+ All Categories
Home > Documents > RADIATION DOSIMETRY IN WR-1 REACTORRADIATION DOSIMETRY IN WR-1 REACTOR PART II. IONIZATION CHAMBERS...

RADIATION DOSIMETRY IN WR-1 REACTORRADIATION DOSIMETRY IN WR-1 REACTOR PART II. IONIZATION CHAMBERS...

Date post: 26-May-2020
Category:
Upload: others
View: 22 times
Download: 0 times
Share this document with a friend
41
Atomic Energy of Canada Limited RADIATION DOSIMETRY IN WR-1 REACTOR PART El. lONIZATION CHAMBERS by K.K. MEHTA and A.M. STADNYK Whiteshell Nucleor Research Establishment Pinawa, Manitoba January 1972 AECL-3796
Transcript

Atomic Energy of Canada Limited

RADIATION DOSIMETRY IN WR-1 REACTOR

PART El. lONIZATION CHAMBERS

by

K.K. MEHTA and A.M. STADNYK

Whiteshell Nucleor Research Establishment

Pinawa, Manitoba

January 1972

AECL-3796

ATOMIC ENERGY OF CANADA LIMITED

RADIATION DOSIMETRY IN WR-1 REACTOR

PART I I . IONIZATION CHAMBERS

by

K.K. Mehta and A.M. Stadnyk

Manuscript prepared August 1971

Whiteshell Nuclear Research Establishment

Pinawa, Manitoba

January, 1972

AECL-3796

RADIATION DOSIMETRY IN WR-1 REACTOR

PART II. IONIZATION CHAMBERS

by

K.K. Mehta and A.M. Stadnyk

ABSTRACT

An ionization chamber for measuring gamma-ray energy deposition

in nuclear reactors has been developed which is capable of continuous

operation at temperatures up to at least 500 C. It is sufficiently small

to be incorporated within in-core experiments with negligible flux

depression. It is rugged, simple in construction and reliable, and

accurate to within 5%.

Gamma-ray dose rates have been measured in the WR-1 reactor.

The values for the centre line of the fuel rod for carbon, magnesium, iron

and Zircaloy-2 are 109, 110, 104 and 114 mW.g'VkW.cm"1, respectively.

The effective value of the gamma-ray mass energy-transfer

coefficient for these materials is calculated for the reactor gamma-ray

spectrum and its relation to the gamma-ray dose rate discussed.

Atomic Energy of Canada Limited

Whiteshell Nuclear Research Establishment

Pinawa, Manitoba

January,1972

AECL-3796

Dosimétrie des radiations dans le réacteur WR-1

II Partie - Chambres d'ionisation

par

K.K. Mehta et A.M. Stadnyk

Résumé

Une chambre d'ionisation permettant de mesurer les

dépôts actifs des rayons gamma dans les réacteurs nucléaires

a été mise au point. Elle peut fonctionner continuellement à

des températures allant au moins jusqu'à 500°C. Elle est assez

petite pour accompagner des expériences faites en réacteur, sans

déprimer notablement le flux. Elle est solide, de construction

simple et sûre et sa précision est inférieure à 5%.

Des débits de dose de rayons gamma ont été mesurés

dans le réacteur WR-1. Les valeurs à la ligne centrale de la

barre de combustible pour le carbone, le magnésium, le fer et

le Zircaloy-2 sont respectivement 109, 110, 104 et 114 mW.g"1/kW.cm"1.

La valeur effective du coefficient de transfert masse-

énergie des rayons gamma correspondant à ces matériaux est

calculée pour le spectre des rayons gamma du réacteur et son

rapport avec le débit de dose des rayons gamma fait l'objet d'un

commentaire.

L'Energie Atomique du Canada, Limitée

Etablissement de Recherches Nucléaires de Whiteshell

Pinawa, Manitoba

AECL-3796

CONTENTS

1. INTRODUCTION 1

2. IONIZATION CHAMBER 2

3. IRRADIATION AND MEASURING EQUIPMENT 6

4. EXPERIMENTAL PROCEDURE 7

5. RESULTS 9

6. DISCUSSION 11

7. CONCLUSION 1 k

8. REFERENCES 15

APPENDIX I Fabrication of the Ionization Chamber 17

APPENDIX II Fricke Dosimetry for the Reference Gamma-RayField 20

APPENDIX III Estimation of Correction to Measured DoseRates 24

FIGURES

Page

1. Dependence of Gamma-Ray Mass Energy-TransferCoefficient and Fast-Neutron Dose Rate on AtomicNumber 26

2. Whiteshtll High Temperature Ionization Chamber, LineDrawing 27

3. Whiteshell High Temperature Ionization Chamber, X-RayPhotograph 28

4. Whiteshell High Temperature Ionization Chamber, Dis-assembled 29

5. Cross Section of the Hollow Hanger Fuel Assembly,

Mark III 30

6. Cross Section of WR-1 Fuel Bundle 31

7. Electrical Circuit for Measuring Ionization Current 32

8. Saturation Curve 33

9. Axial Variation of Ionization Chamber Response alotvgFuel Channel 34

TABLES

Sensitivity of Various lonization Chambers 7

Corrections and Corrected Dose Rates for Carbon,Magnesium, Iron and Zircaloy-2 in WR-1 Reactor 10

Proportionality of Dose Rate to Effective MassEnergy-Transfer Coefficient 12

Comparison of Experimental and Calculated Fast-Neutron Dose Rates 14

1. INTRODUCTION

This is Part II of a three-part series on "Radiation Dosimetry

in WR-1 Reactor". Part I 1 consists of calorimetric measurements in the

WR-1 reactor, while Part III 2 deals with thermal and fast neutron flux

densities at various irradiation positions in WR-1. This report describes

the ionization chamber and measurements taken in WR-1.

