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Title: Molecular Forensic Science of Nuclear Materials
Author(s): Marianne P. Wilkerson
Intended for: LORD-DR Program Review
13 January 2011
Los Alamos, NM USA
Los Alamos
NATIONAL lABORATO'RY
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Form 836 (7/06)
Molecular Forensic Science
of Nuclear Materials
20100048DR
Marianne P. Wilkerson
13 January 2011
Laboratory Directed Research and Development - Directed Research
Los Alamos National Laboratory
NI~l'r(!;5~,6l,1l- "-AlfO'!tA.ITClItV UNCLASSIFIED Slide 1
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Charge and Review Criteria
for 12-15 month projects
Assessment: Strengths and weakness of the project with respect to the
standard OMS criteria for Federally supported R&D:
Quality: Are the science and technology results of high quality compared to
national and international peers?
Performance (Project Execution): Is the project making good progress against
its milestones? Is it well-conceived and executed?
Leadership: Are the results of the project defining R&D directions for the
broader community?
Relevance: Is the project continuing to support the strategic directions of the
Laboratory?
Advice: Given the finite time remaining to the project, how might the project
maximize its impact (both to its field and to the Los Alamos mission) at the end
of 3 years? How should the project approach its transition to non-LORD
funding?
UNCLASSIFIED
~1.(\n6'",,1~!\. i!.ArO'~Alr~It'? _________________________________ Slide 2
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hat is the problem that Molecular Forensic
Science of Nuclear Materials is addressing?
. Increasingly varied and asymmetric threats are
expanding the scope of nuclear forensics
· Signatures are varied and can evolve, while any
given sample may include multiple signatures
LARGE
· The scale of sample may be or
tiny
· Accurate, effective technical analysis depends on
- identifying new signatures
- understanding measurement limitations
- evaluating complementary nature between
traditional and new measurements
- assessing the value of the information
· Production, conversion and aging of actinide
terials are chemical in nature, but chBmical
Los Alamos signatures are not exploited
r:J'Alr,'ONAII!. l.4:8-0~AIT"RY U N C LAS S I FIE D Slide 3
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ium materia science is rich in information!
denitration
• Uranium pitchblend ores
II t ~
must be separated from as precipitation
many as 40 elements I I Ammonium Uranium
Yellow Cake Uranyl Nitrahte diuranate trioxide
65-85% U30S ~ U02(N03 (NH4hU207 U03
· > 10 phases between U0 and
2 I
calcination
f
U0 , in addition to hydrated forms & reduction
3
of U0 hydro
3 enrichment fluorination
fluorination
» » Green Salt Brown Oxide
0lIl( 0lIl( UF ~ U0
A 2
· Deceptively simple formula
and cubic structure of U0 masks ~
reduction
2
incredibly complex speciation
Uranium metal
· Weathering initiates changes in speciation
"The GomRlexily- of the system is awesome.
U~O
11
Edelstein, N. M. et ai, Summary and Comparison of the Actinide and Transactinide Elements. In The Chemistry of the
Actinide and Transactinide Elements, 2006; Chapter 15, pp. 1753-1835. -
LoSAI1amos
..
~'AnOI5lIAl-t tABORAl-TOR,Y UNCLASSIFIED Slide 4
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owe ean by chemical speciation?
Physical (or Phase) Speciation
· Refers indirectly to the phase
association: dissolved, or associated
with various mineral or colloidal phases
U(III) U(IIV) U(V) U(VI)
Chemical Speciation
· Refers to the chemical form and generally
includes a knowledge of phase
· Depending on the type of information,
various levels exist
U0 {OH)+
2
· Identity of the element o 0 2+
<1 11
· Physical state H H Il oH
0 ",,.,,.
2 '... ... ......, . .. ,~ 2
idation state 0
• \ J x ~H'o ~ll, OH2
2
· tv-olacular formula II II
H 0 H OH
2 2
· IVlolecular structure o 0
" J
Los Alamos
1i1iAT"16NAL l-A!HiSIfA,,rOIfY UNCLASSIFIED Slide 5
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nium oxidation is more complex than
• •
tty suggested .
Plutonium metal coupon (1 g)
J:
0:::
o~
o
H 0
N 2
J:
0:::
o~
o
U)
Pu0
2
Traditional views of Pu corrosion:
PU 0
2 3
Pu + 2H20 ~ Pu02+x + 2H2 Pu metal
versus a new understanding of surface
phase relationships
Clark, D. L.; Hecker; S. 5.; Jarvinen, G. D.; Neu, M. P. Plutonium. In The Chemistry of the
Actinide and Transactinide Elements, 3rd ed.; Morss, L. R., Edelstein, N. M., Fuger, J., Katz, J. J.,
Eds.; Springer: Dordrecht, The Netherlands, 2006; Chapter 15, pp. 1753-1835.
UNCLASSIFIED
NIA-,rr65'I'iIiA>~ r..1>i8'O'R',A'T~FfY Slide 6
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· n't chemical speciation already applied to forensic
alvses? Where is the innovation here?
Morphology Elemental/isotopic Structural (lattice)
. X-ray diffraction
· Scanning Electron
analysis
· SEM-EDX
Microscopy
·XANES
·XRF
· EXAFS
· TIMS/SIMS
UNCLASSIFIED
Slide 7
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ar t:nvironmental Science
~
Molecular Forensic Science
RFETS 1995
Molecular level information
#
revolutionized environmental science
because speciation was a better
determinant of future risk
Clark, D. L.; Janecky, D. R.; Lane, L.
J. "Science-based cleanup of Rocky Flats"
Physics Today, 2006,59(9),34-40.
· Developed a more defined scope with
clear endpoint
Molecular Molecular
Forensic Environmental
Establish: Science Actinide- Science Predict:
age 0( I containing • dose
history Back particle Forward risk
source
In time In time
" We propose that chemical speciation
can provide molecular level information
source, production mode, age,
b9!~lr!m~ intended use, and his~~~L
ASS I FIE
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the tools used to determine chemical
-ation in Molecular Environmental Science?
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UNCLAS SIFIED
NJAnO'N'~t lABOIM,OR'Y Slide 9
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