APEX APEX
411 411
,
..:.
.""'T
IRRADIATION TESTING IRRADIATION TESTING OF LIQUIDS OF ORGANIC ORGANIC LIQUIDS G.W. POMEROY POMEROY G.W. CALKINS V. P. CALKINS
LEGAL NOTICE NOTICE LEGAL This report report was was prepared prepared as as an account account of GovernGovernThis sponsored work. Neither Neither the the United United States, States, ment sponsored Commission, nor the Air Force, Force, nor any nor the Commission, person acting acting on behalf behalf of the Commission Commission or the the person Force: . Air Force: A. Makes Makes any warranty warranty or representation, representation, express express implied, with with respect respect to the the accuracy, accuracy, comor implied, pleteness, usefulness the informati informati on pleteness, or usefulness of the contained in this this report, report, or that that the the use use of any any contained information, apparatus, method, or prooe ss information, apparatus, method, prc~ess disclosed this report report may not not infringe infringe disclosed in this privately owned owned rights; rights; or privately Assumes any liabilities liabilities with respect B. Assumes with respect to the the use of, or for damages damages resulting resulting from from the the use use use information, apparatus, method, or of any any information, apparatus, method, process this report. process disclosed disclosed in this report. As used "person acting used in the the above above "person acting on behalf behalf of the the Commission Commission or Air Force" Force" includes includes any any employee the Commission Commission or Air ployee or contractor contractor of the Force conForce to to the the extent extent that that such such employee employee or contractor, tractor preparea, prepares, handles, handles, or distributes, distributes, or proprovi.des access to, his vides access to, any information information pursuant pursuant to his employment employment or contract contract with with the the Commission Commission or Air Force. Force. Printed Printed in in USA. Price Price $1.25. $1.25. Available Available from the the Office Office of Technical Technical Services Services U.S. Department Department of Commerce Commerce Washington Washington 25, 25, D.C. D.C.
APEX- 41' UC·40 Radiation Effects Effects on Mat"rials Mat"rials UC·40 Radiation (TID (TID 4500, 4500, 13th 13th Ed., Ed., Rev.) Rev.)
IRRADIATION IRRADIATION TESTING TESTING OF ORGANIC ORGANIC LIQUIDS LIQUIDS G. W. W. Pomeroy Pomeroy
V. P. P. Calkins Calkins Applied Materials Materials Research Research Sub·Section Sub-Sec+ien Applied
August, 1955 1955 August,
United States States Air Air Force Force United
Contract No. 33(038)-21102 Contract No. AF 33(038)-21102
United States States Atomic Atomic Energy Energy Commission Commission United
Contract No. AT (11-1)-171 (11-1)-171 Contract No. AT
GENERALO ELECTRIC GENERALfi ELECTRIC AIRCRAFT NUCLEAR PROPULSION DEPARTMENT DEPARTMENT AIRCRAFT NUCLEAR PROPULSION ATOMIC PRODUCTS PRODUCTS DIVISION DIVISION ATOMIC Cincinnati 15, Ohio Ohio Cincinnati 15,
Published by Published Technical Publ ications ications Sub.Section Sub.Section Technical
September 5, 1958 1958 September
3
Abstract Abstract This This report report summarizes summarizes the results results of irradiation irradiation tests tests of organic organic materials materials conducted in the HB-2 facility facility of the LITR and in the electron electron beam of the GE-ANPD 2-Mev Van de Graaff Graaff accelerator. accelerator. Several Several organic organic liquids liquids capable capable of withstanding withstanding temperatures tested, and descriptions descriptions temperatures up to 650 65000F have been tested, of the tests tests and typical typical data are are presented. presented.