There are many types of radiation present in a reactor, e.g.

neutrons, gamma rays, fission products, and charged particles such as

protons and alpha particles. Of these, gamma rays and fast neutrons are

the most important for dosimetry since they are the main contributors to

the absorbed energy. The dose rates due to these two sources should be

known separately because the dependence of chemical or physical effects on

the energy deposition is different for each of them; the ionization densities

for protons (knocked out by fast neutrons) and electrons (generated by

gamma rays) differ markedly.

Calorimeters have been used to measure the total energy

deposited in a material 1 . Ionization chambers measure mainly the gamma-

ray dose rates; then, as the total dose rates from calorimetry are known,

the fast-neutron dose rates can be calculated. Like the calorimeters, the

ionization chambers are operable at 500 C and are smaller than h inch in

diameter. The high temperature requirement is essential for power reactor

dosimetry and for experiments located inside a materials testing reactor.

Small chambers can be accommodated much more easily in in-core experiments

and the small size avoids perturbing the radiation field.

Several chambers were made with walls of different materials

to study the variation of the gamma-ray and the fast-neutron dose rates with

atomic number. Fig. 1 shows the dependence of the gamma-ray mass energy-

transfer coefficient (which is proportional to the gamma-ray dose rate) on

the atomic number for two gamma-ray energies^3 . The computer-calculated

fast-neutron dose rate for a reactor spectrum is also shown in the same

figure for several materials . Four materials, viz., carbon, magnesium

(in alloy form), iron and zirconium in the form Zircaloy-2, were chosen to

study these effects. They are common reactor materials (except, perhaps,

magnesium) because of their low neutron absorption cross sections.

2. IONIZATION CHAMBER

2.1 DESIGN PRINCIPLES

The ionizing capability of nuclear radiation has long been

used to measure the exposure or the dose rate. The first suggestion for

this came from Bragg 5 , and a mathematical treatment was given by Gray 6'7 .

The Bragg-Gray principle, as it is commonly known, states that the amount

of ionization produced in a gas cavity is a measure of the energy dissipated

in the surrounding material. In an ionization chamber, the secondary

electrons generated in the chamber wall by the primary gamma rays cause

ionization in the gas cavity such that

E = WJ sm m rn

where E = energy absorbed by unit mass of wall

W = average energy dissipated in the gas per ion pair

formed

J = ionization in unit mass of gas

s^ = ratio of the mass stopping powers of the wall and

the gas.

This is the Bragg-Gray relation.

The Bragg-Gray principle is based on the following assumptions^

(i) the electron spectrum established in the medium

( i . e . , the chamber wall) is not modified by the

presence of the gas cavity;

(ii) photon interactions generating electrons in the

cavity are negligible.

These conditions are fulfilled if the cavity size is sufficiently small

compared with the range in the gas of the radiation traversing it. The

electron spectrum will remain undisturbed if the atomic composition of the

gas is the same as that of the chamber wall, and in this case the size

limitation can be relaxed. The rigorous proof of this theorem is due to

Fano 9 . Also, since the mass stopping power ratio depends upon the

gamma-ray energy, it is desirable to have a matched ionization chamber,

i.e. s = 1.m

In designing the Whiteshell ionization chambers, some degree of

compromise was necessary between the above principles and practical

considerations of size and the ambient temperature in the reactor*.

2.2 CHAMBER WALL

Since we wanted to measure the dose rate in various materials,

a series of similar ionization chambers with different wall materials,

viz., carbon, magnesium, iron and Zircaloy-2, were made. The carbon wall

was of pyrolytic graphite with isotropic planes to make it impervious to

argon gas**. For use as an absolute dosimeter, the gas should match the

wall in each case. Since this was not practical each chamber was

calibrated in a known gamma-ray field. The chosen wall thickness of

2.5 mm was sufficient for the practical fulfillment of the Bragg-Gray

requirements. It generated an equilibrium spectrum of secondary

electrons and shielded the cavity from practically all externally

generated electrons. Since the wail scatters gamma rays disturbing the

* See Figs. 2, 3, 4** Fabricated by H.R. Lee of Fuel Development Branch, WNRE.

gamma-ray field, it was kept as thin as possible. The inside surface of

the wall was machined smooth and kept clean. The wall was 5.1 cm long,

which defined the ion-collecting region. A 0.15 mm thick stainless steel

sheath formed the outer container for all the chambers.

2,3 GAS CAViTY

If a and b are the outer and the inner radii of the gas

cavity, i t is desirable to have a small a/b ratio to minimize the voltage

needed for efficient collection of the ions. Also there is a danger of

ionization by collision near the central conductor where the field strength

is maximum. For the Whiteshell ionization chamber the ratio a/b was 2.36.

The cavity was 1.06 cm3.

Argon was used as the cavity gas because of i ts chemical

stability, absence of unwanted nuclear reactions and a small response to

fast neutrons.

2.k CENTRAL CONDUCTOR

The central conductor was a stainless s teel tubing of 2.42 mm

OD and 1.27 mm ID. The tubing rather than a solid rod was used to minimize

generation of gamma rays and beta rays inside the chamber.

2.5 INSULATOR

The insulator which separates the two electrodes must be

stable at high temperatures and during irradiation. The insulator used

within the Whiteshell chamber was Lava*, which is mainly aluminum silicate

and is available commercially. It was easy to machine before the heat

* Supplied by American Lava Corporation, Chattanooga, Tenn.

treatment and became very hard after the treatment. Its electrical

resistivity was 2 x 109 ohm.cm at 300°C and 5 x 106 ohm.cm at 500°C.

It was stable under radiation for at least two weeks (longest duration

of our experiment). Once it was treated at high temperature, it was

stable against dimensional changes at high temperatures.

