(
MIT-334-33
Reactor Technology
Standard TID 4500
IN-PILE LOOP IRRADIATION STUDIES
OF
ORGANIC COOLANT MATERIALS
PROGRESS REPORT
JANUARY 1,
1965 - SEPTEMBER 30,
D. T. Morgan, Project Supervisor
Report prepared by:
Contributors:
1965
Project Engineer
W. N. Bley,
T. H. Timmins, Research Assistant
DEPARTMENT OF NUCLEAR ENGINEERING
MASSACHUSETTS INSTITUTE OF TECHNOLOGY
CAMBRIDGE, MASSACHUSETTS 02139
(M.I.T. Project No. DSR 9819)
Work Performed Under Contract No.
with the
AT(38-1)-334
Savannah River Operations Office
U. S. ATOMIC ENERGY COMMISSION
Issued:
November 1, 1965
(MITNE-66)
ii
LEGAL NOTICE
This report was prepared as an account of Government
sponsored work. Neither the United States, nor the Commission, nor any person acting on behalf of the Commission:
A. Makes any warranty or representation, express or
implied, with respect to the accuracy, completeness, or
usefulness of the information contained in this report, or
that the use of any information, apparatus, method, or
process disclosed in this report may not infringe privately
owned rights; or
B. Assumes any liabilities with respect to the use of,
or for damages resulting from the use of information, apparatus, method, or process disclosed in this report.
As used in the above, "person acting on behalf of the
Commission" includes any employee or contractor of the Commission to the extent that such employee or contractor prepares, handles or distributes, or provides access to any
information, pursuant to his employment or contract with
the Commission.
.............
iii
DISTRIBUTION
This report is being distributed under the category
"Reactor Technology", TID 4500. Additional copies may be
obtained from USAEC Division of Technical Information
Extension (DTIE), P.O. Box 62, Oak Ridge, Tennessee.
Previous related reports on this project:
MITNE-4
(IDO 11,101)
MITNE- 7
(IDO 11,102)
MITNE-9
MITNE- 12
(IDO 11,103)
MITNE-21
MITNE- 22
(IDO 11,104)
MITNE-29
(IDO 11,106)
(IDQ 11,107)
MITNE-39
MITNE- 41
MITNE- 48
MITNE-55
MITNE-59
MITNE-63
(IDO 11,105)
(SRi-85)
(SRO-87)
(MIT-334-11)
(MIT-334-12)
(MIT-334-23)
iv
T ABLE
OF CONTENTS
Page
1.0
2.0
Summary
Loop Operations and Experimental Radiolysis
Results for This Period
3.0
4.0
Summary of Previous Irradiation Results
In-Pile Dosimetry
5.0
6.0
Heat Transfer and Friction Factor Results
Summary of Property Measurements for Run 14
7.0
Travel and Reports Issued
References
1
4
11
17
23
29
34
35
V
LIST OF TABLES
Page
1.1
2.1
3.1
3.2
4.1
4.2
6.1
6.2
Summary of Operating Conditions and Results
for Runs 13 and 14 Based on Pre-Irradiation
Dosimetry Measurements
Results of Steady-State Run 14 Based on
Pre-Irradiation Dosimetry Measurements
Summary of Results for Steady-State Loop
Irradiations
Summary of Results for Transient Loop
Irradiations
Summary of Results from Calorimeter
Measurements
Summary of Fast Neutron Dose Rates from
Foil Activation Measurements
Average Molecular Weight of Run 14 High Boiler
Summary of Average Molecular Weight for SteadyState Loop Irradiations Through Run 14
2
9
12
13
18
20
29
vi
LIST OF FIGURES
Page
2.1
2.2
3.1
3.2
4.1
4.2
5.1
5.2
5.3
5.4
6.1
6.2
6.3
Cross Section of Reactor Core Showing Fuel
and Control Rod Positions
Total Terphenyl Concentration as Function of
Absorbed Dose for Run 13
Effect of Tcmperature on Irradiation of
Terphenyl Coolants in M.I.T. Loop Irradiations
Pyrolysis of Terphenyl Coolants
Calculated Fast Neutron Dose Rate in Santowax WR
Using Foil Activation Data, Fuel Position 20
Neutron Energy Spectrum Used for Fast Neutron
Dose Rate Calculations from Foil Activation
Data
All M.I.T. Irradiated Organic Coolant Heat
Transfer Data
Friction Factor and Heat Transfer Factor for
Irradiated Santowax WR, Upstream Half of
Test Heater 7
Friction Factor Data for TH7,Selected Santowax
WR Data and Water Data
Colburn Analogy for M.I.T. Irradiated Santowax
OMP, Heat Transfer Data
Density Measurements for Run 14
Viscosity Measurements for Run 14
Average Molecular Weight of High Boiler as
Function of High Boiler Concentration
5
7
15
16
21
22
24
25
27
28
30
31
33
CIIAPTER 1
SUIMIMARY
Irradiation of Santowax WR in the MITR in a new fuel
position with a fast neutron fraction of 0.05-0.06 was initiated on May 10, 1965 as Transient Run 13. This run was
continued until July 19, 1965 when the terphenyl concentration had decreased from 92% to a level of 84% as desired for
Run 14. Steady-State Run 14 was started on July 19 and continued to September 27, 1965 with distillation processing
and recycle of the coolant. The operating conditions and the
preliminary G*(-omp) values from these runs are summarized
in Table 1.1. At the end of Run 14, a tritium dilution for
the circulating organic mass was carried out.
A reevaluation of previous loop data was carried out
and G values calculated for individual terphenyl isomers as
well as the total terphenyl and high boiler. These results
are summarized in this report and will be described in detail
in a topical report on the Santowax WR irradiat.i&Is which will
be issued late in 1965 (to be assigned the number MIT-334-34).
