Metrology for New Generation Nuclear Power Plants–MetroFission

IEEE TRANSACTIONS ON NUCLEAR SCIENCE, VOL. 61, NO. 4, AUGUST 2014 2017

Metrology for New Generation Nuclear PowerPlants–MetroFission

Lena Johansson, Jean-Remy Filtz, Pierino DeFelice, Mohamed Sadli, Arjan Plompen, Jan Heyse, Bruno Hay,Alan Dinsdale, Stefaan Pommé, Philippe Cassette, and John Keightley

Abstract— This EMRP (European Metrology Research Pro-gramme) project, MetroFission, has been looking at solvingmetrological problems related to a new generation of nuclearpower plants. The proposed Generation IV power plants aredesigned to run safely, make efficient use of natural resources,minimize the waste and maintain proliferation resistance. Inorder to reach these goals, the reactor operation involves highertemperatures, high-energy neutron fluence, different types of fuelwhere the minor actinides are included etc. In this overview ofthe multidisciplinary project, which has 12 partners in 10 coun-tries, the work described has focused on improved temperaturemeasurements, investigation of thermal properties of advancedmaterials, determination of new and relevant nuclear data and de-velopment of measurement techniques for radionuclides suitablefor Generation IV power plants.

Index Terms—Digital signal processing, generation IV reactor,instrumentation, liquid scintillation, metrology, neutron cross-sec-tion, nuclear data, temperaturemeasurements, thermal properties,thermochemical data modelling.

I. INTRODUCTION

N UCLEAR energy is one of the energies which emit theleast greenhouse gases - such as -during its lifecycle.

With 31% of Europe’s electricity produced from nuclear at themoment, this is the most important low carbon technology in

Manuscript received July 29, 2013; revised December 14, 2013; acceptedApril 16, 2014. Date of publication July 08, 2014; date of current version Au-gust 14, 2014. This work was supported by the European Metrology ResearchProgramme (EMRP) . The EMRP is jointly funded by the EMRP participatingcountries within EURAMET and the European Union. The authors gratefullyacknowledge funding provided by the National Measurement Office of theUnited Kingdom Department for Business, Innovation and Skills.L. Johansson, A. Dinsdale, and J. Keightley are with National Phys-

ical Laboratory (NPL), Teddington, TW11 0LW, U.K. (e-mail: [email protected]; [email protected]).J.-R. Filtz and B. Hay are with Laboratoire national de Metrologie et d’essais

(LNE), F-78197 Trappes cedex, France (e-mail: [email protected]; [email protected]).P. DeFelice is with Istituto Nazionale di Metrologia delle Radiazioni Ioniz-

zanti (ENEA), I-00123 Roma C.P. 2400, Italy (e-mail: [email protected]).M. Sadli is with Conservatoire National des Arts et Metiers (CNAM),

FR-75141 Paris cedex 03, France (e-mail: [email protected]).A. Plompen, J. Heyse, and S. Pommé are with the European Commission

Joint Research Centre Institute for Reference Materials and Measurements(EC-JRC-IRMM), B-2400 Geel, Belgium (e-mail: [email protected]; [email protected]; [email protected]).P. Cassette is with Laboratoire National Henri Becquerel, F-91191 Gif sur

Yvette cedex, France (e-mail: [email protected]).Color versions of one or more of the figures in this paper are available online

at http://ieeexplore.ieee.org.

Digital Object Identifier 10.1109/TNS.2014.2320793

Europe’s energy mix [1]. Europe can maintain the current levelof nuclear energy by long-term operation of existing plants andan ambitious programme of new build. Some European coun-tries have already decided to build new nuclear reactors; otherEU countries are actively considering whether new nuclearpower plants should form part of their energy strategy [2], [3].The nuclear power plants currently in use are first genera-

tion Magnox and second generation advanced gas cooled andlight water reactors. Generation III+ type light water reactorsof the European Pressurized Water type are currently being de-ployed, e.g. in Olkiluoto in Finland and Flammanville, France.In terms of safety these designs have significant improvementsover second-generation reactors. The purpose of MetroFissionis to provide the metrological infrastructure necessary for thedesign of Generation IV (Gen IV) nuclear power plants. Thereare, however, some areas where this project will improve formergenerations of power plants.Gen IV aims to improve nuclear safety, improve proliferation

resistance, minimize waste and natural resource utilization andto decrease the cost to build and run such plants. Amongst other,these Gen IV reactors pose the following key challenges [4]:1. How can the temperatures bemeasured, since existing ther-mocouple-based methods will not work in the envisionedtemperatures and environments?