2.6 SIGNAL CABLE

The coaxial cable used for transporting the ionization current

from the chamber must be resistant to radiation and high temperatures.

Because of the length required to reach the reactor core (> 5 m) some

flexibility was desired. The insulator must have a very high resistivity

at the working temperature and radiation intensity. We used a coaxial

cable 12 m long and 1.6 mm in diameter. The outer sheath and central

conductor (dia. = 0.25 mm) were made of stainless steel while the insulator

was MgO. The resistance across the MgO when the cable was connected to

the chamber was greater than 10 ohm at room temperature.

Since MgO is hygroscopic, exposing it to atmosphere would

result in deterioration of the insulation resistance (owing to the absorbed

moisture). The cable, therefore, was always stored with the ends sealed

with epoxy glue. During the fabrication of the ionization chamber, the

time interval during which MgO came in contact with the atmosphere was

kept to a minimum. The chamber end of the coaxial cable was sealed using

a high-temperature seal, while at the other end epoxy glue was used. When,

inadvertently, moisture entered the insulation, heating the cable was

sufficient to drive the moisture out. The condition of the insulation was

judged by the value of its electrical resistance. If necessary, in extreme

cases several inches of cable may be discarded.

A major difficulty encountered when developing our high

temperature chambers was the leakage of the cavity gas into the cable

insulation. This loss of gas would cause a decrease in the sensitivity of

the chamber. To prevent this, the chamber end of the cable had to be

sealed against any gas leakage. This seal at the same time should be a

good electrical insulator. Since we were unable to obtain such a seal

commercially, we developed a seal which has operated successfully for at

least 10 days at 5OJ°C in the reactor*.

Details of the fabrication of the Whiteshell ionization

chamber are given in Appendix I.

3. IRRADIATION AND MEASURING EQUIPMENT

The WR-1 reactor and the irradiation equipment are discussed

in more detail in Ref. (1). All the ionization chamber measurements were

made in the hollow hanger fuel assembly, which is a standard WR-1 18-element

fuel rod with a % inch hole in the centre (see Fig. 5). Figure 6 shows the

cross section of the fuel region. The temperature of the ionization

chamber during the measurements reached 500 C maximum when the coolant

temperature was at 400 C. A special irradiation flask 10 was used to

introduce the ionization chamber into the hollow hanger rod. The vertical

position of the chamber was known within 0.25 in. from the revolution

counter on the flask.

To measure the ionization current generated in the chamber

cavity, the electrical circuit shown in Figure 7 was used. All the

connections (except the one going to the chamber) were low noise polythene-

insulated coaxial cables. A 300 volt dry battery with a voltage dividing

circuit in a shielded metal box was used to apply the electrical field

to the chamber. The voltage was varied smoothly between 0 V and 300 V

and was measured by a differential voltmeter. A digital volt meter, DVM,

measured the ionization current. The entire circuit was floating electri-

cally except for a possible grounding of the ionization chamber wall in

the reactor. The uncertainty associated with the current measurement was

The details of the seal are the subject of patent investigation.

less than one per cent.

h. EXPERIMENTAL PROCEDURE

4.1 CALIBRATION

Before using an ionization chamber to measure the dose rate

in a reactor, its sensitivity should be measured in a known gamma-ray

field. The gamma-ray energies in the calibrating field and the reactor

should be similar (this point is amplified in Section 6). We used a

Gammacell 220 Co60 source for calibrating our chamber. The gradient of

the field at the centre of the irradiation chamber was negligible. The

gamma-ray field was measured using Fricke dosimetry (see Appendix II).

The sensitivity for various ionization chambers is listed in Table I.

Since the gamma-ray energy spectra in the calibrating field and in the

reactor were comparable (i.e. the effective gamma-ray mass energy-transfer

coefficients were similar), no correction was needed for the wall

absorption in the reactor measurements.

TABLE I

SENSITIVITY OF VARIOUS IONIZATION CHAMBERS

Wall Material

Carbon

Magnesium

Iron

Zirconium

Sensitivity (Coulombs per Rad)*

0.629 x 10~9

0.604 x 10"9

0.713 x 10"9

0.708 x 10~9

* The pressure in the cavity was about 1 atmosphere and not necessarilyequal in all the chambers. The difference in sensitivities, therefore,is partly due to different amounts of cavity gas.

h.2 REACTOR MEASUREMENT

The ionization chamber, with potential applied, was lowered from

the irradiation flask to a desired position (usually the mid-point of the

third bundle), in the hollow hanger rod. Once the current was steady

(which took about 15 minutes) a current saturation curve was obtained by

varying the applied potential between 0 and 250 volts (see Fig. 8).

Generally, the chamber was then left at the position for several hours to

check that the response was steady. A decreasing signal would indicate

loss of gas either to the atmosphere or into the insulation of the cable.

After ensuring that the chamber was leak-tight, it was moved to various other

positions in the rod to measure the dose rates there, and also to locate

the fuel gaps between the bundles 1 . Some measurements were made at lower

reactor power.

*4.3 SATURATION CURRENT

Since the ionization in the cavity gas is proportional to the

dose rate in the wall material, the saturation current (current when

collection efficiency is unity) must be measured accurately. In the

absence of any extraneous source of current, the measured current would

reach an equilibrium value (saturation current) as the applied voltage is

increased. It can be seen from Fig. 8 that an equilibrium value was

reached at about 150 V. However, the current increased linearly as the

electric field was further increased. From this linear behaviour it was

concluded that the increase was due to leakage current (I = — ) , sinceR

the insulation has some finite resistance, R. The value of R was

determined from the slope of the linear portion of the measured saturation

curve and a corrected saturation curve was plotted Csee Fig. 8).

