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Recent Progress in Research and Development in Neutron Resonance Densitometry (NRD) for Quantification of Nuclear Materials in Particle-Like Debris

Abstract To quantify special nuclear materials (SNM) in particle-like debris, a technique named neutron resonance densitometry (NRD) has been proposed. This method is a combination of neutron resonance transmission analysis (NRTA) and neutron resonance capture analysis (NRCA) or prompt gamma-ray analysis (PGA). In NRTA, neutron transmission rate is measured as a function of neutron energy with a short flight path time-of-flight (TOF) system. Characteristic neutron transmission dips of Pu and U isotopes are used for their quantification. Materials in the samples (H, B, Cl, Fe, etc.) are measured by the NRCA/PGA method. For the NRD measurements, a compact TOF facility is designed. The statistical uncertainties of the obtained quantities of the SNMs in a sample are estimated. A high-energyresolution and high-S/N γ-ray spectrometer is under development for NRCA/PGA. Experimental studies of systematic uncertainties concerning the sample properties, such as thickness and uniformity, are in progress at the TOF facility GELINA of European Commission (EC), Joint Research Centre (JRC), Institute for Reference Materials and Measurements (IRMM).

Keywords Capture • Fukushima • GELINA • Neutron resonance densitometry

• NRD • Nuclear security • Severe accident • Transmission

Introduction

Quantifying nuclear materials (NM) in the debris of melted fuel (MF) formed in a severe accident is considered to be difficult because of their variety of size, shape, unknown composition, and strong radioactivity. Although techniques of nondestructive assay (NDA) are indispensable for the evaluation of NM in debris, quantification methods have not been established so far [1]. In the cases of TMI-2 or Chernobyl-4, accounting for the NM was based on some estimations.

We have proposed a technique called neutron resonance densitometry (NRD) [2, 3] to quantify NM in particle-like debris that is assumed to be produced in the rapid cooling processes of a severe accident [4]. Small pieces are also produced when MF are cut or broken down to be taken out of the damaged reactors [1].

To examine the NRD method, studies have begun. Some experiments were carried out at the time-of-flight (TOF) facility GELINA [5] of EC-JRC-IRMM under the agreement between JAEA and EURATOM in the field of nuclear materials safeguards research and development.

In this chapter, we briefly describe the concept of NRD, give an overview of the development of NRD, and explain some parts of the recent progress.

Neutron Resonance Densitometry

The Concept of NRD

Neutron resonance densitometry is a method of a combination of neutron resonance transmission analysis (NRTA) and neutron resonance capture analysis (NRCA) or prompt gamma-ray analysis (PGA). The fundamental principles of NRTA and NRCA are described by Postma and Schillebeeckx [6].

In NRTA, neutron transmission is measured as a function of neutron energy with a TOF technique. Characteristic neutron transmission dips of Pu and U isotopes are observed in the neutron energy in the range of 1–50 eV [7, 8]. Measurements of these transmission spectra can be carried out with a short-flight path TOF system [9, 10]. Although strong γ-ray radiation from MF samples does not interfere with NRTA measurements, reduction of neutron flux caused by nuclei with large total cross section (such as H, B, Cl, Fe) makes accurate NM quantification difficult. Nevertheless, the quantities of these contained nuclei could not be determined by NRTA only, because these nuclei do not resonantly interact with neutrons in this energy range. To identify and to quantity the composing isotopes, the NRCA/PGA method is required. Characteristic prompt γ rays ware utilized. Table 2.1 shows prompt γ-rays emitted from nuclei after neutron capture reaction. Most of these discrete prompt γ-rays have significant intensities. The information obtained by NRCA/PGA enables us to determine the appropriate sample thickness and measurement time. This information also supports NRTA analysis.