The new G values are slightly different in some cases than
those reported in MIT-334-12 (Q1).
Heat transfer and friction factor measurements using a
new test heater were performed. All previous data as well
as the new data were compared with the Dittus-Boelter and
Colburn relations. The heat transfer data agreed with either
correlation within +10%; the friction factor data agreed
with the Colburn relation within +10%. A report describing
these results in detail was issued in September, 1965 (1.2).
Additional heat transfer measurements were made at the end
of Run 14 but the results are not yet available.
Calorimeter and foil activation measurements were carried
out in the new experimental facility to establish the dose
rate. The preliminary values (see folnote of Table 1.1)
for the total dose rate and fast neutron fraction are (one
Table 1.1
Summary of Operation Conditions and Results for Runs }3 and 14
Based on Pre-Irradiation Dosimetry Measurements k)
Irradiation Temperature
Loop Pressure
572'F
Fast Neutron Fractionl
Average Dose Rate in Total Coolant Mass(l)
0.056
0.0068 watts/gm
G*(-omp)
Run 13 (First Order Kinetics)
Run 14
0.196 molecules/100 ev
P-100 psig
0.192 molecules/100 ev
Terphenyl Condentration
92->84%
84.0->83.5%
Run 13 (Transient Run)
Run 14 (Steady-State Run)
(1)These values are based on pre-irradiation calorimeter and foil
activation measurements in Fuel Position 20. Post-irradiation
calorimeter measurements are planned in the spring of 1966 at
the completion of the irradiations in Fuel Position 20. Slight
changes (<5%) in these values may occur when the additional
measurements are available and included in the data evaluation.
Eli
IIIIIIIIJIMM
IIIII
Jill'
III
3
standard deviation uncertainty limits):
3
FT = 20.4 + o.4 watt-cm
2
f
-
lM-gm
= 0.056 + 0.007
Construction of a new in-pile section (In-Pile Section
No. 4) was started during this period. This new in-pile section is identical to the one now being used (In-Pile Section
No. 3) and is being constructed in the MITR machine shop.
Visits were made to the AECL Chalk River Laboratories for
technical discussions on organic coolants and to Atomics
International for discussion of the future experimental program of the M.I.T. Organic Coolant Project. An experimental
program covering the next two years was agreed on by AI and
M.I.T. and approved by the AEC.
CHAPTER 2
Loop Operations and Experimental Radiolysis
Results .or This Period
All previous irradiations in the M.I.T. In-Pile Loop
were carried out in the central fuel position of the reactor
where the fast neutron fraction was 37-40%. As discussed
in the previous progress report (1.1), it appeared desirable
to perform irradiations at a significantly lower fast neutron
fraction in the same irradiation facility and with the same
loop equipment to provide a direct measurement of the fast
neutron effect or Gn/G . Furthermore, the use of steadystate runs would provide more accurate total G values than
is possible in transient irradiations thus providing a significantly more accurate determination of Gn/G than has
previously been possible.
To accomplish this purpose, plans were made to perform
several steady-state runs in Fuel Position 20 (see Figure 2.1)
near the outside edge of the core where the fast neutron fraction should be significantly less than in the central fuel
position (Fuel Position 1). To minimize the fast neutron
fraction in Fuel Position 20, it was desirable to (1) eliminate the use of any fuel in this fuel position thereby eliminating the production of fast neutrons near the in-pile capsule and (2) to include a cadmium converter to convert thermal
neutrons to gamma rays by the (n,7) reaction thereby increasing the gamma ray dose.
Consequently, a new irradiation facility and in-pile
section were designed and procured. The irradiation facility
consists of an aluminum sample assembly containing no uranium
but with an integral cadmium sleeve as a replacement for the
8 or 10-plate fuel element used in prev'ious irradiations.
The in-pile section fits inside this sample assembly and is
surrounded by the cadmium sleeve. The new in-pile section
(In-Pile Section No. 3), while similar to In-Pile Sections
5
1211 BEAM PORT
SHIM
SAFETY
RODS
FINE
CONTROL
ROD
FIG. 2.1 CROSS SECTION OF REACTOR CORE
AND CONTROL ROD POSITIONS
SHOWING
FUEL
...........
I-
No. 1 and 2, has been modified to increase the in-pile volume
from approximately 205 cm3 to 285 cm' and to provide more
reliable heaters and thermocouples. A central monitor tube
which extends from the top of the reactor shield down into
the center of the in-pile section has also been added so that
foils and other measuring devices having a diameter less than
0.3 inches can be inserted during an irradiation into a region
surrounded by the circulating coolant in the core. The monitor tube outside the thimble as used in all other in-pile
sections is also included.
The new sample assembly with integral cadmium sleeve was
inserted into Fuel Position 20 on February 28, 1965 with a
stainless steel thimble inserted in place of the in-pile
section. Calorimeter and foil activation experiments were
carried out in this thimble during the period March - May,
1965 (see Section 4.0). These measurements indicated a fast
neutron fraction of about 5-6%. The new in-pile section was
inserted in place of the stainless steel thimble on May 1,
1965. The loop was charged with Santowax WR and Transient
Run No. 13 started on May 10, 1965. The purpose of Run 13
was to degrade the coolant from its initial terphenyl concentration of '92% down to -84% as desired for steady-state
Run 14. The operating conditions for this run were 5720F
and 14100 psig. A concentration of 84% terphenyl was reached
and steady-state Run 14 started on July 19, 1965 at a temperature of 572 F and "100 psig. Run 14 was continued until
September 27, 1965 when sufficient terphenyl had been degraded
to provide a one standard deviation uncertainty in the total
terphenyl G value of about +5% and Run 14 was ended.