NORMALIZATION

To compare measurements at various positions along the channel,

at various reactor powers, and for different ionization chambers, the

results were normalized using the fission power generated in the fuel

surrounding the chamber. The linear power density at the location of the

chamber was calculated from the measured channel power assuming a sine

distribution for power along the channel. This was an accurate description

of the general shape as can be seen from Fig. 9 in which the ionization

chamber response along the channel is reproduced (see also Ref. 1). The

results were also corrected for changes in power generation in the

neighbouring fuel elements due to changes of the core loadings.

5. RESULTS

The ionization currents measured by the various chambers at

the mid-point of the third fuel bundle in the hollow hanger rod in WR-1

are listed in the second column of Table II. The values of power generated

in the fuel around the chamber are listed in the third column. Various

corrections which are applied to this measured current and to the

corresponding computed dose rates are also given. The following were the

four factors causing extraneous current:

(i) Leakage Current in the Insulation: Since the insulation

had finite resistance, the presence of the electric field generated an

ohmic current. This leakage current was enhanced by high temperature and

by radiation. The magnitude of this current was estimated from the slope

of the saturation curve in the plateau region assuming that the plateau

would have negligible slope in the absence of the ohmic current. The

maximum correction was for the magnesium chamber (about 14% of the

measured current). The effective resistance of insulation in this case

was about 30 x 106 ohms. The difference in the values of the leakage

current for the various chambers (see Table II) was probably due to the

difference in the quality of the cable or the insulating seal.

(ii) Fast Electron Current: The reactor gamma rays generated

fast secondary electrons in the two electrodes. These electrons did not

10

depend on the electric field for their transportation but rather on the

energy they received from the gamma rays. Because of the difference in

material and in the physical shape of the two electrodes, a net electron

current was present between the two electrodes. This current was measured

by removing the applied field, i.e. V = 0^ The maximum correction was

for the magnesium-walled chamber and amounted to about 5% of the measured

current.

(iii) Capture Gamma Rays; Thermal neutrons were absorbed by

the material of the chamber giving capture gamma rays, which caused

ionization current via the secondary electrons. These additional gamma

rays were negligible in all cases except the iron-walled ionization chamber,

where they contributed about 6% of the measured dose rate. The details of

the calculations are given in Appendix III.

(iv) Fast-Neutron Energy Transfer: Fast neutrons transferred

part of their energy to argon atoms in the cavity through scattering

collisions. As calculated by the computer code NEVEMOR , about

5 mW.g 1/kW.cm energy was received by argon from fast neutrons

(0.1 MeV < E < 10 MeV). Appendix III shows that this energy corresponded

to 0.18 \iA ionization current per kW.cm 1 energy produced in the surrounding

fuel. This current amounted to about 2% of the measured current.

Since materials with high neutron absorption cross section

were avoided, no correction was necessary for ionization current due to

beta rays.

Using the sensitivity of the chamber as measured in the

Gammacell (see Table I), dose rates were computed from the saturation

currents. These dose rates are listed in column 8 of Table II and are

in mW.g VkW.cm 1. Corrections were also necessary to account for the

different power generation in the neighbouring rods for the various

measurements. These are listed in column 9. The last column then lists

the corrected normalized dose rates for different wall materials.

11

TABLE II

CORRECTIONS AND CORRECTED DOSE RATES FOR CARBON.

MAGNESIUM, IRON AND ZIRCALOY-2 IN WR-1 REACTOR

WallMaterial

Carbon

Magnesium

Iron

Zircaloy-2

MeasuredSaturationCurrent

41.3

37.0

48.9

50.4

LocalPower

Density(kW.cn"')

4.90

4.88

5.72

5.80

Leakage(a'Current

-5.3

-5.3

-2.7

-2.3

FastCa)

ElectronCurrent

-1.4

+1.9

-0.4

+1.2

Correction'3 '

NeutronCollisions

-0.9

-0.9

-1.0

-1.0

Corrected'"'Saturation

Current

33.7

32.7

44.8

48.3

IonizationDose Rate

109.3

110.9

109.8

117.6

Neighbouring"1'Channels

Correction

-0.5

-0.6

0

-3.3

Cn.,)<b>1,1 Uall

0

0

-6.1

0

Gamma-Ray*10

Dose Ratein Material

108.8

110.3

103.7

114.3

(a) All values are in uA and correspond to the local power density at the time of rhe measurement ( i . e . un-normalized).

(b) All values are in nH.g'VkW.cp"1 •

6. DISCUSSION

The dose rates measured by the ionization chambers are listed

in Table II. The ionization chambers were insensitive to fast neutrons;

hence the entire measured dose rate was due to gamma rays except for the

small (2%) contribution due to ionization by recoil argon atoms.

Calorimeters on the other hand measured the total dose rate including the

entire recoil energy from fast neutron collisions in the sample material.

The four materials, viz., carbon, magnesium, iron and zirconium,

were chosen to study the dependence of gamma-ray dose rate in different

materials on the gamma-ray spectrum. Now the gamma-ray dose rate

\ = / y(E)<KE)EdE

where u(E) is the mass energy-transfer coefficient. An effective coefficient

can be defined for a composite gamma-ray spectrum, as

f U(E)(j)(E)EdE

/ c|>(E">EdEJeff

For materials of low to medium atomic number, u(E) varies slowly with

energy in the range 0.4 to 5 MeV. For gamma-ray fields having energy

predominantly in this range, vi(E) is relatively insensitive to the spectral

distribution. Reactor gamma-ray spectra and many isotopic gamma-ray

12

sources such as Co60 are in this category. On this basis it is possible

to compare different materials or make approximate predictions about

materials or gamma-ray fields for which measurements are not available.

