電位規制クーロメトリーによる硝酸プルトニウム溶 …jolissrch-inter.tokai-sc.jaea.go.jp/pdfdata/JAEA...Masahiko YAMAMOTO, Atsushi ISHIBASHI, Tetsuya NAGAYAMA,

Masahiko YAMAMOTO, Atsushi ISHIBASHI, Tetsuya NAGAYAMA, Naoki SURUGAYAAkira KUROSAWA and Toshiaki HIYAMA

JAEA-Technology

2010-040

Precise and Accurate Determination of Plutonium

by Controlled-potential Coulometry and Its Uncertainty Evaluation

Technical Services Department Tokai Reprocessing Technology Development Center

Nuclear Fuel Cycle Engineering Laboratories Tokai Research and Development Center

December 2010

Japan Atomic Energy Agency

i

JAEA-Technology 2010-040

(2010 9 28 )

2000

ISO12183:2005 ( National Institute of Standard and Technology: NIST )

Pu(VI) Pu(IV) NBL CRM-126

0.1 % 0.05 % ( n=17 )2

239Pu

MOX MOX 15.5995 mgPu/g ISO/BIPM-GUM 95 % k=2 0.0036 mgPu/g 0.023 %MOX 319-1194 4-33

ii


Precise and Accurate Determination of Plutonium by Controlled-potential Coulometry and Its Uncertainty Evaluation

Masahiko YAMAMOTO, Atsushi ISHIBASHI, Tetsuya NAGAYAMA,

Naoki SURUGAYA, Akira KUROSAWA and Toshiaki HIYAMA

Technical Services Department, Tokai Reprocessing Technology Development Center Nuclear Fuel Cycle Engineering Laboratories, Tokai Research and Development Center

Japan Atomic Energy Agency Tokai-mura, Naka-gun, Ibaraki-ken

(Received September 28, 2010)

Precise and accurate analysis of plutonium is necessary for material control and safeguards in nuclear facilities. In this study, controlled-potential coulometry, which yields absolute results and high precision, was applied to the determination of plutonium for achieving the highest level of accuracy. The measurement cell and electrodes of our coulometry system were optimized following ISO12183:2005, and the calibration of the coulometer was performed using NIST (National Institute of Standards and Technology, U.S.) certified equipments.

The influences of fluoride which was used to dissolve a Pu metal and of nitrite which arise from the decomposition of nitrate were eliminated by adding sulfuric acid and amidosulfuric acid to the sample. Also, hydrogen peroxide was added to the sample to reduce Pu(VI) to Pu(IV).

A plutonium sample prepared from a Pu metal (NBL CRM126) was measured according to the procedure optimized in this study. As a result, the measured value agreed well with the certified value. The relative standard deviation was 0.05 % ( n=17 ).

For spike preparation of isotope dilution mass spectrometry (IDMS), a plutonium solution was prepared from MOX powder stored in Japan Atomic Energy Agency. The plutonium content in the prepared solution was characterized by coulometry. As a result, the plutonium concentration of 15.5995 mgPu/g was obtained. The uncertainty was calculated following the ISO/BIPM Guide to the Expression of Uncertainties in Measurements. The expanded uncertainty was 0.0036 mgPu/g with confidence interval of 95%. The results obtained by coulometry were also in good agreement with those obtained by IDMS. Thus the proposed coulometry method was successfully applied for the determination of plutonium at the highest level of precision and accuracy. Keywords: Plutonium, Coulometry, Uncertainty, GUM


