On Site Laboratories of Euratom at Sellafield and La Hague ... · Introduction: nuclear safeguards...

P. Schwalbach, F. Lipcsei, M. Boella, P. ChareDG ENERGY Dir Nuclear Safeguards, LuxembourgK. Casteleyn, L. Duinslaeger, K. Lützenkirchen, P. van Belle, E. ZulegerJRC ITU KarlsruheY. Aregbe- JRC IRMM Geel

On Site Laboratories of Euratom at Sellafield and La Hague

Ten Years of Excellent Results with Nuclear Reference Materials

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| 2The Future of Reference Materials – Science and Innovation – IRMM Geel 24/11/2010

� Contents

.Introduction: nuclear safeguards in Europe

.On Site Laboratories at the reprocessing facilitiesin Sellafield and La Hague

.The methods for the analysis of nuclear material

.Quality Control: use of reference materials

.Conclusion


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Introduction

.Implementation of Euratom’s nuclear material control» in 25 non nuclear weapon states and» in 2 nuclear weapon countries (FR, UK).Implementation of Verification Agreements under the

Non-Proliferation Treaty in co-operation with the IAEA.Assuring implementation of other international nuclear co-operation agreements.More than 120 inspectors (~1500 inspections/year).More than 1000 installations in 27 countries.Full fuel cycle, including Pu and U bulk handling» Enrichment plants» Fuel fabrication plants » Reprocessing plants: FR, UK

DG ENER Directorate E: Nuclear Safeguards

The Future of Reference Materials – Science and Innovation – IRMM Geel 24/11/2010


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�.Compliance Control» Accounting checks» Verification of construction and process declarations

(Basic Technical Characteristics- BTC).Performance Control» Audit the quality of operators

Nuclear Material Accounting System .Credibility Control» Physical Verifications: measurements etc

Three Types of Control

Physical Verification of Nuclear Materials

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.Item counting and Identification.Non Destructive Assay.Destructive Assay

Gross deviations

Partial deviations

Bias/small deviations

Introduction


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.Reprocessing» ~ 800 t HM/y – 8000 kg Pu/y.MOX fuel fabrication» ~ 100 t HM/y – 8000 kg Pu/y.LEU fuel fabrication» ~ 700 t HM/y .Measurement methods with

highest accuracies are needed

to detect small deviations.Use Destructive Assay methods

Material Balance Challenge:Bulk handling → high throughput

Introduction


�« Take the analyst to the material –

not the material to the analyst »


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.1992 EC decision On-Site Laboratories (OSL). No transports (time, cost, risk, public acceptance). Timely analysis . Quick response to discrepancies. Analysis of unstable samples,

highly active samples. Sample authentication.Waste disposal on-site. Economic benefit vssample transport off-site

On Site Laboratories

Where to analyse the material?


�Commercial reprocessing plants

Areva NC, La Hague, France

Laboratoire Sur-SiteStart-up June 2000

Sellafield Limited, Sellafield, UK

On-Site LaboratoryStart-up October 1999



� Sellafield On-Site Laboratory

.Glove box environment

.Hot Cell environment at THORP

.Two active laboratories

Robotised glove box for separation chemistry and alpha counting



� La Hague On-Site Laboratory

.Three active laboratories » Hot cell facilities» Product (PuO2) lab» Mass spectrometry lab» Hot cell environment plus

glove boxes for low

activity work

Hot cell suite for handling of dissolved spent fuel samples and their assay by Hybrid K-edge densitometry and/or spiking



�Type and number of samples

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About 8200 samples(since 2000)

21400 measurements



� The tasks of the on-site laboratories are:

.Determine the concentration and isotopic composition of Pu and U in process liquors .The same in solid product samples (powders).Safeguards key measurement points par excellence» the reprocessing input

(here the amount of plutonium generated in a reactor

can be accurately determined for the first time)

» The product output (PuO2 nitrate, powder)

.Criteria for selecting the analytical methods were based on a combination of highest possible accuracy (up to 0.1 %) and minimum resource consumption

Analytical Methods


� Analytical methods for element assay

Hybrid K-Edge Densitometry (HKED)

