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Radiochemistry Fuel Cycle Summer SchoolLecture 1: Introduction
Class organizationO utcomesGrading
H istoryChart of the nuclides
D escription and use of chartD ata
Radiochemistry introductionA tomic propertiesNuclear nomenclatureX-raysTypes of decaysforces
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Introduction
Coursed developed with support fromD epartment of Energy-NuclearEnergyExtension of education and researchefforts in the UNLV RadiochemistryprogramCourse designed to increase potentialpool of researchers for the nuclearfuel cycle
Nuclear fuelSeparationsWaste formsSafeguardsNuclear reactors
Course will emphasize the role of radiochemistry in the nuclear fuelcycle
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Course overviewIntensive course in radiochemistry with a focus on the nuclear fuelcycleRadiochemistry includes physics of radioactive decay andchemistry of radioisotopes
Intellectual intersection of the periodic table and chart of thenuclides
Course topics
Chart of the nuclidesD etails on alpha decay, beta decay, gamma decay, and fissionMethods and data from the investigation of nuclearpropertiesFundamental chemical properties in radiation andradiochemistry
Radioisotope production andRadiochemistry in research and technology
Textbooks and published literature are used a reading material
1st course: Input from students valued
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Course overviewCourse has lecture and laboratory component
Lectures daily0900-1200TBE Room B178
Laboratory variedSet laboratories to provided background
* Radiation safety* A lpha spectroscopy* Gamma spectroscopy* Uranium/plutonium separations* Zr O 2-UO 2 synthesis
Research on an aspect of the nuclear fuel cycle* A ssist in ongoing research projects
http://radchem.nevada.edu/classes/rfss/index.htmlWebpage is developed as resource for students
Lectures, readings, tests, homework, links
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O utcomes
1. Understand, utilize, and apply the chart of the nuclides to radiochemistry and nucleartechnology
Bring chart of nuclide to classUnderstand chart of the nuclidestructureA ccess and utilize presented data
2. Understand the fundamentals of nuclearstructure
Why do nuclei have shapes other thansphericalRelationship between shape andbehavior
3. Understand chemical properties of radioelements
Focus on actinidesFilling of 5f electron orbitals
Technetium, promethiumRadioelements Z
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O utcomes
4. Comprehend and evaluate nuclear reactions andthe production of isotopes
Use chart of the nuclidesCross section data
Reaction particlesNeutrons, alpha, ions, photonsReaction energies
Mass differences5. Comprehend types and descriptions of
radioactive decayExpected decay based on location of isotopein chart of the nuclidesD ecay modes relationship with half-life
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O utcomes
6. Utilization of radiochemistry in researchEvaluation of concentrationBehavior of radioelements
Exploitation of isotopes7. Investigate modern topics relating
radiochemistry to the nuclear fuel cycleResearch basis in laboratoryLiterature reviewPresentation of results
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Grading: Lecture course
Pop-quizzes at end of lecture (25 %)Based upon presented information
Five comprehensive quizzes (15 % each)Based on topic covered in lecture and pop
quizzesGoal of quizzes is material comprehensionNature of comprehensive quizzes
In classTake home
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Grading: Laboratory4 groups for initiallaboratoriesWrite up for 4 laboratories(10 % each)
Gamma spectroscopyA
lpha SpectroscopyZr O 2-Pu O 2 synthesisU-Pu separation
O ne report fromeach group
Report on research (30 %)Presentation of research (30%)
15 minute presentation
at end of course
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Laboratory Modules
Radiation safety1st module taken by all students
Swipes, handing of material, generalprotocols
A lpha spectroscopyInverse square lawIsotopicsD ecay energy branching
Gamma spectroscopyCalibrationMeasuring samples
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Laboratory Modules
Radiochemical separationsSolvent extraction with tributylphosphateSeparation of Pu from U
Formation of oxide ceramicsPrecipitation from saltsZr O 2Zr O 2 UO 2Basis for formation of nuclear fuel
Focus on concepts useful for the nuclear fuelcycle
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Grading: LaboratoryReports format from manuscript preparation
A bstractIntroduction
BackgroundWhy is the research performed
ExperimentalMethodsEquipment
Results and discussion
What was observed, what does it meanConclusion
Restatement of main discussion pointsA nswers question posed in introduction