iii

1. 1

2. 2

3. 4 3.1 4 3.2 4 3.3 5

4. 6 4.1 6 4.2 6

5. 8 5.1 8 5.2 Pu(VI)8 5.3 9

6. 10 6.1 10 6.2 10 6.3 11

7. MOX 12 7.1 12 7.2 12 7.3 13

8. 15

16


iv

CONTENTS

1. INTRODUCTION1

2. PRINCIPLE 2

3. EXPERIMENTAL4 3.1 Reagents 4 3.2 Plutonium Standard Sample 4 3.3 Apparatus5

4. UPGRADE OF COULOMETRY SYSTEM6 4.1 Selection of measurement cell and electrodes6 4.2 Calibration of the system6

5. OPTIMIZATION OF MEASUREMENT CONDITION8

5.1 Effect of fluoride and nitrite8 5.2 Effect of plutonium(VI)8 5.3 Selection of Oxidation and Reduction Potential9

6. ANALYSIS OF PLUTONIUM SAMPLE SOLUTION10 6.1 Buoyancy correction of mass measurement10

6.2 Results of plutonium contents 10 6.3 Day to day measurement variability 11

7. ANALYSIS OF PLUTONIUM SOLUTION PREPARED FROM MOX POWDER12 7.1 Measurement of iron contents in the sample12

7.2 Results of plutonium contents12 7.3 Evaluation of uncertainty 13

8. CONCLUSION 15

REFERENCE 16


v

CONTENTS of Figure

Fig. 1 18 Fig. 2 19 Fig. 3 19 Fig. 4 20 Fig. 5 21 Fig. 6 22 Fig. 7 23 Fig. 8 24 Fig. 9 25

CONTENTS of Table

Table 1 20 Table 2 21 Table 3 22 Table 4 24 Table 5 26 Table 6 27 Table 7 28

This is a blank page.


- 1 -

1.

1950 1,2)

3-7)

1980

1983 2000 ( PNC )( DOE )

( SRS ) ISO12183 8)

( MOX ) 9) 239Pu MOX

SI 1,2,10)

( NBL )0.05 % 11, 12)

ISO12183:2005

MOX


- 2 -

2.

3,5,7) PUREX

Pu(III) Pu(IV) + e-

Pu(III) E0-0.26 V vs SCE (E0Pu(III)/Pu(IV))Pu(III) Pu(IV) E0+0.24 V vs SCE 13)

Nernst

100%

( mgPu/g )(1) 13)

1000)(

)/('

fsF

MCQQgmgPu PuBS (1)

SQ ( count ) 'BQ ( count )

C ( C/count ) PuM ( g/mol )

F ( 96485.34 C/mol ) s ( g ) f

C (1)

'BQ

BQ QB(2) 13)

SSredox

redoxBBBB tIBB

SStIQQ

)(

)()(' (2)


- 3 -

BQ ( count ) oxS ( V ) redS ( V ) SI ( mA ) BI ( mA )

St ( sec ) Bt ( sec ) oxB ( V ) redB ( V )

(1) f Nernst (3) 4)

RTESnF

RTESnF

RTESnF

RTESnF

fred

red

ox

ox

)(exp1

)(exp

)(exp1

)(exp

0

0

0

0

(3)

0E Pu(III)/Pu(IV)( V ) R ( 8.3145 J mol-1 K-1 ) n ( ) T ( K )


- 4 -

3.

3.1 (1)

ADVANTECMILLIPOREMilli-Q

(2) 0.9 mol/L 134 mL 2000 mL

(3) 3 mol/L 112 mL 500 mL

(4) 8 mol/L 299 mL 500 mL

(5) 3 mol/L 34 mL 100 mL

(6) 4 mL 16 mL 4 mL

(7) - 0.1 mol/L -8 mol/L

(8) 20% 20 g 100 mL

(9) ( 3035.5 % )

(10) 1.5 mol/L 7.281 g 50 mL

(11) ( 1000 ppm )

3.2 ( 5.0192 mg/g ) NBL CRM126 20 %( 4.5 V ) NBL CRM126- 3 mol/L 6.1


- 5 -

3.3 (1) Fig. 1

PC ( :99.99 %:15 mm:20 mm ) Fisher Scientific ( :0.5-3.0 mm )Fig.2 SRS

Ortec 974 Quad Counter/TimerOrtec 4001A BIN 14)Hewlett-Packard 34970A PC Dell LATITUDE D830 HTBasic Matsusada RK-80 DC Power Supply

2.5 L/min (2) V-570

400-900 nm 5.0 nm 100 nm/min

(3) ICP Seiko Instruments ICP SPS7700

ICP 238.204 nmRF 1.2 kW15 mm 0.45 MPa 0.3 L/min 16 L/min


- 6 -

4.