2. What materials should be used in these reactors and whatare their thermal properties?

3. What are the nuclear data and radionuclide and neutronmetrology techniques that will be needed?

In this multidisciplinary project, which includes twelveNational Measurement Institutes (NMIs) in 10 countries, wehave been working from the point of view of developing novelmetrology with traceability to the SI units in order to addressthese challenges.

II. SCIENTIFIC AND TECHNICAL OBJECTIVES

The EMRP project MetroFission [5] has aimed to address thementioned challenges by the following specific scientific andtechnological objectives:A. Contribute to improved temperature measurements for

nuclear power plant applications.B. Contribute to improved thermo-chemical data and mod-

elling for nuclear design.C. Development of reference metrological setups and

methods for the measurement of thermal properties ofadvanced materials at high and very high temperatures.Characterisation of reference materials for high tempera-ture thermal properties measurements.

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2018 IEEE TRANSACTIONS ON NUCLEAR SCIENCE, VOL. 61, NO. 4, AUGUST 2014

D. Contribute towards improved neutron cross section datathrough neutron fluence measurements and standards

E. Measurement of nuclear decay parameters and emissionprobabilities of priority nuclides.

F. Development of the Triple-to-Double Coincidence Ratio(TDCR) method for radionuclide standardisation of ra-dionuclides relevant to nuclear power and

G. Incorporate Digital Coincidence Counting (DCC) tomakethese systems mobile and suitable for on-site use.

A. New High-Temperature References, Sensors and ValidationMethods

New temperature sensors and methods for in-situ measure-ments in nuclear power plants have been investigated and devel-oped with an emphasis on extending the measurement range tohigher temperatures and characterising, limiting, or completelyeliminating the sensor drift in a high temperature, high-neu-tron-flux environment.Reference fixed points above the copper point (1084.62) have been developed as an auto validation method of

thermocouples measuring during irradiation and at high tem-perature and, if possible, to perform post-irradiation studies ofthermocouples. This project has achieved the realisation of theFe-C fixed point (1154 ); in a joint effort between NPL andLNE-CNAM, different combinations of materials and designshave been tested and a comparison of different realisations hasbeen performed [6]. The results show a promising repeatabilitywithin of this fixed point. It has been observed thatthere was no influence from the metal origin or differencebetween the two different designs. ITS-90 temperatures havebeen assigned by both NMIs.Suitable thermocouples from the Mo/Nb family were inves-

tigated. These thermocouples are showing negligible neutronicdrift (low neutron activation) [7]. The thermocouples were iden-tified, constructed, and studied with respect to their referencefunctions, stability, and thermoelectric homogeneity. The re-sults showed that the homogeneity of the thermo couples (sup-plied by Thermocoax) at 200 was better than 0.2 in allcases. However, the measurements at silver fixed point (961.78) showed instabilities, even after long annealing. Hence, a

decision was made to discontinue the work with Mo/Nb ther-mocouples within this project but might still be pursued in thefuture [8], [9].The practicality of self-validation methods for thermocou-

ples has been examined as a means to reduce or eliminatedrift related problems. Self-validating methods suitable forthermocouples were identified and feasibility demonstratedto high temperatures. Two methods were developed by bothLNE-CNAM (France) and NPL (UK). The mini-cells werebased on graphite crucibles, embedded on thermocouples. Themethods were compared to the copper point and measurementsgave an agreement within 0.8 . In order to achieve a proofof concept of an innovative driftless thermodynamic methodof temperature measurement, an acoustic thermometer wasstudied for possible application in an ionising environment attemperatures up to 1000 [10], [11].The aim of this task was to construct a demonstrator of a drift-

less primary thermometry method, by speed of sound measure-

Fig. 1. A PAT thermometer made from Inconel. The exposed length of Inconelis the temperature sensitive region.