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O utline: LecturesClass # D ate Topic
1 Monday 07-Jun Orientation, Introduction, Chart of the nuclides (0800 start, SEB2251)
2 Tuesday 08-Jun Cosmochemistry (processes), Nuclear properties (masses and matter distribution)
3 Wednesday 0 -Jun Ken Moody Presentation ( H RC A uditorium, 1330-1530 )
4 Thursday 10-Jun Decay Kinetics (equations, utilization natural radiation, dating)(A fternoon lecture, 1330-1630 )
5 Friday 11-Jun Review and Quiz 16 Monday 14-Jun Tour of General A tomics: A lpha D ecay Lecture7 Tuesday 15-Jun Tour of San O nofre Nuclear Power Plant8 Wednesday 16-Jun Alpha Decay, Beta Decay
9 Thursday 17-Jun Beta Decay (continued), Gamma Decay10 Friday 18-Jun Fission (models and product distribution), Dosimetry11 Monday 21-Jun Nuclear Structure and Models and Nuclear Forces12 Tuesday 22-Jun Nuclear Reactions (Energetics, Mechanisms, Cross Sections)13 Wednesday 23-Jun Nuclear Reaction (continued), Analytical Applications (neutron
activation, tracers)14 Thursday 24-Jun Review and Quiz 215 Friday 25-Jun Uranium Chemistry and Enrichment
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O utline: LecturesClass # D ate Topic16 Monday 28-Jun Chemistry in Reactor Fuel17 Tuesday 2 -Jun Actinide Chemistry18 Wednesday 30-Jun Fission Product Chemistry
19 Thursday 01-Jul Review and Quiz 320 Friday 02-Jul Nuclear Fuel Design and Fabrication
21 Monday 05-Jul Light Water Reactor Fuel22 Tuesday 06-Jul Fast Reactor Fuels23 Wednesday 07-Jul Particle Fuels
24 Thursday 08-Jul Review and Quiz 425 Friday 0 -Jul History of Nuclear Fuel Reprocessing
26 Monday 12-Jul Modern Nuclear Fuel Reprocessing27 Tuesday 13-Jul Design Considerations in Fuel Reprocessing28 Wednesday 14-Jul International Nuclear Fuel Cycle Center
29 Thursday 15-Jul Waste Forms and Repositories ( Quiz 5 Take H ome)30 Friday 16-Jul Presentations
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O utline: LaboratoriesClass # D ate Topic
1 Monday 07-Jun Radiation Safety Training (Tom ODou)2 Tuesday 08-Jun General Laboratory Procedure (Nick Smith)3 Wednesday 0 -Jun Laboratory I (0 00-1200)
4 Thursday 10-Jun Laboratory II (0 00-1200)5 Friday 11-Jun Laboratory write up6 Monday 14-Jun Tour of General A tomics
7 Tuesday 15-Jun Tour of San O nofre Nuclear Power Plant8 Wednesday 16-Jun Project Review
9 Thursday 17-Jun Laboratory III (1330-1630)10 Friday 18-Jun Laboratory IV (1330-1630)11 Monday 21-Jun Development and literature review for project12 Tuesday 22-Jun Development and literature review for project13 Wednesday 23-Jun Project discussion and initiation
14 ThursdayTuesday
24-Jun13-Jul
Research
28 Wednesday 14-Jul Report and presentation finalization
29 Thursday 15-Jul Report and presentation finalization30 Friday 16-Jul Presentations
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H istory of Radiation Research1896 D iscovery of radioactivity
Becquerel used K 2UO 2(SO 4)2 H 2O exposedto sunlight and placed on photographicplates wrapped in black paperPlates revealed an image of the uraniumcrystals when developed
1898 Isolation of radium and poloniumMarie and Pierre Curie isolated from U ore
1899 Radiation into alpha, beta, and gammacomponents, based on penetration of objects andability to cause ionization
Ernest Rutherford identified alpha1909 A lpha particle shown to be H e nucleus
Charge to mass determined by Rutherford
1911 Nuclear atom modelPlum pudding by Rutherford1912 D evelopment of cloud chamber by Wilson1913 Planetary atomic model (Bohr Model)1914 Nuclear charge determined from X rays
D etermined by Moseley in Rutherfordslaboratory
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H istory1919 A rtificial transmutation bynuclear reactions
Rutherford bombarded 14N withalpha particle to make 17O
1919 D evelopment of mass
spectrometer1928 Theory of alpha radioactivity
Tunneling description by Gamow1930 Neutrino hypothesis
Fermi, mass less particle with spin, explains beta decay1932 First cyclotron
Lawrence at UC Berkeley
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H istory1932 D iscovery of neutron
Chadwick used scattering datato calculate mass, Rutherfordknew A was about twice Z.Lead to proton-neutron nuclearmodel
1934 D iscovery of artificial
radioactivityJ ean Frdric J oliot & IrneCurie showed alphas on A lformed P
1938 D iscovery of nuclear fissionFrom reaction of U with
neutrons,H
ahn and Meitner1942 First controlled fission reactor1945 First fission bomb tested1947 D evelopment of radiocarbondating
i
nle
3014
3015
3015
10
2713
42
p
p
F
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Radioelements
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Technetium
Confirmed in aD
ecember 1936experiment at the University of PalermoCarlo Perrier and Emilio Segr.Lawrence mailed molybdenum foilthat had been part of the deflectorin the cyclotron