4.1 2000 SRS ISO12183:200514) Fig. 3 5.1

8)

8 mol/L 8 mol/L 2.5 mm ( : 0.01 m ) 4.2 ( National Institute of Standard and Technology: NIST ) SI Automatic Systems Laboratory Model RR100Agilent 3458A Agilent 53131A

( 50 )

2 ( Volt Frequency Converter: VFC )

VFC 21.1 VFC 49.9453 10000.02945 count Hz V-1

( 100 ) 500 / 10


- 7 -

(1) C VFC (4) 13) Cth(5) C Cth

100.0154

C

CC

QtI

C (4)

C ( C/count ) CI ( A ) ct ( sec )

CQ VFC ( count )

SRth RL

C 1 (5)

thC ( C/count ) RL ( ) SR VFC ( count Hz V-1 )

C

C 10 0.0001 %ISO12183:2005 0.002 %


- 8 -

5.

5.1 NBL CRM126

15)

3 mol/L 1 mL 200

16) Fig. 4

17)

1.5 mol/LHNO2 + NH2SO3H H2SO4 + N2 + H2O 18)Table 1

0.5%-0.09% ISO12183:2005 13

5.2 Pu(VI)

1015 mgPu 3 mol/L 1 mL 200 0.9 mol/L 18 mL ( n=3 ) 0.20%Table 2 Pu(III) 20004000 Pu(III) Pu(IV) 6501400 ISO12183:2005 500700 13) ISO12183:2005

5 Pu(III)Table 2 99.599.7 % 99.9 % 8)


- 9 -

Cohen Pu(VI) Pu(III)Pu(III) Pu(IV) + e- 19)

Pu(VI) Pu(III) 7)

NBL CRM126 10 3 mol/L 6 Pu(VI)

Fig. 5 477 nm Pu(IV)833 nm Pu(VI) 26% Pu(VI)

Pu(VI) Pu(IV) Pu(VI) Pu(IV)Pu(VI)Fe(II)Fe(II) 20,21)Pu(VI)

100 L 1 90 30 Pu(IV) Fig. 6 Pu(IV)Pu(VI)Pu(VI) Pu(III)Pu(IV) Table 3 500 99.9%

Fig. 7 5.1 5.3 Fig. 7 0.9 mol/L Pu(III)/Pu(IV) E0 ISO12183:2005 0.91 V vs. SCE

Nernst E0 13) E0 0.69 V vs. SCE Pu(IV) 0.93 V vs. SCE ( E0 + 0.24 V vs. SCE )Pu(III) 0.43 V vs. SCE ( E0 - 0.26 V vs. SCE )


- 10 -

6.

6.1

(6)(7)8.0 g/cm3(8) 22)

fWmC (6)

SA

CAf

11

(7)

Cm ( g ) W ( g ) f

A ( g/cm3 )

C ( 8.0 g/cm3 )

S ( g/cm3 )

31015.273

)020582.000252.0(34844.0

tht

A (8)

( hPa ) t ( ) h ( % )

1012.8 hPa 19.0 66.0 %

1.1 g/cm3 1.00094 0.1 %(6)(8) 6.2 ISO12183:2005 415 mgPu 4 mgPu

10 gPu 0.1%


- 11 -

10 mgPu 15 mgPu 13)

1015 mgPu Fig. 7 Table 4 No.1No.2No.3 1012.515 mgPu No.1No.2No.3 5.0192 mgPu/g 0.1 %No.1No.2No.3 0.07 %0.05 %0.02 % 1015 mg 0.1% 6.3

2008/11/192009/1/23 Fig. 8 2008/11/192009/1/23 2 0.15 % 0.05 % ( n=17 ) 0.010.08 %2 Tandon 0.1 % 23) 2 0.1 %