The results of Run 13 are presented in Figure 2.2 in
terms of total terphenyl concentration as a function of absorbed dose. The reaction rate constant for the total terphenyl disappearance was calculated based on first, second,
and third-order kinetics. The calculated values based on the
pre-irradiation dosimetry measurements (see footnote of
Table 1.1) and their one standard deviation uncertainty limits
are:
1.00
I
I
I
I
0.95[0
0.90
H
0.851
z
w
0-
0.80K
-J
AVG. EXPERIMENTAL VALUE OF AT LEAST
4 CHROMATOGRAPHY RUNS
w 0.750.70
FIG. 2.2
I
1.0
I
I
I
2.0
3.0
4.0
TOTAL ABSORBED DOSE, r, WATT HOURS/GM
TOTAL TERPHENYL CONCENTRATION
AS FUNCTION
5.0
6.0
OF ABSORBED DOSE FOR RUN 13
8
kR(First Order) = G*(-omp)
G*(-omp)
kR(Second Order)
= (1.69 + 0.20) x 10-2
w
-hr
= 0.196 + 0.023 molecules degraded.
ev rd
G*~op)_100
= 1.93 + 0.19 x 10-2 wa-shr
G*(CAvg = 0.878) = 11.65 kRCAvg = 0.198 Molecules
100 ev
g s
kR(Third Order) = (2,.20 + 0.22) x 102 watt-hr
G*(CAvg
=
0.878)
=
11.65 kAvg
=
0.198 molecules
The operating conditions were:
T = 572 0 F, P E 100 psig, fN = 0.056, Avg Dose Rate = 0.0068 watts
gm
The kinetics for the individual isomers will be reported
at a later date. It should be noted that the above results
are directly dependent on the loop mass. A tritium dilution
was carried out at the end of Run 14 for another loop mass
determination but the results are not yet available; the
numbers quoted above may therefore change slightly when the
results of the mass determination are available. Any change
should be less than 5% however since the mass used in these
calculations is based on previous tritium dilutions.
The results of steady-state Run 14 are presented in
Table 2.1 including operating conditions and G values for the
terphenyl isomers. It will be noted that-the concentration
change over the run is small so that the run is, in fact;- a
steady-state run. The statistical uncertainty is also excellent, the percentage uncertainty (one statistical deviation) being +5% for the total terphenyl G value. For this
run, to obtain good statistical accuracy, 140 separate analyses were made on the samples and returns used in the run.
Three additional steady-state runs are planned for
Fuel Position 20 (fN = 0.056). At the end of these runs, the
irradiation capsule will be moved back to Fuel Position 1 and
Table 2.1
Results of Steady-State Run 14 Based on Pre-Irradiation Dosimetry Measurements(l)
Irradiation Temperature = 572 0F
Type of Distillation - Quaterphenyls Not Recycled
Density = 0.897 gms/cm 3
Total Terphenyl Degraded = 534 grams
Total Loop Circulating Mass = 5230 grams
Fast Neutron Fraction = 0.056
Total Average Dose Rate = 0.0068 watts/gm
Total
Initial Loop Concentration, wt %
Final Loop Concentration, wt %
m-
15.4
63.6
5.0
84.0
10.9
14.6
63.9
5.0
11.2
0.136
+0.004
0.034
G(-), molecules/00 ev
-*(-1i) = G(-i)/C
HB
pmp
o-0
0.222
+.007
(')See footnote of Table 1.1.
Error limits are one standard deviation.
0.1115
0.010
83.5
0.161
+0004
+0.001
+0.008
0.20
+0.02
0.192
+0.009
0.181
+0.007
D
10
irradiations will be continued at the higher fast neutron
fraction of about 40%. Construction on In-Pile Section No. 4
was initiated during this reporting period for use in this
change as well as a back-up in case of failure of the present
in-pile section (No. 3) before the irradiations in Fuel
Position 20 are completed. In-Pile Section No. 4 will be
identical to In-Pile Section No. 3,
11
CHAPTER 3
SUrV4ARY OF PREVIOUS IRRADIATION RESULTS
During this period, the results of previous loop irradiations of Santowax WR in Position 1 of the MITR were reevaluated and the G values calculated for the disappearance
of the individual terphenyl isomers as well as for the total
terphenyl disappearance and HB generation. The new values are
slightly different in some cases than those reported in
MIT-334-12 (1.1). The G value for any pure component, G(-i)
or G(i), is defined as the molecules of that component destroyed or produced per 100 ev of energy absorbed from fast
neutron and gamma interactions in the total coolant. The G
value for
molecules
of energy
11 it was
high boiler production, G(4-HB), is defined as the
of terphenyl degraded to high boiler per 100 ev
absorbed in the total coolant. In Runs 8, 10, and
found that the statistical uncertainty was larger
than desired due to the relatively large scatter of the concentration data resulting from poor reproducibility of the
chromatographic column used for these analyses. The samples
from these runs were therefore reanalyzed and more precise
results were obtained.
The complete results are summarized in Table 3.1 for
the steady-state runs and in Table 3.2 for the transient
runs. For the steady-state runs, both G(i) and G*(i) values
are reported for each of the terphenyl isomers and the total
terphenyl; only the G(i) values are reported for high boiler
generation.
The G*(i) values are defined as:
G*(i) = 2i).
(3.1)
is the concentration of component i in the coolant.