Succeeded in isolatingthe isotopes 95,97 TcNamed afterGreek word , meaningartificial
University of Palermo officialswanted them to name theirdiscovery " panormium ", afterthe Latin namefor Palermo, Panormus
Segre and Seaborg isolate 99m Tc
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Promethium
Promethium was first produced andcharacterized at O RNL in 1945 by J acob A .Marinsky, Lawrence E. Glendenin and CharlesD . Coryell
Separation and analysis of the fission productsof uranium fuel irradiated in the GraphiteReactorA nnounced discovery in 1947
In 1963, ion-exchange methods were used atO RNL to prepare about 10 grams of Pm fromused nuclear fuel
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Np synthesis
Neptunium was the first synthetic transuranium element of theactinide series discoveredisotope 239Np was produced by McMillan and A belson in1940 at Berkeley, Californiabombarding uranium with cyclotron-produced neutrons
238U(n, K)239U, beta decay of 239U to 239Np (t 1/2=2.36 days)
Chemical properties unclear at time of discoveryA ctinide elements not in current locationIn group with W
Chemical studies showed similar properties to UFirst evidence of 5f shellMacroscopic amounts
237Np238U(n,2n) 237U
* Beta decay of 237U10 microgram
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Pu synthesisPlutonium was the second transuranium element of the actinide
series to be discoveredThe isotope 238Pu was produced in 1940 by Seaborg,McMillan, Kennedy, and Wahldeuteron bombardment of U in the 60-inch cyclotron atBerkeley, California
238U( 2H , 2n) 238Np
* Beta decay of 238
Npto238
PuO xidation of produced Pu showed chemically different
239Pu produced in 1941Uranyl nitrate in paraffin block behind Be target bombardedwith deuteriumSeparation with fluorides and extraction with diethyletherEventually showed isotope undergoes slow neutron fission
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A m and Cm discoveryProblems with identification due to chemicaldifferences with lower actinides
Trivalent oxidation state239 Pu( 4H e,n) 242 Cm
Chemical separation from PuIdentification of 238 Pu daughter from alphadecay
A m from 239 Pu in reactorA
lso formed242
CmD ifficulties in separating A m from Cm andfrom lanthanide fission products
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Bk and Cf discovery
Required A m and Cm as targetsNeeded to produce theses isotopes in sufficientquantities
MilligramsA m from neutron reaction with PuCm from neutron reaction with A m
241 A m( 4H e,2n) 243Bk Cation exchange separation
242Cm( 4H e,n) 245Cf A nion exchange
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Cf data
D owex 50 resinat 87 C, elutewith ammoniumcitrate
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Einsteinium and Fermium
D ebris from Mike test1st thermonuclear test
New isotopes of Pu244 and 246
Successive neutron capture of 238UCorrelation of log yield versus atomic mass
Evidence for production of transcalifornium isotopesH eavy U isotopes followed by beta decay
Ion exchange used to demonstrate new isotopes
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1. E decay (occurs among the heavier elements)
2. F decay
3. Positron emission
4. Electron capture
5. Spontaneous fission
Types of D ecay
Energy Rn Ra p E 4222286
22688
E nergy Xe I p R F
131
54
131
53
Energy Ne Na p R 22102211
Energy Mg Al p R 26122613
Energyn RueCf p10
10844
14054
2528 4
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Fission ProductsFission yield curve varies with fissile isotope
2 peak areas for U and Pu thermal neutron induced fissionVariation in light fragment peak
Influence of neutron energy observed 235U fission yield
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Chart of the Nuclides
Presentation of data on nuclidesInformation on chemical elementNuclide information
Spin and parity (0 + for even-even nuclides)Fission yield
Stable isotopeIsotopic abundanceReaction cross sectionsMass
Radioactive isotopeH alf-life
Modes of decay and energiesBeta disintegration energiesIsomeric statesNatural decay seriesReaction cross sections
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Chart of Nuclides
D ecay modesA lphaBetaPositronPhotonElectron captureIsomeric transitionInternal conversionSpontaneous fissionCluster decay
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Chart of the Nuclides QuestionsH ow many stable isotopes of Ni?What is the mass and isotopic abundance of 84Sr?Spin and parity of 201 H g?D ecay modes and decay energies of 212 BiWhat are the isotopes in the 235 U decay series?
What is the half-life of 176Lu?What is the half-life of 176YbH ow is 238 Pu produced?H ow is 239 Pu made from 238U
Which actinide isotopes are likely to undergoneutron induced fission?Which isotopes are likely to undergo alpha decay?