- 12 -

7. MOX

7.1 Fe(II)/Fe(III)Pu(III)/Pu(IV) 0.668 V vs SCE 0.493 V vs SCE 13) 20,21)MOX

ICP-AES ICP-AES TEVA ( Eichrom ) MOX 0.0028 mgFe/g ISO12183:2005 1000 ppm (9) 13)MOX (9)

Fe

PuFeFePuCPu M

Mfmmm

0,

(9)

0,CPum Pu ( mg )

Pum Pu ( mg ) Fem Fe ( mg ) PuM Pu ( g/mol ) FeM Fe ( 55.847 g/mol )

Fef Fe (3) E0 Fe (0.493V)

7.2

MOX

MOX 15 mgPu Fig. 7 1015.3 hPa 25.4 53.0 % 1.244 g/cm3(6)(8)(9)

Fig. 9 MOX 15.5995 mgPu/g ( n=8 )

15.610 mgPu/g 0.06 %


- 13 -

7.3 MOX ISO/BIPM

Guide to the Expression of Uncertainties in Measurement (ISO/BIPM GUM) 24) 95 % k = 2 15.59950.0036 mgPu/g 0.023 %( International Target Value 2000: ITV2000 ) 25)

0.15%MOX MOX

ISO/BIPM GUM Table 5 Table 6 mPu7.3 Wsol WTare 2.4 %ICP-AES FeICP 2.3 % 1 %

mPu mPu(10)

1000)(

)('

fF

MCQQmgm PuBSPu (10)

SQ ( count ) 'BQ ( count ) C ( C/count )

PuM Pu ( g/mol ) F ( 96485.34 C/mol ) f Pu

),,,( 21 nxxxfy y

)(yuc ix )( ixu (11)

22 )()( iic xucyu (11)

ic (12) f

ii x

fc

(12)


- 14 -

ic Holland

26)(10)(10)(13)(18)(13)(18)Fig. 9 No.1 mPu,No.1 Table 7

111 1000 fFMCQm

PuS

Pu (13)

111 1000'

fFMCQm

PuB

Pu (14)

111 1000)'( fFMQQCm

PuBSPu (15)

111 1000)'( fFCQQMm

BSPu

Pu (16)

112 1000)'( fFMCQQFm

PuBSPu (17)

121 1000)'( fFMCQQfm

PuBSPu (18)

Table 7 mPu,No.1(QS

QB) 34 %51 % f 14 % 1 %


- 15 -

8.

SRS 2000 ISO12183:2005 NIST

Pu(VI) Pu(IV)

NBL CRM-126 0.10 % 1012.515 mg 0.070.050.02 %2 0.05 %

MOX MOX 15.5995 mgPu/g ISO/BIPM GUM 0.0036 mgPu/g 0.023 %ITV2000 0.15 %

IDMS 0.1 % MOX


- 16 -

1) , : , , 16, p.927-930 (1967).

2) , , : , , 15, p.1234-1238 (1966).

3) C.Bergey, : Precise Coulometric Determination of Uranium, Plutonium and Americium, Mikrochimica Acta, II, p.207-217 (1981).

4) M.K.Holland, J.R.Weiss, and C.E.Pietri : Controlled-Potential Coulometric Determination of Plutonium, Anal. Chem., 50, p.236-240 (1978).

5) G.C.Goode and J.Herrington : High-Speed Controlled-Potential Coulometry, Anal. Chim. Acta, 33, p.413-417 (1965).

6) G.L.Silver : Plutonium Coulometry, Talanta, 29, p.959-960 (1982). 7) W.D.Shults : Applications of Controlled-Potential Coulometry to the Detemination of

Plutonium, Tlanta, 10, p.833-849 (1963). 8) , , , K , V :

, 9, p.57-63, (2000).

9) , : , , 51, p.606-610 (2009).

10) , , , , , , , , , , , , , , : , , 57, p.363-392 (2008).

