) Its fission yield
known solution (see 5.12) and 1.000 mL of Nd known
235 239
is nearly the same for U and Pu and is essentially solution (see 5.9).Add 10 drops of concentrated HF and dilute
independentofneutronenergy(6).(6)Ithasashieldedisotope,
exactly to the 1-litre mark with HNO (1 + 1) and mix
142Nd, which can be used for correcting natural Nd contami- thoroughly.
nation. (7) It is not a normal constituent of unirradiated fuel.
5.3.1 From K (see 5.9), calculate the atoms of Nd/mL
4.2 The analysis of Nd in irradiated fuel does not depend of calibration standard, C , as follows:
on the availability of preirradiation sample data or irradiation
mL Nd known solution
history. Atom percent fission is directly proportional to the C 5 3 K (1)
148 148
1000 mL calibration standard
Nd-to-fuel ratio in irradiated fuel. However, the production
148 147 5.3.2 From K (see 5.12), calculate the atoms of U/mL
of Nd from Nd by neutron capture will introduce a
of calibration standard, C , as follows:
systematic error whose contribution must be corrected for. In
power reactor fuels, this correction is relatively small. In test
mL U known solution
C 5 3 K (2)
23 8 238
reactor irradiations where fluxes can be very high, this correc-
1000 mL calibration standard
tion can be substantial (see Table 1).
148 147 A
TABLE 1 K Factors to Correct Nd for Nd Thermal Neutron Capture
Total Neutron Exposure, fI (neutrons/cm )
Total Neutron Flux,
20 20 21 21 21
f (neutrons/cm /s)
1 3 10 3 3 10 1 3 10 2 3 10 3 3 10
3 3 10 0.9985 0.9985 0.9985 0.9985 0.9985
1 3 10 0.9956 0.9952 0.9950 0.9950 0.9950
3 3 10 0.9906 0.9870 0.9856 0.9853 0.9852
1 3 10 0.9858 0.9716 0.9598 0.9569 0.9559
3 3 10 0.9835 0.9592 0.9187 0.9008 0.8941
1 3 10 0.9826 0.9526 0.8816 0.8284 0.8006
A 147
Assuming continuous reactor operation and a 274 6 91 barn Nd effective neutron absorption cross section for a thermal neutron power reactor. This cross section
was obtained by adjusting the 440 6 150 barn Nd cross section (7) measured at 20°C to a Maxwellian spectrum at a neutron temperature of 300°C.
4.3 The test method can be applied directly to U fuel 5.3.3 From K (see 5.11), calculate the atoms of Pu/mL
containing less than 0.5 % initial Pu with 1 to 100 GW
of calibration standard, C , as follows:
23 9
days/metric ton burnup. For fuel containing 5 to 50 % initial
mL Pu known solution
Pu, increase the Pu content by a factor of 10 to 100,
C 5 3 K (3)
239 239
1000 mL calibration standard
respectively in both reagents 5.3 and 5.4.
5.3.4 Flame seal 3 to 5-mL portions in glass ampoules to
5. Reagents and Materials
preventevaporationafterpreparationuntiltimeofuse.Foruse,
5.1 Purity of Reagents—Reagent grade chemicals shall be
break off the tip of an ampoule, pipet promptly the amount
used in all tests. Unless otherwise indicated, it is intended that
required, and discard any unused solution. If more convenient,
all reagents shall conform to the specifications of the Commit-
calibration solution can be flame-sealed in pre-measured
tee onAnalytical Reagents of theAmerican Chemical Society,
1000-µL portions for quantitative transfer when needed.
where such specifications are available. Other grades may be
150 233 242
5.4 Blended Nd, U, and Pu Spike Solution—
Prepare a solution containing about 0.4 mg Nd/litre, 50 mg
5 233U/litre, and 2.5 mg Pu/litre in HNO (1 + 1) with 0.01 M
Reagent Chemicals, American Chemical Society Specifications, American
Chemical Society, Washington, DC. For suggestions on the testing of reagents not HF. These isotopes are obtained in greater than 95, 99, and
listed by the American Chemical Society, see Analar Standards for Laboratory
99 % isotopic purity, respectively, from the Isotopes Sales
Chemicals, BDH Ltd., Poole, Dorset, U.K., and the United States Pharmacopeia
DepartmentofOakRidgeNationalLaboratory.Standardizethe
and National Formulary, U.S. Pharmacopeial Convention, Inc. (USPC), Rockville,
MD. spike solution as follows:
E321–96 (2005)
5.4.1 In a 5-mL beaker, place about 0.1 mL of ferrous 5.10 Perchloric Acid—70 % HCIO .
solution, exactly 500 µL of calibration standard (see 5.3) and 5.11 Pu Known Solution—Add 10 mL of HCl (1 + 1) to
exactly 500 µL of spike solution (see 5.4). In a second beaker, a clean calibrated 100-mL flask. Cool the flask in an ice water
place about 0.1 mLof ferrous solution and 1 mLof calibration bath. Allow time for the acid to reach approximately 0°C and
standard without any spike. In a third beaker, place about 0.1 place the flask in a glove box. Displace the air in the flask with
mL of ferrous solution and 1 mL of spike solution without inert gas (Ar, He, or N ). Within the glove box, open the U.S.