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Radiochemistry Introduction
RadiochemistryChemistry of the radioactive isotopes and elementsUtilization of nuclear properties in evaluating and understanding chemistryIntersection of chart of the nuclides and periodic table
A tomZ and N in nucleus (10 -14 m)Electron interaction with nucleus basis of chemical properties (10 -10 m)
Electrons can be excited* H igher energy orbitals* Ionization
Binding energy of electron effects ionizationIsotopes
Same Z different NIsobar
Same A (sum of Z and N)Isotone
Same N, different ZIsomer
Nuclide in excited state99m Tc
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Terms and decay modes: Utilization of chart of the nuclides
Identify the isomer, isobars, isotones, and isotopes60m Co, 57Co, 97Nb, 58Co, 57Ni, 57Fe, 59Ni, 99m Tc
Identify the daughter from the decay of the followingisotopes
210 Po196 Pb204 Bi209 Pb222 A t212
Bi208 PbH ow is 14C naturally producedIdentify 5 naturally occurring radionuclides with Z
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X-rays
Electron from a lower level is removedelectrons of the higher levels can come to occupyresulting vacancyenergy is returned to the external medium as
electromagnetic radiationradiation called an X-ray
discovered by Roentgen in 1895In studying x-rays radiation emitted by uranium
ores Becquerel et. al. (P. and M. Curie) discoveredradioactivity in 1896
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X-raysRemoval of K shell electrons
Electrons coming from thehigher levels will emit photonswhile falling to this K shell
series of rays (frequency R or wavelength P) arenoted as K E, K F, K KIf the removed electronsare from the L shell,noted as L E, L F, L K
In 1913 Moseley studied thesefrequencies R , showing that:
where Z is the atomic number and, A and Z 0 are constants depending onthe observed transition.K series, Z 0 = 1, L series, Z 0 = 7.4.
K
L F
K F L E
K E
O
N
M
L
K
)( o Z Z A!R
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Fundamentals of x-rays
X-raysX-ray wavelengths from 1E-5 angstrom to100 angstrom
D e-acceleration of high energy electronsElectron transitions from inner orbitals* Bombardment of metal with high
energy electrons* Secondary x-ray fluorescence by
primary x-rays* Radioactive sources* Synchrotron sources
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H alf Lives
N/N o=e -Pt
N=N oe- Pt
P=(ln 2)/t 1/2
P is decay constant
Rate of decay of 131I as a function of time.
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Equation questions
Calculate decay constant for the following75Se74m Ga81Zn
What percentage of 66A s remains from a givenamount after 0.5 secondsH ow long would it take to decay 90 % of 65Zn?
If you have 1 g of 72
Se initially, how muchremains in 12 days?
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Forces in nature
Four fundamental forces in natureA ll interactions in the universe are the result of these forces
GravityWeakest forcemost significant when the interacting objects are massive,
such as planets, stars, etc.Weak interaction
Beta decayElectromagnetic force
Most observable interactions
Strong interactionNuclear properties
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Fundamental Forces
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Classic and relativistic
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Use of relativistic terms
relativistic expressionsphotons, neutrinosElectrons > 50 keVnucleons when thekinetic energy/nucleonexceeds 100 MeV
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Wavelengths and energy
Planck evaluated minimum from ( Ex ( t when he studied theradiation emitted by a black body at a given temperatureQuantum called Plancks constant h (h = 6.6 10 -34 J .s).
radiation conveys energy E in the form of quanta E = h R R the frequency of the emitted radiation
Based on the wave mechanics worked out by de Broglie P = h/p
P is the wavelength associated with any moving particle withthe momentum p
T!
!
2h
p/
J
J&
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Wavelengths
Photon relationships
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Particle Physics: Boundary of Course
fundamental particles of nature and interactionsymmetriesParticles classified as fermions or bosons
Fermions obey the Pauli principle
antisymmetric wave functionshalf-integer spins* Neutrons, protons and electrons
Bosons do not obey Pauli principle* symmetric wave functions and integer spins
Photons
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Particle physics
Particle groups dividedleptons (electron)hadrons (neutron andproton)
hadrons can
interact via thestrong interactionBoth can interactwith other forcesFermionic H adrons
comprised of quarks
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Topic review
H istory of nuclear physics researchD iscovery of the radioelements
Methods and techniques usedTypes of radioactive decay
Understand and utilize the data presented in thechart of the nuclidesUtilize the fundamental decay equationsIdentify common fission productsD efine X-rays
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Study QuestionsWhat are the course outcomes?What were important historical moments inradiochemistry?Who were the important scientists in the
investigation of nuclear properties?What are the different types of radioactivedecay?What are some commonalities in the discoveryof the actinides?Provide 5 radioelements
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Pop Quiz
Provide 10 facts about 129 IFill in the periodic table