11) J. Neuhoff, A.Voeks, B.Srinivasan, D.Temer, M.Holland: Proceeding of INMM 45th Annual Meeting, (2004).

12) NBL Certificate of Analysis 126 (1986). 13) International Standard: Nuclear fuel technology controlled potential coulometry assay

of plutonium, Second Edition, ISO 12183:2005(E) (2005). 14) M.K.Holland and J.V. Cordaro: An Automated Instrument For Controlled-Potential

Coulometry: System Documentation, U.S. Department of Energy Publication, DP-1751 (1988).

15) American Society for Testing and Materials: Standard Test Method for Plutonium by Controlled-Potential Coulometry ASTM C1108-99 (1999).

16) , , , , : , , 11, p.627-631 (1971).

17) , , : XVII-2 , (1967), (). 18) , : , , 18,

p.1264-1265 (1969).


- 17 -

19) D.Cohen : Electrochemical Studies of Plutonium Ions in Perchloric Acid Solution, J. Inorg. Nucl. Chem., 18, p.207-210 (1961).

20) , : ,, 49, p.537-541 (2000).

21) J.R.Stokely and W.D.Shults : Controlled-Potential Coulometric Determination of Plutonium in the Presence of Iron, Anal. Chem., 43, p.603-605 (1971).

22) , , , : , 18, p.83-90, (2003).

23) L.Tandon, K.Kuhn, D.Decker, D.Porterfield, K.Laintz, A.Wong, M.Holland and D.S.Peterson: Plutonium metal standards exchange program for actinide measurement quality assurance (2001-2007), J. Radioanal. Nucl. Chem., 282, p.565-571 (2009).

24) International Standard: Evaluation of measurement data guide to the expression of uncertainty in measurement, JCGM 100:2008 (2008).

25) H.Aigner, R.Binner, E.Kuhn, U.Blohm-Hieber, K.Mayer, S.Guardini, C.Pietri, T.Adachi, B.Rappinger, B.Mitterand, J.Reed, O.Mafra-Guidicini and S.Deron : International Target Values 2000 for Measurement Uncertainties in Safeguarding Nuclear Materials, IAEA STR-327 (2001).

26) M.K.Holland and J.V. Cordaro: Mass measurement uncertainty for plutonium aliquots assayed by controlled-potential coulometry, J. Radioanal. Nucl. Chem., 282, p.555-563 (2009).


- 18 -

Fig. 1 Controlled-potential coulometry system for determination of plutonium installed by

SRS.

P

S

1D

P

S

A

ArGas

Working Electrode

Stirrer and motor

Digital Voltmeter

Coulometer

ControlComputer

Ar gas tube

Ar gas valve

Reference Electrode

Counter Electrode

Glove Box

Flowmeter


- 19 -

Fig. 2 Block diagram of the coulometry system

Fig. 3 Measurement cell and electrodes of coulometry system.

Glass tube for reference electrode

Reference electrode

Counter electrode

Glass tube for counter electrode

Working electrode

Measurement cell

OxidationPotentiostat

OrtecCounter/Timer

AutomationModule

Linear DC Power Supply

Isolation Module

DigitalAnalog

Converter

ControlComputer

DigitalVoltmeter

ReductionPotentiostat

IntegratorModule

WorkingElectrode

CounterElectrode

ReferenceElectrode

NIM BIN

Coulometer


- 20 -

Fig. 4 Plutonium sample after sulfuric acid treatment.

Table 1 Comparison of analytical results of plutonium samples with or without sulfuric acid and amidosulfuric acid treatment.

Sample ID Concentration

(mgPu/g)

Difference from certified value*

(%) No.1

(without H2SO4 and NH2SO3H treatment) 4.9962 -0.46

No.2 (with H2SO4 and NH2SO3H treatment)

5.0149 -0.09

*Certified value: 5.0192 mgPu/g


- 21 -

Table 2 Oxidation and reduction time and fraction electrolyzed of plutonium samples obtained by coulometric measurement.