standard. Mix well and allow to stand for 5 min to reduce Pu National Institute of Standards and Technology Plutonium
(VI) to Pu (III) or Pu (IV). Metal Standard Sample 949, containing about 0.5 g of Pu
(actual weight individually certified), and add the metal to the
5.4.2 Follow the procedure described in 7.2.4-7.5.8 or
7.6.2-7.7.11. Measure the Pu, U, and Nd isotopes by surface cooled HCl. After dissolution of the metal is complete, add 1
dropofconcentratedHFand40mLofHNO (1 + 1)andswirl.
ionization mass spectrometry following the procedure de-
scribed in 7.8.1-7.8.3.2 . On the Pu fractions, record the atom Place the flask in a stainless-steel beaker for protection and
242 239
invert a 50-mL beaker over the top and let it stand for at least
ratios of Pu to Pu in the calibration standard, C ; in the
2/9
spike solution, S ; and in the standard-plus-spike mixture, 8 days to allow any gaseous oxidation products to escape.
2/9
233 238
Dilute to the mark with HNO (1 + 1) and mix thoroughly. By
M .OntheUfractionsrecordthecorresponding U-to- U
2/9
using the individual weight of Pu in grams, the purity, and the
ratios, C , S , and M . On the Nd fractions, record the
3/8 3/8 3/8
molecular weight of the Pu given on the NIST certificate, with
corresponding Nd-to- Nd ratios, C , S , and M .
50/48 50/48 50/48
the atom fraction, A , determined as in 8.8, calculate the atoms
Correct all average measured ratios for mass discrimination
239 239
of Pu/mL of Pu known solution, K , as follows:
bias (see 6.2).
5.4.3 Calculate the number of atoms of Nd/mL of Spike,
K 5 [~mg Pu/100 mL solution!3 % purity/100!
A , as follows:
3~6.025 3 10 atoms/Pu molecular weight!3 A # (8)
A 5 C @~M 2 C !/~1 2 M /S !# (4)
50 148 50/48 50/48 50/48 50/48 5.12 U Known Solution—Heat U O from the National
3 8
Institute of Standards and Technology Natural Uranium Oxide
5.4.4 Calculate the number of atoms of U/mL of spike,
Standard Sample 950 in an open crucible at 900°C for1hand
A , as follows:
cool in a dessicator in accordance with the certificate accom-
A 5 C M 2 C / 1 2 M /S (5)
@~ ! ~ !#
33 238 3/8 3/8 3/8 3/8
panying the standard sample. Weigh about 12.0 g of U O
3 8
5.4.5 Calculatethenumberofatomsof Pu/mLspike, A ,
accurately to 0.1 mg and place it in a calibrated 100-mL
as follows:
volumetric flask. Dissolve the oxide in HNO (1 + 1). Dilute to
the 100-mL mark with HNO (1 + 1) and mix thoroughly. By
A 5 C @~M 2 C !/~1 2 M /S !# (6) 3
42 239 2/9 2/9 2/9 2/9
using the measured weight of U O in grams, the purity given
3 8
5.4.6 Store in the same manner as the calibration standard
on the NIST certificate, and the atom fraction U, A ,
(see 5.3), that is, flame seal 3 to 5-mL portions in glass
238 238
determined as in 8.5, calculate the atoms U/mL of U
ampoules. For use, break off the tip of an ampoule, pipet
solution, K , as follows:
promptly the amount required, and discard any unused solu-
K 5 [~ g U O /100 mL solution! 3 ~% purity/100
238 3 8
tion. If more convenient, spike solution can be flame sealed in
3 848.0 mg U/1 g U O ! 3 ~6.025
3 8
a premeasured 1000-µL portions for quantitative transfer to
3 10 atoms/238.03 molecular weight 3 A (9)
! #
individual samples.
5.13 Reagents and Materials for Procedure A:
5.5 Ferrous Solution (0.001 M)—Add 40 mg of reagent
5.13.1 Dowex AGMP-1 Resin—Convert Dowex AGMP-1
grade ferrous ammonium sulfate (Fe(NH ) (SO ) ·6H O) and
4 2 4 2 2
(200 to 400 mesh) chloride form resin to nitrate form by
1 drop of concentrated H SO to 5 mL of redistilled water.
2 4
washing 200 mL of resin in a suitable column (for example, a
Dilute to 100 mL w
...

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