This is the basis for using a Co60 source to measure the sensitivity of

the chambers for reactor measurements. To test the validity of such a

procedure we compare the ionization chamber results with calculated values

for yeff.

Effective values of the mass energy-transfer coefficient, Peff>

were computed in Part I of this series , where it was assumed that the

gamma-ray field incident on the dosimeter was the appropriate mixture of

the prompt fission gamma rays, the fission product gamma rays and the

uranium capture gamma rays. These are listed in column 2 of Table III.

These values agree with values calculated by Unruh and Tomlinson ll for

various measured reactor and other gamma-ray source spectra within a few

percent for Z < 26 (i.e. up to iron). Table III shows that the ratio of the

dose rate to p „ was constant within ± 3%. The constancy of this ratioef r

supports the validity of the y ff values and confirms the accuracy of the

ionization chamber measurements.

TABLE III

PROPORTIONALITY OF DOSE RATE TO EFFECTIVEMASS ENERGY-TRANSFER COEFFICIENT

Material

Carbon

Magnesium

Iron

Zircaloy-2

(cm

0.

0.

0.

0.

eff2g 1)

0261

0259

0253

0262

Dose Rate(mW.g 1/kW.cm

108.8

110.3

103.7

114.3

Dose Rate Q-3

*»eff

4.17

4.26

4.10

4.36

The accuracy of the measured dose rate values was dependent

on the accuracy of the current measurements and the accuracy with which the

13

calibrating gamma-ray field was known. The latter depended on the errors

involved in Fricke dosimetry and was about 2% (see Appendix II). The DVM

used for current measurement was accurate to 1%. The reactor power was

known within 5% and the precision was much better, of the order of 1%.

Thus the accuracy of the dose rates reported as mW.g~1/kW.cm"l was about

6 to 7%, while the precision was about 3 to 4%. The precision and the

accuracy were about the same as for the calorimetry measurements * .

The main purpose of the dosimetry program was to measure the

gamma-ray and the fast-neutron dose rates separately. The calorimeters *

gave the total dose rate and the ionization chambers gave the gamma-ray

dose rate. The difference represented the fast neutron contribution. Table

IV lists all the dose rates including those calculated for fast neutrons by

the NEVEMOR code ^ . The mass numbers of ~ron and zirconium are suffi-

ciently high for the fast-neutron dose rate to be negligible. This was

borne out by the experimental results which also agreed with NEVEMOR

calculations. For magnesium and carbon the fast-neutron dose rates

measured by difference were 10 and 16 mW.g l lower than the computed values,

respectively. The discrepancy is within experimental error for magnesium

but may be significant for carbon. No satisfactory explanation is available

at present.

Calorimetry measurements with samples for which the fast-

neutron dose rate contribution is higher than that of carbon may help to

resolve this discrepancy. Measurements using beryllium and terphenyl

samples in calorimeters are to be attempted.

14

TABLE IV

COMPARISON OF EXPERIMENTAL AMDCALCULATED FAST-NEUTRON DOSE RATES

Material

Carbon

Magnesium

Iron

Zirconium

Gamma-Ray ̂Dose Rate

108.8

110.3

103.7

114.3

Total D o s e ^Rate

131.5

110.1

103.5

115.8

(c)Fast-Neutron

Dose Rate(Experimental)

22.7

- 0.2

- 0.2

1.5

(d)Fast-Neutron

Dose Rate(Calculated)

39.0

10.0

2.1

1.3

Note: All dose rates are in mW.g VkW.cm 1

(a) From ionization chamber measurements, this report.

(b) From calorimeter measurements(l)

(c) Difference between the calorimeter and the

ionization chamber measurements.

(d) Computed by the code NEVEMOR^.

7. CONCLUSION

An ionization chamber has been developed which is capable of

continuous operation at temperatures up to at least 500°C. It is

sufficiently small to be incorporated within in-core experiments with

negligible flux depression. It is rugged, simple in construction and

reliable. It is accurate within 5%.

Gamma-ray dose rates in the dosimetry hole of the Mark III

hollow hanger rod in WR-1 have been measured using these chambers. The

gamma-ray dose rates for carbon, magnesium, iron and Zircaloy-2 at the

15

centre line of the fuel rod are 109, 110, 104 and 114 raW.g VkW.cm 1

fission power, respectively. Dose rates at other locations and in similar

reactor systems can be estimated with the aid of supplementary calculations

or experimental data.

These values compare favourably with the total dose rate

values measured by calorimeters l} for the medium atomic number materials,

viz. iron and Zircaloy-2, in which the fast neutron dose rate is negligible.

For magnesium, the experimental value of the fast-neutron dose rate

(difference between the total and the gamma-ray dose rates) is lower than

that calculated using a computer code, but the discrepancy is within the

experimental error. However, the discrepancy for carbon may be significant.

It is shown that the calculated value of the gamma-ray mass

energy-transfer coefficient for carbon, magnesium and iron for the reactor

gamma-ray spectrum is proportional to the measured gamma-ray dose rate.

8. REFERENCES

1. Mehta, K.K., and Stadnyk, A.M., Radiation Dosimetry in WR-1Reactor. Part I. Calorimetry, AECL-3795, October, 1971.

2. Mehta, K.K.. and Stadnyk, A.M., Radiation Dosimetry in WR-1Reactor. Part III. Neutron Fluence Measurements,AECL-3797,in press.

3. Storm, E. and Israel, H.I., Photon Cross Sections from 0.001to 100 MeV for Elements 1 through 100, LA-3753, Los AlamosScientific Laboratory, 1967.

4. Mehta, K.K.. and Kry, P.R., Calculations of Flux Spectra andEnergy Deposition for Fast Neutrons, AECL-3423, 1969.

5. Bragg, W.H., The Consequences of the Corpuscular Hypothesisof the y and X-Rays and the Range of 3 Rays, Phil. Mag.,20 (1910) 385.