Sample ID Reduction Time Pu Pu(III)

( sec )

Oxidation Time Pu(III) Pu(IV)

( sec )

Plutonium fraction electrolyzed

( % ) No.1 3983 650 99.5 No.2 2536 1392 99.5 No.3 2093 1047 99.7

-0.01

0.01

0.03

0.05

0.07

0.09

400 500 600 700 800 900

Wavelength [nm]

Abso

rban

ce

Pu(IV)Pu(VI)

Fig. 5 Absorption spectrum of plutonium sample in 0.9 mol/L HNO3. Pu concentration: 267 mg/L, Measurement range: 400-900 nm, Band width: 5.0 nm, Scanning speed: 100 nm/min.


- 22 -

-0.01

0.01

0.03

0.05

0.07

0.09

400 500 600 700 800 900

Wavelength [nm]

Abso

rban

ce

Pu(IV)

Fig. 6 Absorption spectrum of plutonium sample in 0.9 mol/L HNO3 after H2O2 treatment. Pu concentration: 267 mg/L, Measurement range: 400-900 nm, Band width: 5.0 nm, Scanning speed: 100 nm/min.

Table 3 Oxidation and reduction time and fraction electrolyzed of plutonium sample obtained by coulometric measurement after H2O2 treatment.

Sample ID Reduction Time Pu Pu(III)

( sec )

Oxidation Time Pu(III) Pu(IV)

( sec )

Plutonium fraction electrolyzed

( % ) No.1 542 484 99.9 No.2 492 429 99.9 No.3 523 464 99.9


- 23 -

Fig. 7 Optimized sample pretreatment scheme for determination of plutonium by controlled-potential coulometry.

Plutonium Sample

Aliquoting ( Pu1015 mg/cell )

Valence Adjustment ( H2O2 100 L )

Add 3 mol/L H2SO4 1 mL

Dried over 200

Dissolution ( 0.9 mol/L HNO3 18 mL )

Add NH2SO3H ( 12 drops )

Coulometric Measurement


- 24 -

Table 4 Analytical results of plutonium samples. No.1 sample contains about 10 mg of Pu in the cell. No.2 contains about 12.5 mg of Pu in the cell. No.3 contains about 15 mg of Pu in the cell.

Sample ID No. of runs per sample

Concentration ( mgPu/g )

RSD (%)

No.1 3 5.0188 0.07

No.2 5 5.0148 0.05

No.3 9 5.0180 0.02

5.00

5.01

5.02

5.03

5.04

5.05

2008/11/18 2008/12/8 2008/12/28 2009/1/17

Date

Conc

entr

atio

n [m

gPu/

g]

Certified Value (5.0192 mgPu/g)

;

Fig. 8 Day to day measurement variability of plutonium samples between 2008/11/18 2009/1/17.


- 25 -

No.8No.7No.6No.5No.4

No.3No.2No.1

15.55

15.56

15.57

15.58

15.59

15.60

15.61

15.62

15.63

15.64

15.65

Sample No.

Conc

entr

atio

n [m

gPu/

g]; Samples

; Average Value (15.5995 mgPu/g); error bar

Fig. 9 Analytical results of plutonium solution prepared from MOX powder.


- 26 -

Table 5 Uncertainty budget for Pu measurement by coulometry.

Quantity Value Standard

uncertainty

Uncertainty contribution

(%) p 1015.30 hPa 0.05 hPa < 1 T 25.4 0.1 < 1 h 53.0 % 0.5 % < 1 SS 8.000 g/cm3 0.015 g/cm3 < 1 sol 1.2442 g/cm3 0.0008 g/cm3 < 1