ments in a gas. A prototype acoustic thermometer (PAT) was de-signed and constructed (Fig. 1), applicable to at least 1000 .It was demonstrated that the drift was less than 2 at 1000of this primary acoustic thermometer. The drift of the tempera-ture sensors was performed by comparison with thermocouplesthrough extended exposure in a high temperature environmentat NPL [12].

B. Improved Thermo-Chemical Data and Modelling

Following a review of the fuel and coolants of potentialuse in Gen IV nuclear plants it was decided that the work onthermodynamic modelling would concentrate on the develop-ment of data needed to support the development of the sodiumcooled fast reactor (ASTRID) in order to best target availableresources. There have already been a number of well-fundedsuccessful projects concerned with the development of data forthe nuclear fuel and its potential interaction with a clad. How-ever, there was limited modelled thermochemical data availableconcerning the liquid sodium coolant and its interactions withthe fuel, the containment materials and the environment whichled to that MetroFission decided to target this area. The useof chemical thermodynamic data is well established in the nu-clear sector and the various compilations of data thus far havebeen mainly concerned with the properties of stoichiometriccrystalline materials and gas phase species. However to modelcomplex chemical processes involving nuclear materials it isnecessary to model the thermodynamic properties of phasesover ranges of both temperature and composition. This requiresuse of the CALPHAD technique where critically assessed ther-modynamic data for component binary and ternary systems canbe extrapolated to multicomponent systems and then softwaresuch as MTDATA [13] used to calculate chemical and phaseequilibria. During this project a thermodynamic database hasbeen developed through critical assessment of all related exper-imental thermodynamic and phase diagram data for a numberof systems and data gleaned from the scientific literature.For the modelling, the nuclear fuel was taken to be based on

(see Fig. 2) but incorporating minor actinides suchas Np and Am. Data for the fuel, fission products and contain-ment materials have been reviewed and new data assessed torepresent their interaction with the Na coolant, in order to permit

JOHANSSON et al.: METROLOGY FOR NEW GENERATION NUCLEAR POWER PLANTS–METROFISSION 2019

Fig. 2. Calculated phase diagram for the Pu-U system.

calculation of phase and chemical equilibria for severe accidentscenarios. The ultimate aim is to publish the data developedduring this project within a revised version of “Thermochemicaldata for reactor materials and fission products”, last publishedin 1990.This resulted in a thermodynamic database. Data currently

in the MetroFission thermodynamic database represent the sys-tems:— O-U-Pu—Am-Fe-Np-Pu-U-Zr (some binary systems)—Mo-Pd-Rh-Ru-Tc (metallic fission products)

which have been validated, modified and/or reassessed withconsistent reference states for elements [14].Further critical assessments for the systems Na-O, Na-I, Cs-I,

Na-Te, Cs-Te, Zr-Te, and Zr-O are currently being carried outusing available experimental data supplemented by calculationsusing ab-initio quantum mechanics. This will be extended inany follow on project with the systems: Na-U-O, Na-Pu-O,Na-Fe-O, Na-Zr-O, Na-Cs, and Zr-I.The thermodynamic database(s) arising from this work will

be compatible with the major software packages used to calcu-late phase equilibria from thermodynamic data.Using the combination of models and data assessed in the

project it will be possible to make predictions related to thehigh-temperature phase equilibria (such as phase transformationtemperatures, vapour pressures or the potential interaction be-tween the fuel and coolant), which can partly be validated bycomparison with experimental observations.