For the transient runs, only G*(i) values are reported based
on use of first-order kinetics for the degradation. The G*
values sorvenas a useful normalization factor for comparison
where C
of the low and high temperature runs made at a given terphenyl
Table 3.1
Summary of Results for Steady-State LOOP Irradiations**
Mterial
Santowax
Temperature in
Irradiation Zone
0
0F
C
300
0.163 321
610
0.115
0.0102
0.136
+0.004
+0.0011
+0.004
22.0
56.6
4.8
9.6
0.34
(30.8)
(14.4)
+0.02
0.200
+0.009
(30.3)
(16.2)
750
399
53.5
Santowax
OMP
0.034
+0.001
83.3
750
750
399
399
60.5
69.5
T.5
44.6
2.5
43.4
3.3
7.1
0.155
+0.003
0.23
+0.003
0.020
+0.004
+0.01
+0.003
0.003
0.287
+0.009
0.029
+0.002
0.154
+0.008
0.015
+0.002
+0.008
0.0963
+0.0006
0.087
0.192
+0.009
0.264
+0.008
0.222
0.181
0.20
0.056
+0.009
0.26
+0.01
+0.007
0.256
+0.008
+0.02
0.41
0.40
0.40
0.015
0.37
+0.04
0 40
+0.02
0.36
+0.02
+0.02
+0.02
0.34
+0.02
0.39
+0.03
G*(-m)
0.28
+0.01
0.43
+0.08
0.60
+0.09
Run IDate of
Wno
Run
14
7/19/65
lC
11
+0:04
0.40
+0.04
5
9/27/65
5/24/62
8/30/62
8/25/64
9/25/64
1/20/64
3/10/64
10/2/63
0.26
0.014
0.245
o.63
1.00
0.59
0.42
0.40
+0.01
+0.04
0.46
+.04
0.37
3B
11/27/63
2/26/63
+0.005
+0.04
0.79
+0.04
+0.03
0.53
+0.002
0.085
+0.009
0.282
+0.006
+0.03
0.53
+0.01
0.31
+0.02
0.41
+0.001
0.085
+0.003
0.54
+0.02
0.45
+0.02
0.35
+0.04
0.40
2
6
4/18/63
3/12/64
4/12/64
4/20/64
5/8/64
6.1
35.3
18.6
49.5
4.0
(15.2)
(15.3)
(14.8) +0.03
+0.005
0.106
+0.009
0.186
0.22
+0.01
0.27
750
399
73.7
18.2
51.1
4.4
(11.5)
Santowax
WR
780
416
61.6
8.2
50.2
3.1
24.9
13.5
0.53
+0.03
0.090
+0.006
0.41
+0.03
Santowax
Satoax
800
427
80.03
51.5
11.3
36.9
3.0
(26.9)
(21.6)
-0.91
0.1
+
0.269
029
+0.009
o.61
069.3
+0.02
Santowax
80
(
1.06
+o.o4
0.35
+0.01
+0.03
.
G*(~o)
o.067
Santowax
4
0.173
O*(~omP)
+0.003
o.048
15.7
W
00
.0157
Fast
Neutron
Fraction
fm
G*(P)
+0.01
0.32
034
.6.7
32.4
G(~HB)
o.161
61.9
54.8
I
+0.008
06
+0.005
11.0
371
Q(-n)
5.
5.8
5.0
18.3
700
Santowax
Santowax
321
G(-m~
fl(-omn~
63.8
37.6
32.3
tl(-o'I
T.Th
15.0
6.0
83.7
G*(i) = G( i)/Ci
G(i), molecules/100 ev
572
7
Santowax
OMP
Santowax
WR
Santowax
Average Loop Concentrations, wtlt
HB*
p
(Bottoms)
m
o
omp
0.02
0.64
0.30
+0.01
0.33
+0.02
0.45
+0.03
o.56
+0.03
+0.03
+0.06
0.04
0.58
0.05
0.53
+0.04
0.34
0.15
0.034
+0.013
0.032
0.47
+0.04
o.86
+0.06
1.10
+0.07
0.81
+o.06
+0.001
+0.03
0.77
.7
1. 76
1.6
+0.06
-2.2336
+0.08
i~.5
+0.06
0.014
+0.002
0.015
0.006
0.074
+0.013
0.01
0.70
+0.03
1.62
+0.06
2.18
+0.08
1.42
+0.06
1.1
+0.4
1.0677(
F+0.04
7
1.9
+0.3
+0.04
0.40
0.04
o.4o
+0.04
12/4/63
12/23/63
6/18/64
7/20/64
0.40
.086
+0.04
0.40
+0.04
*HB refers to distillation where the quaterphenyl were not recycled.
Bottoms refers to distillation where about 75% of the quaterphenyls were carried over with the terphenyls and LIB and therefore recharged to the loop.
**Error limits are one standard deviation except for fast neutron fraction which is approximately two standard deviations.
10
7/21/64
8/25/64
Table 3.2
Summarm of Results for Transient Loop Irradiations*
Temperature in
Irradiation Zone
Material
Santowax
WR
Santowax
WR
Santowax
OMP
Santowax
0F
0C
425
218
572
300
6lo
321
G*(i) molecules/100 ev
Concentration Range, wt%
omp
69-858
91.8-83.8
66.6-+-39.6
0
m
p
-
-
~
41.2-+w25.1
18-.+10 4
321
100.1+- 59.6
10.7-+6.3
64.8-+37.4
24.6-v16.2
OMP
OH?
Santowax
Santowax
750
399
65. -41.
69-,>,3.1
38.54-+4.
20.6-+v13.8
750
399
90.4--063.0
10.4-+-a6.3
53.0+-37.0
27.0o+19.7
WR
750
399
78-+45
Santowax
WR
78o
416
68+v55
m
p
0.26
-
No.