Wsol,No.1 12.1079 g 0.0001 g 2.4 WTare,No.1 11.1064 g 0.0001 g 2.4 Wsol,No.2 11.9162 g 0.0001 g 2.4 WTare,No.2 10.9190 g 0.0001 g 2.4 Wsol,No.3 12.0042 g 0.0001 g 2.4 WTare,No.3 11.0069 g 0.0001 g 2.4 Wsol,No.4 12.0134 g 0.0001 g 2.4 WTare,No.4 11.0157 g 0.0001 g 2.4 Wsol,No.5 12.0341 g 0.0001 g 2.4 WTare,No.5 11.0371 g 0.0001 g 2.4 Wsol,No.6 12.0502 g 0.0001 g 2.4 WTare,No.6 11.0540 g 0.0001 g 2.4 Wsol,No.7 12.0331 g 0.0001 g 2.4 WTare,No.7 11.0365 g 0.0001 g 2.4 Wsol,No.8 12.0510 g 0.0001 g 2.4 WTare,No.8 11.0532 g 0.0001 g 2.4

FeICP 0.0028 mg/g 0.0001 mg/g 2.3 MPu 239.1397 g/mol 0.0001 g/mol < 1 MFe 55.845 g/mol 0.002 g/mol < 1

Pu,No.1 15.64419 mg 0.00393 mg 7.3 Pu,No.2 15.57490 mg 0.00391 mg 7.3 mPu,No.3 15.57027 mg 0.00391 mg 7.3 mPu,No.4 15.58054 mg 0.00391 mg 7.3 mPu,No.5 15.57061 mg 0.00391 mg 7.3 mPu,No.6 15.55798 mg 0.00391 mg 7.3 mPu,No.7 15.56694 mg 0.00391 mg 7.3 mPu,No.8 15.58071 mg 0.00391 mg 7.3 CPu,AVE 15.59945 mg/g 0.00181 mg/g -----


- 27 -

Table 6. Definition of terms in Table 5. p The atmospheric pressure during mass measurement T Temperature during mass measurement h Humidity during mass measurement SS The density of the stainless steel reference weight in the analytical balance,

which are adjusted by the manufacturer to 8.0 g/cm3 sol The density of the plutonium solution

Wsol,No.1 The mass of the solution aliquot in coulometer cell for sample No.1 WTare,No.1 The mass of the coulometer cell for sample No.1 Wsol,No.2 The mass of the solution aliquot in coulometer cell for sample No.2

WTare,No.2 The mass of the coulometer cell for sample No.2 Wsol,No.3 The mass of the solution aliquot in coulometer cell for sample No.3






WTare,No.8 The mass of the coulometer cell for sample No.8 FeICP The contents of iron in the plutonium solution MPu The relative atomic mass of plutonium MFe The relative atomic mass of iron

Pu,No.1 The contents of plutonium in the sample No.1 measured by coulomery Pu,No.2 The contents of plutonium in the sample No.2 measured by coulomery mPu,No.3 The contents of plutonium in the sample No.3 measured by coulomery mPu,No.4 The contents of plutonium in the sample No.4 measured by coulomery mPu,No.5 The contents of plutonium in the sample No.5 measured by coulomery mPu,No.6 The contents of plutonium in the sample No.6 measured by coulomery mPu,No.7 The contents of plutonium in the sample No.7 measured by coulomery mPu,No.8 The contents of plutonium in the sample No.8 measured by coulomery CPu,AVE The average concentration of plutonium in the sample


- 28 -

Table 7 Propagation of plutonium content measurement uncertainty . Variables, X

Units

QS

count

QB

count

C

C/count

MPu

g/mol

F

C/mol

f none

Value 6313581 6500 0.99966 239.1397 96485.34 0.99889

Uncertainty

1 1400 1700 3.6010-5 0.00002 0.0024 0.00014

XPu 2.4810-6 -2.4810-6 1.56101 6.5410-2 -1.6210-4 -1.56101 22)( UXPu 1.2110-5 1.7810-5 3.1710-7 1.1810-12 1.5110-13 4.8110-6

Variance 34 % 51 % < 1 % < 1 % < 1 % 14 %

SSII

1024 10-1 d1021 10-2 c1018 10-3 m1015 10-6 1012 10-9 n109 10-12 p106 10-15 f103 10-18 a102 10-21 z101 da 10-24 y