C. Thermophysical Properties of Advanced Materials

This work package of the MetroFission project aimed to im-plement a European metrological infrastructure for the study ofthermophysical properties at high temperature [15], [16], [17]for materials having thermal properties similar to those used in

Fig. 3. New diffusivimeter of LNE.

fission reactors. The main objective was to enable the nuclearresearch laboratories to insure the traceability of the measure-ments that they carry out with their own apparatuses on irradi-ated materials and nuclear fuels in some cases up to 2000 .For that, the measurement capabilities of European NationalMetrology Institutes (LNE, PTB and NPL) for the characteriza-tion of thermal properties have been improved, with in partic-ular the development of new metrological facilities. Two com-plementary apparatuses have been designed by PTB and LNEfor the measurement of normal spectral emissivity of solid ma-terials up to 1500 , and the reference diffusivimeter of LNEhas been modified to perform thermal diffusivity measurementsup to 2000 .Fig. 3 shows the new configuration of the high temperature

diffusivimeter of LNE, and Fig. 4 presents a scheme of the lampimage furnace designed to heat the specimens up to 1500 inthe new high temperature emissometer of LNE. More informa-tion about the equipment developed in the framework of thisproject by PTB and LNE can be found in [18] and [19]. Theseapparatuses have been validated in their operating temperatureranges by measuring emissivity and thermal diffusivity of twohomogeneous materials (tungsten and graphite) [20]. Thermaldiffusivity measurements were also performed on these ma-terials by EC-JRC-ITU (Institute for Transuranium Elements)with two homemade facilities as well as by NPL and PTB withcommercial equipment. Obtained results are in agreement withmeasurements performed with the new high temperature diffu-sivimeter developed for this project and with data available inliterature. These new metrological facilities will be applied tothe characterisation of thermophysical properties of some ma-terials (Ni, MgO and ) that could be used as “transfer ref-erence materials” by nuclear research laboratories for high tem-perature thermal properties measurements.


Fig. 4. Schematic of the lamp image furnace of the high temperature emis-someter of LNE.

D. Improved Cross Sections Through Neutron Metrology

New fast reactor designs will involve materials exposed tohigher-energy neutron fields. The current nuclear databasesconcentrate on thermal energies. Work will need to be done todetermine and/or achieve lower uncertainties of nuclear dataat higher energies. Advantage was taken of the experience ofNational Metrology Institutes (NMIs) in neutron metrology,particularly fluence measurements. Practically the project aimsat improving neutron interaction data measurements beyondthe present state-of-the-art, which is set by self-normalizingmethods and the neutron data standards used at laboratorieswhere the data are measured [21], [22].The program of work included the establishment of an

easy-to-use secondary fluence standard at the EC-JRC-IRMM(Institute for Reference Materials and Measurements) GELINAfacility along with a procedure for reliable determination ofthe efficiency of fluence measurement devices used in neutrondata measurements at EC-JRC-IRMM and elsewhere. Theset-up consists of a fixed flux monitor, consisting of a doubleFrisch-gridded ionization chamber loaded with layers, anda reference chamber, consisting of a double Frisch-griddedionization chamber (see Fig. 5) loaded with a well characterized

layer on one side and a layer on the other side. Thisreference chamber was installed at one of GELINA’s flightpaths and allowed determining the neutron flux as a functionof neutron energy in an absolute way. The reference chambercan be replaced with any other fluence monitor in order to cal-ibrate this device. A multilayer parallel plate transfer chamberconsisting of 8 layers of was calibrated in this wayand used for fluence measurements at other neutron beams.All layers were prepared and carefully characterized atEC-JRC-IRMM.

Fig. 5. A double Frisch-gridded ionization chamber loaded with andwas used as a reference chamber for neutron fluence measurements.

Fig. 6. The 3.5 MV Van de Graaff accelerator at NPL (UK) produces mono-energetic neutrons in a low-scatter environment.

The potential of these fluence measurement devices wasdemonstrated by a number of neutron induced fission cross sec-tion measurements on and with mono-energeticneutron beams produced at two different NMIs, i.e. at the Van deGraaff accelerator and the cyclotron of the Physikalisch-Tech-nische Bundesanstalt (PTB) in Braunschweig (Germany) andat the Van de Graaff accelerator of the National PhysicalLaboratory (NPL) in Teddington (UK), shown in Fig. 6. Themeasurement were performed using gas filled detectors, con-sisting of a Frisch-gridded ionization chamber containing thePu sample, mounted back to back to a parallel plate chambercontaining a sample [23]. During the experiments theneutron fluence was measured in parallel with the parallelplate chamber and with the fixed neutron fluence monitorsavailable at the respective institutes.