N
+0.04
0.056
-
0.25
0.25
+0. 04
0.30
+0.05
+0.04
0.34
+0.09
+0.13
0.46
+0.07
+0.25
0.63
+0.27
0.58
+0.05
0.97~~
+0.10
Run iDate of
Run
N
0.40
~
+0.08
+0.02
610
Santowax
0
0.19
--6.7-+--4.1
1omp
Fast
Neutron
Fraction
02
033
o.2W
02
+0.015
13
0.37
1B
+0.21
+0.04
0.45
+0.07
+.41
+0.04
+0.101
3A
8
5/12/64
6/12/64
37 2B
0.7 2
2A
0.40
+0.04
+0.46J
+0.04-
18/9/61
10/5/61
10/5/61
1/3/62
1/14/63
2/15/63
12/4/62
1/10/63,
7/25/63
9/26/63
+0.0
+0.09
1/1/64
1/18/64
5/lo/65
7/19/65
*Error limits are one standard deviation except for fast neutror fraction which is approximately two standard deviations.
(A
14
concentration regardless of whether first or second-order
radiolysis and pyrolysis occurs.
In Figure 3.1, the G*(-omp) values are plotted for those
runs with similar total terphenyl concentrations. A large
increase in the G*(-omp) value with temperature above an
irradiation temperature of about 7000F is apparent. Our
present interpretation of this result is based on assuming
separability of the radiolysis and pyrolysis. The radiolysis
rate is extrapolated from low temperature measurements where
pyrolysis is negligible to higher temperatures using a constant activation energy of 1 kilocalorie/mole. This extrapolated rate is then subtracted from the total degradation
rate to give the pyrolysis rate. In Figure 3.2, the pyrolysis rate constant calculated in this fashion (assuming
first-order kinetics for pyrolysis) is given using the M.I.T.
data presented in Table 3.1; data from Euratom are also presented for comparison. It is apparent that the data from
M.I.T. and Euratom provide a consistent picture when analyzed
in this fashion supporting the proposed model for the total
degradation rate including both radiolysis and pyrolysis.
Additional data are required however before any definitive
conclusion can be stated and data from the M.I.T. loop as
well as other sources will be interpreted in terms of this
model as the data become available.
No detailed analysis of the data has been presented here
since a topical report on the Santowax WR irradiations through
Run 11 is in preparation and will be issued at a later date
(to be assigned the number MIT-33-3 11).
15
ERROR
250
LIMITS ARE 2o
300
400
350
*C
I
I
A SANTOWAX WR,25-31% BOTTOMS
1.8 |--
0
0 SANTOWAX
A
WR, 10-17% BOTTOMS
SANTOWAX OMP,
33% BOTTOMS
0
(f)
1.6 I-
(D
z
w z
w
0
0
C)
0
0
1.4|--
1.2
z
0
0-
0
a.
0
O
0
0
1.0 F--
z
0.8 |(f) 0L
w
-i
0.6 |-
-i
0
0'
0
0.4 F-
0.2 E-
0.01
40 0
I
I
500
600
IRRADIATION
FIGURE 3.1
700
800 *F
TEMPERATURE
EFFECT OF TEMPERATURE ON IRRADIATION OF
TERPHENYL COOLANTS IN M.I.T. LOOP IRRADIATIONS
.....................
u
16
5
7
S0
I UNIRRADIATED TERPHENYL OM- 2
II MIT IRRADIATED SANTOWAX WR
(27-31% BOTTOMS, 0.020 w/g)
III EURATOM IRRADIATED OM - 2
O MIT - 17 % BOTTOMS
AMIT - 27 -31 % BOTTOMS
O MIT - 12 -15% BOTTOMS
MIT - 25 % BOTTOMS
* EURATOM - BLO 2 (0.040 w/g)
0 EURATOM - BLO3 (0.015 w/g)
* EURATOM - UNIRRADIATED OM -2
2
z
z
ERROR LIMITS ARE 2 oI
0
u
w
51
cf)
*
0
21
a::
0W
it
10
-4
H-
n- u
5
0 0
0
o
L0ON
0
I
cxq
0 0
00
I
0uto
0 0
I
LoO0
2
1.40
FIGURE 3.2
1.45
EFFECTIVE
PYROLYSIS
1.50
TEMPERATURE
OF TERPHENYL
1.55
1.60
I/T,*K~ x 103
COOLAN T S
0
0
00
o0L
n-.
1+
CHAPTER 4
IN-PILE DOSIMETRY
During this period, several calorimetric dose rate
measurements were made in the M.I.T. Reactor to determine the
pre-irradiation dose rate and fast neutron fraction in Fuel
Position 20. These runs and the measured dose rates for
each individual run are summarized in Table 4.1. These
measurements will be repeated at the conclusion of irradiations in Position 20 so that an estimate of any dose rate
variation during the irradiation period can be made.
The fast neutron fraction in Fuel Position 20 is difficult to determine with any precision due to the small neutron dose rate relative to the gamma dose rate in this position and the fact that the fast neutron dose rate is basically
determined as the difference between the total and gamma dose
rates. This difficulty is particularly obvious at the edge
of the core and in the reflector region where the uncertainty in the measured fast neutron dose rate is as large as
the quantity itself. To alleviate this difficulty and to
obtain the best possible fast neutron dose rate integrated
over the in-pile capsule volume, the results of the calorimeter
measurenc's have been combined with the foil activation
results. The fast neutron dose rate from calorimeter measurements at positions where the experimental uncertainty is
a minimum was used as a normalization basis. The normalized
fast neutron dose rate calculated from foil activation results was then used to extend the fast neutron dose rate to
positions where the calorimetric measurements of the fast
neutron dose rate are less accurate.
Using this procedure, the final estimate for the gamma
and fast neutron dose rates integrated over the in-pile
volume are (one standard deviation uncertainty):
F
=
2'M
19.30 + 0.25 watt-cm
-g
Table 4.1
Summary of Results from Calorimeter Measurements
Calorimeter
Series No.
Core
Position
Dates of
Measurement
I
-----
Fuel Loading
23
in 23
3/3-4/65
20
I--.-.----------.