6. Gray, L.H., The Absorption of Penetrating Radiation, Proc.Roy. Soc. (London), A122 (1929) 647.

7. Gray, L.H., An Ionization Method for the Absolute Measurementof y-Ray Energy, Proc. Roy. Soc , A156 (1936) 578.

16

8. Attix, F.H. and Roesch, W.C., Radiation Dosimetry, Vol. I,Academic Press, 1968.

9. Fano, U., Note on the Bragg-Gmy Cavity Principle for MeasuringEnergy Dissipation, Radiation Res., 1 (1954) 237.

10. Mehta, K.K.-and Payne, W.E., Manual for Experimental IrradiationFlask Assembly No. 1, Unpublished report WNRE-44, AECL, 1970.

11. Unruh, W.G., and Tomlinson, M., Mean Gamma Ray Energy AbsorptionCoefficients* Nucl. Appl., J3 (1967) 548.

12. Attix, F.H. and Roesch, W.C., Radiation Dosimetry, Vol. II,Academic Press, 1966.

13. Weiss, J. et al., Use of the Friake Ferrous Sulfate Dosimeterfor Gamma-Ray Doses in the Range 4 to 40 kr, Proc. 1st Int.Conf. PUAE, 14 (1956) 179.

14. International Commission on Radiological Units and Measurements,Rep. 10b: Physical Aspects of Irradiation, Handbook 85,National Bureau of Standards (USA), 1964.

15. Schreiber, R.E.. and Allio, R.J., Gamma Keating in ReactorExperiments, Nucleonics, _22_ (August 1964) 120.

16. Henderson, W.J. and Whittier, A.C., Handbook of Shielding andHeat Production Calculations for the NRU Reactor, AECL-403, 1955.

17. Burlin, T.E.,and Chan, F.K., The Effect of the Wall on theFricke Dosimeter, Int. J. Appl. Radiat. Isotopes, 20 (1969) 767.

18. Stone, J.A., Radiolysis of Cyolohexane in a Xenon Matrix at77 K, Can. J. Chem., 46 (1968) 1267.

19. Primak, W., Gamma-Ray Dosage in Inhomogeneous Nuclear Reactors,J. Appl. Phys., T]_ (1956) 54.

20. Bartholomew, G.A. and Higgs, L.A., Compilation of ThermalNeutron Capture Gamma Rays, AECL-669, July, 1958.

21. Evans, R.D., The Atomic Nucleus, McGraw-Hill Book Company Inc.,1955.

22. Boyd, A.W. (Ed), Ths Determination of Absorbed Dose in Reactors,International Atomic Energy Agency, technical report seriesNo.127, June,1971.

17

APPENDIX I

FABRICATION OF THE I ON IZATI ON CHAMBER

The steps in the fabrication and calibration of the ionization

chamber are as follows:

1. The machine shop made all the component parts according

to our design.

2. All the components were cleaned in an acetone bath

for about 20 minutes in an ultrasonic cleanser and then

dried at 150°G for 30 minutes.

3. All components were weighed.

4. The high-temperature insulating seal was formed at

the chamber-end of the coaxial cable. A standard male

BNC connector was installed at the other end of the cable.

5. The high-temperature insulating seal was tested for

leaks and insulation properties as well .as integrity

at 500°C.

6. If the seal was leak-proof and showed a room tempera-

ture electrical resistance of more than 1012 ohms,

the chamber was assembled but no joints were brazed.

7. A radiograph of the chamber was made to check that the

components fitted properly.

8. If the radiograph was satisfactory, all the joints

were silver-brazed leaving the end fill-tube still

open.

18

9. The chamber was checked for leaks using a helium

leak-detector.

10. If satisfactory, the chamber was vacuum degassed at

500°C overnight.

11. The chamber was flushed with pure argon gas several

times. It was finally filled with pure argon at

about one atmosphere pressure at room temperature and

the fill-tube silver-brazed.

To check further for any possible leak, the following test was performed:

12. The ionization chamber was placed at the centre of

the irradiation chamber of the Gammacell 220 and a

saturation current curve obtained by varying the

applied voltage between 0 and 250 volts.

13. The chamber was heated outside the Gammacell at 500 C

for about 2 hours and slowly cooled to room temperature

so as not to damage the seal.

14. The chamber was once again placed in the Gammacell

and the saturation current curve obtained. If no

change was observed in the saturation current, the

chamber was ready for calibration and a reactor

experiment.

Calibration (also see Appendix II):

15. Besides measuring the saturation current when the

chamber was located in the Gammacell (step 14),

currents were also measured at 0 volts applied inside

the Gammacell to estimate the fast electron current

correction and at 150 volts outside the gamma-ray

19

field to estimate the leakage current correction.

The ratio between the corrected saturation current

and the gamma-ray field in the irradiation chamber

was the sensitivity of the ionization chamber.

20

APPENDIX I I

FRICKE DOSIMETRY FOR THE REFERENCE GAMMA-RAY FIELD

To measure the sensitivity of an ionization chamber, its

response was measured in the reference gamma-ray field?viz^the irradiation

chamber of a Gammacell 220. The gamma-ray field in the chamber was due

to cobalt pencils situated in a ring around the chamber, which was 8 in.

long and 6 in. in diameter. The field in the centre of the chamber was

nearly uniform. Fricke dosimetry 1 2 was used to measure this gamma-ray

field.