Table 2.1 Energies of prominent prompt γ-rays and the first neutron resonances of nuclei

Nucleus

Reaction

Prompt γ rays (KeV)

First resonance (KeV)

1H

1H (n, γ) 2H

2,223

10B

10B (n, αγ) 7Li

478

170

27Al

27Al (n, γ) 28 Al

3,034, 7,724

5.9

28Si

28Si (n, γ) 29Si

3,539, 4,934

31.7

53Cr

53Cr (n, γ) 54Cr

835, 8,885

4.2

56Fe

56Fe (n, γ) 57Fe

7,631, 7,646

1.1

59Co

59Co (n, γ) 60Co

230, 6,877

0.132

58Ni

58Ni (n, γ) 59Ni

465, 8,999

6.9

Fig. 2.1 A rough draft of an NRD facility. The neutron flight path length for NRTA is 5 m and that for NRCA/PGA is 2 m

A Rough Draft of an NRD Facility

For practical application, the scale of an NRD facility should be minimized. Figure 2.1 shows a rough draft of the NRD facility. An electron linear accelerator with a power of 1 kW and acceleration voltage of 30 MeV is assumed [11]. High-energy neutrons are generated in the order of 1012 n/s by photonuclear reactions following Bremsstrahlung at the electron target. The generated neutrons are slowed down to epithermal energy by collisions in a moderator surrounding the target. Neutrons from the moderator are collimated to supply for NRTA and for NRCA/PGA.

The length of the flight path is important to design a TOF system, because the longer flight path reduces the neutron flux whereas it increases the energy resolution of the system. It may require at least a 5-m flight path to achieve a good enough resolution to resolve resonances of NMs below 50 eV in NRTA [9, 10]. A shorter neutron flight path is feasible for NRCA/PGA because the nuclei in Table 2.1 are identified by the prompt γ-ray energies. We consider that a 2-m flight path is sufficient for NRCA/PGA. The beam line lengths mainly determine the scale of

Table 2.2 Estimated statistical uncertainty of quantities of U and Pu isotopes in a sample

Nucleus

Concentration in a fuel (kg/tHM)

Statistic error (%)

238Pu

0.19

0.85

239Pu

5.25

0.074

240Pu

2.13

0.051

241Pu

1.23

0.23

242Pu

0.48

0.069

235U

14.6

0.049

238U

928

0.010

The measurements are assumed to be carried out for 40 min with a 1012 n/s neutron source

the facility. One beam line for NRTA and three beam lines for NRCA/PGA are placed as shown in Fig. 2.1. The sample size for NRTA is assumed to be 10–30 cm in diameter and 1–2 cm in thickness. In comparison, the sample size for NRCA/ PGA is smaller; the diameter is 1–2 cm, and the thickness is 1–2 cm. A collimator is placed between the NRCA/PGA sample and the γ-ray detector to reduce the background γ-rays from the sample. Because optimal sample thickness for NRTA strongly depends on the amount of impurities or matrix material, the quantity of the interfering nuclei in debris has to be measured roughly by NRCA/PGA preceding NRTA measurements [12].

The statistical uncertainties of NMs quantified by NRTA were estimated [12]. The size of a MF sample is assumed to be 1 cm in thickness and 30 cm in diameter. The weight of the sample becomes about 4 kg: it consisted of nuclear fuel (64 vol.%), natFe (8 vol.%), natB (8 vol.%), and 20 vol.% of vacancy. The composition of the nuclear fuel was taken from Ando and Takano [13] [a fuel of 40 GWd/t burn-up in a boiling water reactor (BWR)]. The measurement was assumed to be carried out for 40 min, in which 20 min was for sample and 20 min for background. Table 2.2 shows the estimated statistical uncertainties of quantified Pu and U isotopes in the sample. The achieved statistical uncertainties are less than 1 %.

With the measurement cycle given here, about 0.15 ton of debris can be handled in a day; this enables us to measure 30 tons of debris in a year (200 working-days are assumed). This amount can be increased with the number of NRTA beam lines.

 
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