XIII
3/16-18/65
No
Cd
No
SS
20
+1.8
SW
27.4
19.0
1-
4 ----------
9
XIV
4/6-9/65
20
Same as XII
XV
4/28-29/65
20
xv'
5/25-26/65
1
1
0.094
0.055
22.8
All
t
0.053
+0.039
18.0
SW
3
0.20
+o.6
+1.2
Al
Less PS
SW
I
+0.06
29.0
Al
Less PS,
Fuel in 20
Lined Sample Assembly
Fuel in 21
Thimble
Same as XII
0.26
30.5
Less PE,
4
fN
I
+2.0
Fuel in 21 and 24
SS Thimble
XII
watt-cm 3
MW-gm
All***
No Fuel in 23
Cd Lined Sample Assembly
Fast
Neutron
Fraction
Mr.
~------~
1/19-20/65
XI
Absorbers
Used in
Data
Analysis
20.9
21.9
I
I
o.o68
All
21.0
Same as XII except
Aluminum Thimble
*
*
*
10 Plate New Fuel
Element
Aluminum Thimble
**
**
**
*This series was not made at all axial positions in the core and thus cannot be used to
directly evaluate FT and fn- This series did include the axial positions -6 inches,
0 inches, and +6 inches relative to the core midplane and is used with the results from
Series XII, XIII, and XIV in determining a best estimate of the fast neutron dose rate
at these three positions.
**This series was made to evaluate the possible effect of thermocouple size on the measurements in the low thermal conductivity absorbers using a new method of inserting
thermocouples in the absorbers. Unfortunately, poor thermal contact between the thermocouple and absorber invalidated the measurements and no conclusions could be made.
This experiment will be repeated at a later date using more carefully constructed calorimeters.
***Beryllium, aluminum, carbon, polyethylene, polystyrene, and Santowax OMP absorbers.
19
F
= 1.15 + 0.20
MWt-cm
FT = 20.45 + 0.36
wt- cm
fN = 0.056 + 0.007
These values have been used in evaluating the G values for
Runs 13 and 14 as presented in Section 2.0.
Three foil activation measurements were completed during
this period. The calculated values of FN and fN using these
data are summarized in Table 4.2. In Figure 4.1, the axial
variation of the calculated neutron dose rate in Santowax WR
is presented for Series 29, 30 side, and 30 center. The neutron energy spectrum used for these calculations is illustrated in Figure 4.2 with the positions of the detector
energies denoted. The spectrum is based on assumption of a
l/E spectrum from the Co5 9 resonance (120
Mev, a shape of O(E) = pEq from 0.711 Mev
a measured fast spectrum above 2.81 Mev.
culated from the foil activation data are
ev) to 0.711
to 2.81 Mev, and
The FN values cal-
en-the eder-of'
sligitly less than values obtained from the calorimeter measurements. This discrepancy is believed due to the lack of detectors between the Co 59 resonance of 120 ev and the lowest
threshold detector of 2.9 Mev now used, where a large percentage of the deposited energy by fast neutrons is derived.
The neutron spectrum in this energy region must therefore be
faired for the calculation of FN with a resulting large
uncertainty. Additional resonance and threshold detectors
are now being developed for use in this region so that the
spectrum may be better defined.
Table 4.2
Summary of Past Neutron Dose Rates from Foil Activation Measurements
Calculated
Fuel Position
Numbarv
Date of
watt-cm
3
Foil Activation
Series No.
Measureftent
29
March 1965
20
No fuel in 20
Cd Lined Sample
Assembly
No fuel in 21
SS Thimble
1.15
0.053
June 1965
20
No ful1 in 20
1.12
0.052
1.06
0.o48
30 side
In-Pile Section
No fuel in 21
30 Side in Side
Monitor Tube
30 Center in Center
Monitor Tube
30 center
31 side
31 center
September 29,
Fuel Loading
1965
20
Same as 30 Side and
30 Center
data not
yet analyzed
0
0.005
0.004
S0.003
0.002
0.001
-II
-6
0
AXIAL DISTANCE
6
11
15
FROM CORE CENTER, INCHES
20
25
FIG. 4.1 CALCULATED FAST NEUTRON DOSE RATE IN SANTOWAX WR USING FOIL ACTIVATION DATA,
FUEL POSITION 20
22
(n
a, I 0r
z
0
c-
w
0
w
(I)
N
z
0
w
104
102
104
ENERGY
106
,
eV
FIG. 4.2 NEUTRON ENERGY SPECTRUM USED FOR FAST NEUTRON
DOSE RATE CALCULATIONS FROM FOIL ACTIVATION
DATA - RUN 29
CHAPTER 5
HEAT TRANSFER AND FRICTION FACTOR RESULTS
Heat transfer data have been taken using an out-of-pile
test heater since the beginning of loop operation in August,
1961. Also, as described in the previous progress report, a
new test heater (THT) was installed with provision for pressure drop (or friction factor) measurements as well as heat
transfer measurements. During this period, friction factor
measurements and additional heat transfer measurements were
made using out-of-pile loop operation and the new test
heater THT.
A report (1.2) was issued in September, 1965
summarizing and analyzing the new friction factor and heat
transfer data as well as all previous heat transfer data
obtained with the M.I.T. Loop and establishing the best
correlations for both the heat transfer coefficient and the
friction factor.
In Figure 5.1, a comparison of all M.I.T. data taken
up to Run 14 (466 data points) are presented on a plot of
Nu/Pr *4 vs Re and compared with the Dittus-Boelter correlation,
NuB
o4 = 0.023 Re0.8
Nu/rB
RB'
with all properties evaluated at the bulk temperature.