E. Nuclear Decay Data

The minor actinides and their decay products have gener-ated increased interest in recent years because of their signifi-cant role in the foreseen development and adoption of nuclearfuel. A list of specific needs for improved actinide decay data


has recently been outlined in a review by the IAEA [24], [25].Responding to those needs, an objective of this project wasto measure the alpha-particle emission probabilities of ,using highly enriched material with certified isotopic compo-sition. Furthermore, as fission fragments containing more beta-decaying radionuclides will result from proposed fast reactors,developing beta spectrometry by cryogenic detectors was an-other objective aimed at improving the measurement of betaspectra and verifying theoretical models, particularly for thoseof the forbidden type. This will lead to improved calculations ofdecay heat produced by nuclear fission, a quantity important forsafe reactor operation (reactor shutdown, post irradiation han-dling of nuclear fuels).Thus two major objectives steer this part of the research at

improvingA) Our knowledge of decay data for radionuclides plays a

major role in power-related fields. It was proposed tomeasure some nuclear data that have been identified asincomplete or inconsistent, and in which NMIs couldprovide a major impact with their dedicated facilitiesfor primary standardization of radioactivity. NMIs havea proven record of providing accurate decay data suchas half-lives and alpha-particle emission probabilities.It was decided to perform alpha-particle emission prob-ability measurements in the decay of , for whichdecay data were very scarce and an explicit demand forbetter data had been expressed [24], [25]. To achievethis goal, extensive tests were needed to optimize thesource preparation by electrodeposition [26], the sourceshad to be measured for 1-2 years in several detectors[27] and a magnet system had to be developed to elim-inate interfering conversion electrons that distorted thealpha spectrum [28]. The quality of the alpha spectrumobtained, in terms of accuracy, statistical precision andenergy resolution was significantly better than in anyprevious measurement. The alpha-particle emissionprobabilities of have been improved by an order ofmagnitude [27]. The newly obtained decay data will bemade publicly available to the international community.

B) The use of a cryogenic detector - and in particular ametallic magnetic calorimeter - to measure beta energyspectra is quite innovative. It will help us to improve ourknowledge of the shape of beta spectra through exper-iment and implement this into theoretical models. Thenew technology of cryogenic detectors offers exceptionalcharacteristics in terms of energy resolution and detectionefficiency in a wide energy range. In particular, it canobtain information also at the low-energy side (thresholdas low as 180 eV), as it is less prone to energy losses andelectronic noise compared to other methods. Measure-ments have been performed on a beta spectrum with adecay through an allowed nuclear transition, , and ofa first forbidden transition, . The tests have taughtus how sources should best be prepared for this methodand has confirmed some theoretical models of the shapeof an allowed beta spectrum. It was also demonstratedto be applicable to , since for this nuclide certainspecial conditions are met. One of the most important

Fig. 7. An example of a miniature TDCR system (this specific prototype hasbeen developed at CEA-LNHB in France).

conclusions following from these measurements is theclear evidence for an ‘exchange effect’ occurring inbeta decay, which has as effect a clear increase of thebeta spectrum at low energy. No other measurement hasever demonstrated this effect so clearly, as the thresholdlevel in this experiment was exceptionally low [29]. Acorrection factor for the exchange effect has been im-plemented in the theoretical calculation of beta spectra,which correctly predicts the enhancement by 20% of thebeta spectrum of at 180 eV. This improvement willhave an impact in several fields, such as primary stan-dardization of radioactivity and decay heat calculations.More detailed results from the nuclear decay data workin MetroFission can be found in [30].