PROCEDURE

The Fricke solution was made according to the formulae

recommended by Weiss, Allen and Schwarz . The irradiation cells were

made from Corning Pyrex #7740 (density = 2.23 g.cm 3) . Pyrex is about

80% silica, the wall material recommended by ICRU^14 . Two cells of

different wall thickness (0.622 cm and 0.282 cm) were used having the

same inside diameter of 0.955 cm, which was nearly equal to the outside

diameter of the ionization chamber wall (1.08 cm). The solution was

irradiated in the centre of the irradiation chamber for time intervals

ranging from 5 seconds to 100 seconds. The amount of the ferric ions

produced was measured by measuring the optical density of the solution for

light of wavelength 3040 X using a spectrophotometer. The dose rate to

Fricke solution was calculated from the slope of the straight line obtained

by plotting the optical density vs time of irradiation.

PRECAUTIONS

Since any error in measuring the reference gamma-ray field

would directly propagate to the dose rate value in the reactor, the

following precautions were taken to minimize any error in the measurements.

21

1. All chemicals were from fresh stock.

2. The temperature of the solution affects the yield

(G value) of the reaction as well as the extinction

coefficient, hence the temperature should be controlled.

The freshly prepared Fricke solution was stored in

the spectrophotometer laboratory for several hours

prior to use so that it was at room temperature, which

was measured with a thermometer. The cell carriage

of the spectrophotometer was stored outside the

spectrophotometer between runs to maintain it at room

temperature to minimize heating of the solution during

measurements. The measurement time in the spectrophoto-

meter was kept to a minimum. The irradiation cells were

handled by their support stem to minimize heating the

solution.

3. To measure the average dose rate at the point of

location in the Gammacell, the irradiated solution

was thoroughly mixed before measuring its optical

density. This was achieved by pouring the solution

between the spectrophotometer quartz cell and the

irradiation cell three times.

4. The design of the irradiation cell was such that its

positioning in the centre of the irradiation chamber

was reproducible.

5. An electronic counter was used to measure the time

of irradiation to one hundredth of a second. The

'start' and 'stop' signals for the counter came from

a specially placed microswitch at the bottom of the

Gammacell.

22

RESULTS

The uncorrected dose rate to Fricke solution was 255 R.sec

and 256 R.sec l for the two cells. The molar extinction coefficient, z ,

which was measured for the i

radiolytic yield, G = 15.6.

which was measured for the spectrophotometer, was 2154 at 22 C. The

Two corrections were applied to these dose rates: first,

the attenuation due to the wall of the cell and second, the self attenuation

of the solution. The wall attenuation A = 2 \it, where y(cm l) = linearw

energy-transfer coefficient of Pyrex for the gamma rays and t (cm) = wall

thickness 1 5 . The self attenuation of the solution A = -? uR, whereS J

y(cm -1) = linear energy-transfer coefficient of Fricke solution for the

gamma rays and R(cm) = inside radius of the cell 16 . Now, the gamma rays

in the irradiation chamber were not only the primary ones emitted by Co°"

(E = 1.17 and 1.33 MeV) but there was a large abundance of the backscattered

gamma rays (E "^0.2 MeV). On the average it was assumed that \i for

Pyrex was 0.0602 cm ^ and for Fricke solution was 0.031 cm *• Using

these values the wall attenuation was 7.5% and 3.4% for the two cells.

The self attenuation for the solution was 1.9%. The correction necessary

to account for the difference in electron stopping power of the Fricke

solution and the Pyrex wall was about %% -1 . Thus the corrected dose rate

to Fricke solution was 279 R.sec"1 and 270 R.sec"1 for the two cells.

Therefore, the corrected dose rate to Fricke solution in the

centre of the irradiation chamber of the Gammacell 220 was 275 R.sec"1 ± 2%

on April 1, 1971.

SENSITIVITY OF I0NIZATI0N CHAMBERS

In measuring the sensitivity of the ionization chamber,

however, the ionization current should be correlated to the dose rate in

the wall material and not in Fricke solution. These two dose rates are

in ratio of their gamma-ray mass energy-transfer coefficient, y, (cm2g~1).

This ratio is calculated in the following manner:

23

y (wall)U (Fricke)

y (wall)y (carbon)

y (carbon)y (Fricke)

The energy absorption in a Gammacell 220 for various materials relative to

that of carbon has been reported by Stone. 18\ A similar ratio of carbon

to Fricke solution was calculated from Ref. (8). From these ratios, the

dose rate to various materials in the Gammacell was calculated and is listed

in Table A.I along with the sensitivities for the corresponding ionization

chambers.

TABLE A.I

WallMaterial

Carbon

Magnesium

Iron

Zirconium

Fricke solution

y (wall)u (carbon)

1.00 (a)

1.00 (a)

1.09 (a)

1.16 (a)

1.11 (b)

y (wall)y (Fricke)

0.90

0.90

0.98

1.05

1.00

(c)Dose Rateto Wall

Material(R.sec"1)

247.5

247.5

269.5

288.8

275.0

IonizationChamber

Sensitivity(Coulombs peri\.3.Q /

0.629 x 10"9

0.604 x 10~9

0.713 x 10~9

0.708 x 10~9

-

(a) These values were obtained by interpolation of data in Ref. (18).(b) From Ref. (8).(c) These values are for April 1, 1971.

24

APPENDIX III

ESTIMATION OF CORRECTION TO MEASURED DOSE RATES

CONTRIBUTION OF CAPTURE GAMMA RAYS IN THE IRON WALL

Thermal neutron capture gamma rays produced in the iron wall

of the chamber contributed to the gamma-ray dose rate. The source

strength, s, of these gamma rays was given by:

s = No* ,_E = 1.72 x 106 x | , eV.cm~3sec~1th y th

where N = number of iron atoms per unit volume = 8.45 x 10 2 2 cm 3

o = thermal neutron absorption cross section for iron

= 2.62 x 10~2l+ cm2

<j> . = average thermal neutron flux density within the

iron wall

E = binding energy of the last neutron averaged over

all the iron isotopes = 7.78 MeV.