- An alternative X-ray technique- Not as accurate as IDMS, but simple- Analysis completed within 1 hour

Isotope Dilution Mass Spectrometry (IDMS)

- Primary reference method- Highest accuracy, but sophisticated - Analysis not completed within 1 day

©H. Ottmar

Analytical Methods


� Hybrid K-Edge Densitometry

2) X-ray fluorescence:Pu and U conc, 0.5-40 g/l

Accuracy: 0.5 – 0.6 %

and Pu/U ratio, acc. 0.3-0.65%

1) K-edge densitometryPu and U, 50-350 g/l

Accuracy: 0.2 %

Photon Source

(X-ray tube)

Transmitted photon beamfor KEDG

Sample

HPGe

detector

HPGe

detector

Fluoresced

X-ray beam

for K-XRF

1) + 2): HKED – Hybrid K-edge

Accuracy: 0.2 % for U

0.3 – 0.65 % for Pu

Analytical Methods


� Isotope Dilution Mass Spectrometry

.Thermal Ionisation Mass Spectrometry» JRC developments

• Use of LSD (Large-Sized Dried) spike (IRMM)• Total evaporation (ITU)• Robust reliable procedures (ITU)

.Accuracies» U: 0.07 %

» Pu: 0.06 %.Used for:» Quality control

» Calibration

» Resolve operator –

Inspector differences

Analytical Methods


� Elaborate quality assurance to stay routinely within ESARDA Target Values

.5 independent levels» Instrument operation

» Procedural accuracy» Duplicate sample measurements with comparison to

reference materials

» Permanent method inter-comparison

» External quality control

.Basis of quality control» Primary method IDMS

» Certified Reference Materials provided by IRMM

Quality Control


� Certified Reference Materials


�.First level QC instrument check + mass calibration» HKED

• IRMM 3501 U/Pu K-edge CRM 250/2.5 g/l• BC 2113 U/Pu mixture RM of various concentrations

(200/1.3, 150/1.5, 150/1)• BC 567 low enriched U RM (270 and 90 g/l)• BC 831M natural U RM (360 and 180 g/l)

» Mass Spectrometry• IRMM 183, 184, 185, 186, 187: U isotope CRM with

235U abundances ranging from depleted to lowenriched (0.3 %, 0.7 %, 2.0 %, 3.0 % and 4.5 %)

• IRMM 290 A1 to G1 Pu isotope CRM with abundance ratio 239Pu/242Pu from 0.1 to 10

• IRMM 199 U isotope CRM with 33.3 % each of 233U, 235U, and 238U

Quality Control


� Secondary Reference Solutions


�.Second level QC material undergoes the same treatment and measurements as the samples

» HKED• CRMs as used for first level QC• Reference materials prepared out of sample

material and certified using IDMS

» Mass Spectrometry• Reference materials prepared out of

sample material and certified using CRMs (as used for first level QC) and IDMS

Quality Control


� HKED calibration


�.Energy-dispersive X-ray methods are not primary ones,they require calibration and frequent re-calibration» Calibration solutions

• Prepared out of samples to achieve various concentrations and U/Pu ratios

• Certified using IDMS using IRMM 1027 LSD spike

» Accuracy of OSL element assay results is dependent on LSD spike which provides traceability to the SI unit

• Increased accuracy• IRMM 1027 e uncertainty U: 0.087 %

Pu 0.089 %

• IRMM 1027 m uncertainty U: 0.019 %

Pu: 0.040 %

Quality Control


� External Quality Control

.Eqrain quality control programme for uranium CETAMA

Quality Control


� External Quality Control

.IRMM REIMEP round robin quality control isotopic ratios

Quality Control


� Conclusion


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.Direct physical verification of nuclear material is fundamental to Euratom Safeguards

.The On-Site Laboratories –» deliver now for 10 years high-quality, independent

measurements –» play a crucial role for safeguards at reprocessing

plants

.Nuclear Reference Material providers, mainly the Institute of Reference Materials and Measurements, support directly the OSLs to achieve the required high level of detection probability for small deviations

Conclusion

On Site Laboratories of Euratom at Sellafield and La Hague ... · Introduction: nuclear safeguards...

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