F. TDCR: Metrology for in-situ Activity Measurements

The general aim of this work was to enhance operation of newgeneration nuclear power plants (NNPP) by enabling on-sitemeasurement of low-energy beta-emitters created in the fuelcycle (e.g. ) and/or as activation products in the reactorand its enclosure (e.g. , , , etc.).Addressing the demand of nuclear power plants for on-site

activity measurements of pure beta emitters, the objective forthis part of the project was therefore to develop a miniature sizeTriple-to-Double-Coincidence-Ratio (TDCR) system, clearlyadvancing technology beyond the current state-of-the-art [31],[32], [33]. The aim was to develop metrology instrumentssuitable for use on-site, with lowered measurement uncer-tainties and traceability to SI units by applying the primarytechnique of TDCR. Five partners have built miniature TDCRsystems, miniaturising the instrument’s detection chamber byusing small and efficient photomultiplier tubes. One exampleis shown in Fig. 7. The systems [34], [35], [36], [37], [38], [39]have been validated with previously standardised radioactivesolutions and inter-compared using solutions of and ,with traceability to the International Reference System. A moredetailed description of the specific TDCR systems that wasdeveloped within the MetroFission project can be found in [36].

G. Digital Coincidence Counting for Radionuclide Metrology

The work has focused on the provision of a means of on-siteactivity standardisations for various photon-emitting radionu-clides that may be readily standardised using the - coin-


cidence counting technique [40]. The data acquisition systemsutilised are based on high-speed digitizers, where the A/D con-version is performed as close as possible to the outputs of thedetectors/preamplifiers [41]. Critical examinations on optimi-sation of the coupling of ADCs to the detector systems (inputimpedance, bandwidth and voltage ranges, signal to noise ratioetc.), as well as the analysis of the digitized data streams (both“on-line” and via list-mode data sets) in order to realise robust

- Coincidence Counting systems were performed as de-scribed in paper by Keightley et al. [42]. An international effortis now underway to develop a standard data format for list-modedata sets used in radionuclide metrology.

III. CONCLUSION

This paper presents on overview of the various work com-pleted within an EMRP Joint Research Project MetroFission,which started in September 2010. This project has aimed at pro-viding solutions to metrological challenges in relation to nuclearnew build and specifically Gen IV reactors so that these reac-tors can be designed, built and operate safely. The project pro-poses innovative temperature measurements in order to satisfythe need for measurements at the higher temperatures experi-enced in Gen IV reactors and possible solutions for long-termstability of such equipment. The project has delivered thermophysical and thermo chemical data, by experimental methodsand modelling, in order for new nuclear power plants to be ableto more accurately choose suitable construction materials andpredict their thermophysical behaviour. It has also addressed theissue of nuclear fuel and how accurate and traceable methodsof measurements of neutron flux and nuclear data can improvecross-section measurements, crucial for the calculation of thefission yield and the reactor efficiency. The nuclear data will fur-thermore benefit the operation of the power plant, once realised,as such data is required for calculations of for example the radi-ation heat. With regards to methods for radionuclide metrologythat previously were designated to specialist primary conditions,this project has been investigating the possibility of realising anin-situ measurement facility that will enable accurate determi-nation of difficult to measure radionuclides during operation. Insummary, this project has provided a range of metrology solu-tions, with a focusing on traceability to SI units that are workingtowards the realisation of a low-carbon emission source of en-ergy that will provide Europe with a source of sustainable en-ergy.

ACKNOWLEDGMENT

The authors would like to thank all participating scientistsfrom CEA-LNHB (France), CEM (Spain), CIEMAT (Spain),CMI (Czech Republic), CNAM (France), ENEA (Italy),IFIN-HH (Romania), JRC-IRMM (Belgium), JRC-ITU (Ger-many), LNE (France), NPL (UK), PTB (Germany), and SMU(Slovakia) for their contributions to this project.The authors also wish to thank Dr. Andrew Worrall,

Dr. Massimo Salvatores, Dr. Uwe Hampel, Mathias Laurie, andDr. Jacques Lechelle for their scientific expertise and advisoryrole in the MetroFission project.

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Metrology for New Generation Nuclear Power Plants–MetroFission