(5.1)
The
data fall within +10% of this correlation over the Reynolds
number range covered in the experiments of 7 x 103 to 1.5 x
1050
A Colburn type correlation has been used for correlation
of both heat transfer and friction factor data,
j*
= StPro. 6 = 0.023 Re-0.2 =
(5.2)
In several measurements on Santowax WR, simultaneous heat
transfer and friction factor measurements were made using
test heater TH7. These results are presented in Figure 5.2
and compared with the Colburn relation with good agreement.
400
-
300-
0
Nu/Pr0.4 0.023
Re0.8
0
± 10%
*
200
150-
a100
z- 0
~80
-
0
Ts 0
0
50 /o
40
ORGANIC,
SANTOWAX
I
OMP
-e
&1~
30
-
15
4
5
6 7 8 910
1
1.5
ALL M.I.T.,IRRADIATED
TEST
HEATEF
USED
OMP
TH5
TH6
0
2
OMP
TH6
o
v
3
5
II
x
12
13
WR
WR
WR
WR
WR
TH6
TH6
TH6
TH7
TH7
-
20
FIG. 5.1
0
M.1.T.
IRRADIATION
RUN No.
111111
1
1
5 6 7 8910
4
3
2
Reynolds No., Re.
1
1.5
ORGANIC COOLANT, HEAT TRANSFER DATA
25
10-I
I
i
i
I
I
I
I
I
I
-
%I-
0
IL<
f = 0 023
z
8
0
Reo-.20
U-
o
RUN 12
a
RUN 13
10-2
III
2F
0
St Pr
2/ 3
=0.023Re-.
20
0
0
|I
I
1.5
FIG. 5.2
I
I
I
4
I
5
I
6
3
2
REYNOLDS NO., ReB
I
I
8 105
I
1.5
FRICTION FACTOR AND HEAT TRANSFER
FACTOR FOR IRRADIATED SANTOWAX WR,
UPSTRE AM HALF OF TEST HEATER 7
2
26
Additional measurements on both Santowax WR and distilled
water were made in which only the friction factor was measured.
In Figure 5.3, the friction factor data measured for Santowax
WR and for distilled water with test heater THT are presented
and compared with the Colburn relation with excellent agreement. In Figure 5.4, the heat transfer data for Santowax OMP
are compared with the C olburn relation, again with excellent
agreement.
In summary, the heat transfer data and friction factor
data obtained in the M.I.T. Organic Coolant Project can be
represented within +10% by the following standard correlations
over a Reynolds number range of 10 to 105:
Dittus-Boelter Equation
NuB = 0.023 ReO'8 Pr0. 4
(5.3)
or
Colburn Equation
StPr.
=
0.23 Re 0 2
where f =
1A2P
L
pVT
(5.4a)
(5.4b)
0.05
0.04
0
0.03
UL
z
9 0.02
L
0.01
4
FIG, 5.3
6
8
104
3
2
1.5
REYNOLDS NO.,
4
6
8
105
1.5
2
Re B
FRICTION FACTOR DATA FOR TH7, SELECTED
DATA AND WATER DATA
SANTOWAX
WR
t~3
28
0.01
(0
c
.. 0.005
C
0
0.004
0.003
0.002-
6
FIG. 5.4
I
I
0.001
8
104
1.5
5
4
3
2
REYNOLDS NO., ReB
6
8
COLBURN ANALOGY FOR M.I.T., IRRADIATED
SANTOWAX OMP, HEAT TRANSFER DATA
105
.4-
--
CHAPTER 6
SUMMARY OF PROPERTY MEASUREMENTS FOR RUN 14
During Run 14, the density, viscosity and number average
molecular weight of three samples, 14L-4, 8, and 12, were
measured.
In Figures 6.1 and 6.2, the density and viscosity
results respectively are presented for these three samples
representative of the beginning, middle, and end of Run 14.
From Figure 6.1, the density appears to decrease by 1.0 to
1.5% depending on temperature during Run 14. The viscosity
from all three samples is essentially the same, however, as
is evident from Figure 6.2.
In Table 6.1, the average molecular weight of the bottoms
from Samples 14L-4, 8, and 12 are presented; the average value
is 449. In Table 6.2 and Figure 6.3, a summary is given of
previous measurements of the average molecular weight of the
bottoms for steady-state runs. Additional data are required
before any definitive conclusions can be drawn. It will be
noticed however that the average molecular weight appears to
increase with %HB at a given irradiation temperature in all
cases. Also, the molecular weight appears to decrease as
irradiation temperature increases at a given HB content.
Table 6.1
Average Molecular Weight of Run 14 High Boiler
(quaterphenyls not recycled)
Sample No.
Average Molecular Weight
14L-4
14L-8
14L-12
444
450
452
Average
449
.. .........
30
1.00
-
0.98
0.96
0.94
0.92
C-)
0.90
0.88
0.86-
0.84-
0.82
0.80
0.78 .
400
450
500
700
650
550
600
TEMPERATURE, *F
FIG. 6.1 DENSITY MEASUREMENTS
750
FOR RUN 14
800
1.0
I
0.9* -
I
|I
1.10
|
1.20
31
0 14L -4
-
0.8
I
A
14L-8
+ 14L -12
0.7*
0.6 -
0.5
w
c'n
0
a_
z
0.4 k-
0.3 10
C-)
0.2 I-
0.1
L
0.70
I
0.80
FIG. 6.2
|I
0.90
|I
1.00
I/ T x 103
VISCOSITY
1.30
OR-I
MEASUREMENTS
FOR RUN 14
Table 6.2
Summary of Average Molecular Weight for
Steady-State Loop Irradiations Through Run 14
Run
No.