SI

SI min 1 min=60s h 1h =60 min=3600 s d 1 d=24 h=86 400 s 1=(/180) rad 1=(1/60)=(/10800) rad 1=(1/60)=(/648000) rad

ha 1ha=1hm2=104m2

Ll 1L=11=1dm3=103cm3=10-3m3

t 1t=103 kg

SISI

SI eV 1eV=1.602 176 53(14)10-19J Da 1Da=1.660 538 86(28)10-27kg u 1u=1 Da ua 1ua=1.495 978 706 91(6)1011m

SISISI

SI Ci 1 Ci=3.71010Bq R 1 R = 2.5810-4C/kg rad 1 rad=1cGy=10-2Gy rem 1 rem=1 cSv=10-2Sv 1=1 nT=10-9T 1=1 fm=10-15m 1 = 200 mg = 210-4kg Torr 1 Torr = (101 325/760) Pa atm 1 atm = 101 325 Pa

1cal=4.1858J154.1868JIT4.184J

1 =1m=10-6m

10SI

cal

(a)SI(b)radsr(c)sr(d)(e)

(f)activity referred to a radionuclideradioactivity(g)PV,2002,70,205CIPM2CI-2002

cCGSSI

aamount concentrationsubstance concentrationb

SI

Pa s m-1 kg s-1

N m m2 kg s-2

N/m kg s-2 rad/s m m-1 s-1=s-1 rad/s2 m m-1 s-2=s-2 , W/m2 kg s-3

, J/K m2 kg s-2 K-1 J/(kg K) m2 s-2 K-1 J/kg m2 s-2 W/(m K) m kg s-3 K-1

J/m3 m-1 kg s-2

V/m m kg s-3 A-1 C/m3 m-3 sA C/m2 m-2 sA C/m2 m-2 sA F/m m-3 kg-1 s4 A2

H/m m kg s-2 A-2

J/mol m2 kg s-2 mol-1

, J/(mol K) m2 kg s-2 K-1 mol-1

C/kg kg-1 sA Gy/s m2 s-3 W/sr m4 m-2 kg s-3=m2 kg s-3

W/(m2 sr) m2 m-2 kg s-3=kg s-3 kat/m3 m-3 s-1 mol

SI

SI

m2 m3 m/s m/s2 m-1 kg/m3

kg/m2

m3/kg A/m2 A/m (a) mol/m3 kg/m3 cd/m2 (b) 1 (b) 1

SI

SI

SI

SI

() rad 1 m/m () sr(c) 1 m2/m2 Hz s-1 N m kg s-2 , Pa N/m2 m-1 kg s-2 , , J N m m2 kg s-2 W J/s m2 kg s-3 , C s A , V W/A m2 kg s-3 A-1 F C/V m-2 kg-1 s4 A2 V/A m2 kg s-3 A-2 S A/V m-2 kg-1 s3 A2 Wb Vs m2 kg s-2 A-1 T Wb/m2 kg s-2 A-1 H Wb/A m2 kg s-2 A-2 () K lm cd sr(c) cd lx lm/m2 m-2 cd Bq s-1, ,

Gy J/kg m2 s-2

, , ,

Sv J/kg m2 s-2

kat s-1 mol

SISI

SI bar bar=0.1MPa=100kPa=105Pa mmHg 1mmHg=133.322Pa =0.1nm=100pm=10-10m M=1852m b b=100fm2=(10-12cm)2=10-28m2

kn kn=(1852/3600)m/s Np

dB

SISI

SI

m kg s A K mol cd

SI

SI

SI erg 1 erg=10-7 J dyn 1 dyn=10-5N P 1 P=1 dyn s cm-2=0.1Pa s St 1 St =1cm2 s-1=10-4m2 s-1

sb 1 sb =1cd cm-2=104cd m-2

ph 1 ph=1cd sr cm-2 104lx Gal 1 Gal =1cm s-2=10-2ms-2

Mx 1 Mx = 1G cm2=10-8Wb G 1 G =1Mx cm-2 =10-4T Oe 1 Oe (103/4)A m-1

CGS

82006

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