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Improvement of INVS measurement uncertainty for Pu and U-Pu nitrate solution

Pu及びU-Pu硝酸溶液に対するINVS測定の高精度化

牧野 理沙; Swinhoe, M. T.*; 鈴木 快昌 ; 向 泰宣 ; Menlove, H. O.*; Marlow, J. B.*; 中村 仁宣 

Makino, Risa; Swinhoe, M. T.*; Suzuki, Yoshimasa; Mukai, Yasunobu; Menlove, H. O.*; Marlow, J. B.*; Nakamura, Hironobu

在庫サンプル測定システム(INVS)は、プルトニウム転換技術開発施設の査察において採取されたサンプル中のMOX粉末またはPu溶液中のPu量を測定する非破壊測定装置であり、31.3%の比較的高い検出効率を有している。現在のINVSの測定不確かさは、3-5%程度であるが、仮に測定の不確かさを1%以下まで改善することができれば、計量管理に用いる破壊分析の低減、Puの迅速確定、Kエッジデンシトメトリー(KEDG)の代替機器としての活用等、種々の効果が期待できる。本研究では、INVSの高精度化を目的として、実際の硝酸Pu溶液(再処理施設で通常用いられている濃度範囲に限定)を用いた校正試験を、3つの手法(キャリブレーションカーブ法、known-$$alpha$$法及びマルチプリシティ法)を適用して行った。なお、実試料の測定に先立ち、検出器の最適なパラメータ及び測定位置を確認する特性試験を行い、最適化されたパラメータを用いて校正を行った。校正試験の結果、それぞれの手法において不確かさに違いはあるものの、計数値とPu量との間に良い相関があることを確認した。特にキャリブレーションカーブ法が最も相関がよく、結果として1%以下の測定不確かの測定ができる見通しを得ることができた。溶液の測定は、様々な因子(濃度,酸濃度及び容量)が影響を与えるため、その結果についてもあわせて考察を行った。

The Inventory Verification Sample systems (INVS) is a non-destructive assay (NDA) system for small inventory samples to quantify the Pu amount in Pu and U-Pu nitrate solutions and MOX powder with 31.3% counting efficiency (for Cf). It has been used for IAEA safeguards measurement for many years at the Plutonium Conversion Development Facility (PCDF) for the samples taken at the time of Random Interim Inspection (RII) and Physical Inventory Verification (PIV), and is currently used as partial defects verification equipment with uncertainty about 3$$sim$$5% accuracy for solution samples. The INVS is a inline detector therefore it is very convenient to use since it can be used for a sample inside the glove box without bag-out. If the measurement uncertainty can be improved (to $$sim$$1%), it is expected that the usage can be extended to the operator's own measurements in MC&A to reduce effort and the number of destructive analyses (DA). In order to improve the measurement uncertainty, we have performed multiplicity measurements using a variety of solution samples (concentration, acidity and volume) to determine the Pu amount and uncertainty, although the multiplicity analysis is challenging. To control the measurement quality, a few MOX ceramic fuel pellets with known Pu amount are used. The results are evaluated by three kinds of methods (calibration curve, known-$$alpha$$ and multiplicity) to determine the best measurement method. In the range of concentration of typical samples, we could confirm good correlations between measured doubles and $$^{240}$$Pu effective mass in the three methods. Especially, the conventional calibration curve method showed a good performance with short measurement time and small uncertainty when the calibration standards were a good match to the unknown samples. In this paper, we present the INVS system design and measurement results with uncertainty using solution samples and comparison results among the three calibration methods.

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