Irradiation
Temperature, OF
% HB
Average Molecular
Weight of HB
Quaterphenyls
Recycled
11
14
1C
610
9.6
416
No
572
610
11.0
32.3
449
690
No
No
5
700
30.8
702
Yes
7
6
3
750
750
750
11.5
15.2
30.3
599
644
666
Yes
Yes
Yes
2
750
32.4
580
No
4
78o
24.9
658
No
10
800
17.2
540
Yes
9
800
26.9
633
Yes
U)
R)
33
720
I
I
cc:
w 6801-J
m-6 40F+
0
600-
w
/
5601--
/
w
-J
0
w
w
520H-
480H-
0 572 -610 *F, QUATERPHEN YLS
NOT RECYCL ED
o
440|-
+ 7500F, QUATERPHENYLS
RECYCLED
bO800F, QUATERPHENYLS
z
RECYCLED
400 0
FIG. 6.3
5I
I
I
20
15
10
% HB IN COOLANT
I
I
25
I
30
I
35
AVERAGE MOLECULAR WEIGHT OF HIGH BOILER AS
FUNCTION OF HIGH BOILER CONCENTRATION
. ........
34
CHAPTER 7
TRAVEL AND REPORTS ISSUED
In June, 1965 E. A. Mason and T. H. Timmins of M.I.T.
visited the Chalk River Laboratories of AECL for two days and
participated in technical discussions concerning the organic
coolant work being carried out at these laboratories and at
M.I.T.
On August 5 and 6 1965 D. T. Morgan, W. N. Bley, and
T. H. Timmins visited Atomics International at Canoga Park,
California to discuss the experimental program planned for the
M.I.T. In-Pile Loop for the next two years, considering the
requirements of the HWOCR Program and the capabilities of the
M.I.T. Loop. An experimental program which satisfied the
HWOCR requirements was agreed on by both Atomics International
s4pd M.I.T. and submitted to the AEC where approval was granted
to the program.
A report describing and analyzing the friction factor
and heat transfer measurements performed at M.I.T. on organic
coolants was issued in September, 1965 (1.2). A topical
report (to be assigned the number MIT-334-34) describing all
results on Santowax WR up to Run 13 is in preparation and
should be completed during the next quarter.
REFERENCES
1.1
1.2
Mason, E. A., "In-Pile Loop Irradiation Studies of
Organic Coolant Materials," Progress Report, October 1
December 31, 1964, MIT-334-12, Department of Nuclear
Engineering, M.I.T., February 1, 1965.
Swan, A. H., and E. A. Mason, "Friction Factor and Heat
Transfer Correlation for Irradiated Organic Coolants,"
MIT-334-23, Department of Nuclear Engineering, M.I.T.,
September, 1965.
-
M.I.T. REPORT DISTRIBUTION LIST
AEC Contract AT(38-1)-334
ADDRESSEES
COPIES
Idaho Operations Office, P.O. Box 2108, Idaho
Falls, Idaho, Att: Dir. of Nucl. Tech. Div.
Canoga Park Area Office, P.O. Box 591, Canoga
Park, Calif., Att: Chief, Power Systems Br.
Chicago Operations Office, 9800 S. Cass Ave.,
Argonne, Ill., Att: Dir. of Reactor Engr. Div.
New York Operations Office, 376 Hudson St., N.Y.,
N.Y. 10014, Att: Dir. of Reactor Div.
Savannah River Operations Office, P.O. Box A,
Aiken, S. Carolina
Att: Dir., HWOCR Div.
J. H. Kruth
USAEC Technical Representative, USAEC, Whiteshell
Branch, Pinawa, Manitoba, Canada
Brussels Office, USAEC, US Mission to the European
Communities, 23 Avenue des Arts, Brussels, Belgium
USAEC, Washington 25, D.C.
Att: Mr. Angelo Giambusso, Div. of Reactor
Development
Att: Chief, High Temp. Reactors Br., Div. of
Reactor Development
Att: Clitef, Water Reactors Br., Div. of Reactor
Development
Att: A. N. Tardiff, Div. of Reactor Development
Atomics International, P.O. Box 309, Canoga Park, Calif.
Att:
Att:
Att:
C. A. Trilling
R. T. Keen
Combustion Engineering, Inc., Windsor, Conn.
Att: R. J. Rickert
Dr. C. W. J. Wende, E. I. du Pont de Nemours,
Explosives Dept., AED, Wilmington, Delaware 19898
Dr. W. M. Campbell, Dir., Chem. and Met. Div.,
Chalk River Proj., AECL, Chalk River, Ontario,
Canada
Dr. R. F. S. Robertson, AECL, Whiteshell Branch,
Pinawa, Manitoba, Canada
Dr. H. Hannaert Chemistry Department, Euratom CCR,
Ispra (VareseS, Italy
1
1
1
1
6
2
2
2
1
1
2
1
4
1
4
1
3
3
4
ADDRESSEES
COPIES
Babcock and Wilcox Co., Lynchburg, Virginia
Atomic Energy Div., Att: W. M. Vannoy
USAEC Div. of Tech. Information Ext., P.O. Box 62,
Oak Ridge, Tenn. (for standard TID-4500 dist.)
Dr. W. G. Purns, Atomic Energy Research Establishment,
Radiation Chemistry Building 146, Harwell, Didcot,
Berks., United Kingdom
Mr. P. A. Houllier, Laboratoire Central de Recherches
Progil, 10 #'uaidu Commerce (Boite Postale 105),
Lyon-Vaise, France
Mr. P. Leveque, Chef du Service de Physico-Chimie
Appliquee, CEA Centre D'Etudes Nucleaires de Sac~lay,
Boite Postale No. 2, Gif-sur-Yvette (Seine-et-Oise),
France
Dr. E. Proksch, Reactorzentrum Seibersdorf,
Lenaugasse 10, Wien VIII, Austria
Mr. J. R. Puig, CEA Centre D'Etudes Nucleaires de
Saclay, Boite Postale No. 2, Gif-sur-Yvette (Seineet-Ose), France
1
1
1
1
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