The thermal neutron flux in the wall was obtained from the activity of the

cobalt wire monitors located on the outer surface of the chamber. After

applying a small correction (about 6%) for the attenuation of the thermal

neutron flux in the wall, d> = 2.86 x 1012n.cm~2sec~1 per kW.cm"1 fission power

The average gamma-ray flux density, $ , present within the wall due to

these sources was estimated from the two cases (T16 and T17) considered by

Primak(l9):

<f> ^ 1.5 sT where T = thickness of wall = 0.254 cm

^ 1.87 x 1018 eV.cm~2sec"1

The effective mass energy-transfer coefficient for iron for the capture

gamma-ray spectrum was computed as:

25

V(E).(KE).E

where the gamma-ray spectrum, <f>(E) , was obtained from Ref. (20). The value

of u g f f = 0.0203 cm2g 1. The energy absorbed by iron then was given by

<f>Y x u e f f = 3.8 x 1016 eV.sec^g"1 per kW.cm"1

= 6.1 mW.g 1 per kW.cm l fission power.

IONIZATION CURRENT DUE TO THE FAST-NEUTRON DOSE RATE IN ARGON

Fast neutrons transfer energy to the struck atoms through

collisions. Thus, in the reactor the argon atoms in the gas cavity

received energy from the fast neutrons. According to the NEVEMOR code ^ ,

the energy transferred to argon was 5 mW.g * per kW.cm 1 fission power.

The struck argon atom received on the average about 50 keV energy during a(„,)

collision with a 1-MeV neutron Z1 . The range of such an argon atom was(,,)

much smaller than the size of the cavity *•*• and hence it lost all its

energy in the cavity in ionization and excitation of the gas atoms.

The mass of the argon gas in the cavity for the Whiteshell Chamber

was about 18 x 10 ^ g and hence received 5.6 x 1013 eV.sec ] from fast

neutrons per kW.cm 1 power generation in the surrounding fuel. The energy,

W, expended to create one electron-ion pair in argon gas by a 50 keV argon

ion is between 30 and 100 eV^22 . Assuming W = 50 eV, the ionization

current caused by these argon ions was 0.18 yA per kW.cm 1, i.e. about 2%

of the total current.

26

100

10

CM

O

5

1.0

0.0

i 1 1 1 1 1 r

O FAST-NEUTRON DOSE RATE IN REACTOR -

Ey = I MeV

O

C Mg Fa Zr Pb U

0.0011 1 1 l l I J I i i10 20 30 40 50 60 70 80 90 100

ATOMIC NUMBER

000

39m

00

mTO

3

1.0

01

Figure 1: Dependence of Gamma-Ray Mass Energy-Transfer Coefficient andFast-Neutron Dose Rate on Atomic Number

27

STAINLESS STEEL

MONITOR WIRE TUBES

COAXIAL CABLE SEAL

CENTRAL CONDUCTOR

ARGON CAVITY

STAINLESS STEEL SHEATH

ARGON

STAINLESS STEEL

Figure 2: Whiteshell High Temperature Ionization Chamber, Line Drawing

LAVA

MONITOR WIRE TUBES

COAXIAL CABLE SEAL

COAXIAL CABLE

CENTRAL CONDUCTOR

ARGON CAVITY

WALL'

K500

Figure 3: Whiteshell High Temperature Ionization Chamber, X-Ray Photograph

FILL-TUBE STAINLESS STEEL SHEATH

LAVA

CENTRAL CONDUCTORCOAXIAL CABLE

COAXIAL CABLE SEAL

N9

Figure 4: Whiteshell High Temperature Ionization Chamber, Disassembled

30

ELEV. 871'-6"

MARK HI FUELHANGERFILLER PIECE

1/2 " I. D.DOSIMETERHOLE

ELEV. 852'-4fHOT (REF)

8 4 " TO TOPOF DECK PLATE

•j I.D. DOSIMETERHOLE

ELEV. 852 ' -4 - j - '(REF)

Figure 5: Cross Section of the Hollow Hanger Fuel Assembly, Mark III

31

4" in. DOSIMETRYHOLE

MODERATOR(D 2 O)

CALANDRIA TUBE(aluminum)

NOTE '• All dimensions in an . Radiiare measured from bundlecentre except where otherwiseindicated.

Figure 6: Cross Section of WR-1 Fuel Bundle

32

COAXIAL CABLE

DIFFERENTIAL VOLTMETER

V

ISHIELDED

POWER SUPPLY

IONIZATIONCHAMBER

COAXIAL CABLE

Figure 7: Electrical Circuit for Measuring Ionization Current

33

60-SATURATIONCURRENT

REACTOR

REACTOR

GAMMACELLCURRENT

0.2

CURRENT (MEASURED)

CURRENT ( CORRECTED FORLEAKAGE CURRENT)

O.I o

O<

Z

<

10

50 100 150

APPLIED VOLTAGE

200 250

Figure 8: Saturation Curve

co

UJ

UJtooo

IO

co

QC

oS

COMPUTER FITTED SINECURVE

UJ

u.

u.

o

oom

1st FUEL I [2nd FUEL BUNDLE! |3rd FUEL BUNDLE! I4th FUEL BUNDLE)|5th FUEL BUNCX.E1

<L OF FUEL

I l I

220 230 240 250 260 270 280 290 300

DISTANCE FROM DECK PLATE (inches)

310 320

Figure 9: Axial Variation of Ionization Chamber Response along Fuel Channel

Additional copies of this documentmay be obtained from

Scientific Document Distribution OfficeAtoirk Energy of Canada Limited

Chalk River, Ontario, Canada

Price - $1 00 per copy


Recommended