5
Introduction Introduction tests was conducted on organic organic liquids liquids in the HB-2 experimental experimental series of irradiation irradiation tests A series facility of the Low Low Intensity Intensity Test Test Reactor Reactor (LITR) (LITR) and in the beam beam of the General General Electric Electric facility Aircraft Nuclear Propulsion Department Department 2-Mev Van Van de Graaffaccelerator. Graaffaccelerator. Aircraft Nuclear Propulsion The HB-2 facility in the LITR is a horizontal horizontal hole that runs runs east east and west and extends extends inward from the cility east side reactor to the shell shell containing containing the reactor reactor core. core. Figure Figure 1 is a plan view east side of the reactor reactor showing the location location of the hole with respect respect to the core core and reflector. reflector. of the reactor liquids of promising promising radiation radiation stability, stability, as determined determined by preliminary evaluOrganic liquids preliminary evaluations conducted by GE-ANPD and outside outside contractors, contractors, were were subjected subjected to engineering engineering ations tests in reactor reactor radiation radiation fields at temperatures temperatures up to 650 650o0F. Liquids that have been tested tested tests alkylbenzene 350, alkylbenzene alkylbenzene 250, Dowtherm-A, Dowtherm-A, Pentalene Pentalene 195, 195, and to date include alkylbenzene number 290.* This report report describes describes the test test facilities facilities and and test test operation operation and presents presents typical typical test test data This and their analyses. and their analyses. presents a more more detailed detailed treatment treatment of the material material presented presented in the main The appendix presents report. portion. of the report.
*Alkylbenzene 350 and alkylbenzene alkylbenzene 250 are are commercial commercial liquids liquids obtained obtained from from the the California California Research Research *Alkylbenzene Corporation. They They are mixtures mixtures of mono- and di-alkylated di-alkylated benzenes. benzenes. The The numbers numbers 350 and 250 designate designate Corporation. the average average molecular molecular weights weights of of each each liquid. liquid. the Dowtherm-A is is a commercial commercial heat heat transfer transfer liquid l iq uid manufactured manufactured by the the Dow Chemical Chemical Company Company containing containing Dowtherm-A mixture of of diphenyl diphenyl oxide oxide and diphenyl. diphenyl. a mixture The Pentalenes Pentalenes are are mixtures mixtures of of monomono-,, didi-,, and poly-amylnaphthalenes. Pentalene 95 is is an undistilled undistilled The poly-amylnaphthalenes . Pentalene mixture, and and the the Pentalene Pentalene 195 is a distilled distilled mixture mixture of the the amylnaphthalenes amylnaphthalenes obtained from Pentalene Pentalene 95; mixture, obtained both mixtures mixtures are are corr.mercially corr.mercially available. available. The The numbers numbers 95 and 195 are are designations designations by the the Sharples Sharples ChemiChemiboth cal Company Company and do not not refer refer to molecular molecular weights the respective respective rr:ixtures rr:ixtures. . The The residue residue of Pentalene Pentalene cal weights of the after a 62500 FF distillation distillation has has been been designated designated number number 290 by GE-ANPD GE-ANPD. . The The number number 290 approximates approximates 195 after the molecular molecular weight. weight. the
7
8
66n
II
BERYLLIUM BERYLLIUM
FUEL ELEMENTS FUEL ELEMENTS
CONTROL (SHIM) (SHIM) RODS RODS CONTROL
SPECIAL PIECES
arrangement of the the LITR LITR Fig. 1- Lattice-reflector Lattice-reflector arrangement Fig.
Irradiation Facilities and and Test Systems Systems Irradiation Facilities Reactor Irradiation Irradiation Test Test System System Reactor The experimental experimental loop and accessory accessory equipment equipment used for reactor irradiation testing reactor irradiation testing of selected organic organic liquids liquids were were designed designed to be used with the HB-2 facility the selected facility of the LITR. LIT R. system included a canned rotor rotor pump; heat exchangers exchangers to heat the test The system test liquid, liquid, to cool viscosity measurements, measurements, and to serve serve as pump bearing the liquid for viscosity bearing coolant; coolant; a can for containing the liquids liquids within the reactor; reactor; a filter; filter; a remote-indicating remote-indicating flowmeter; flowmeter; a remotecontaining remoteindicating viscometer; viscometer; a sump or reservoir; reservoir; and a wet-test wet-test gas meter indicating meter to measure measure the offgas. Figure Figure 2 shows typical typical equipment equipment used at the LITR. The equipment gas. equipment is is inclosed inclosed in a gas-tight container container filled with carbon carbon dioxide because because of the flammable gas-tight flammable nature nature of the liquid liqUid tested. Figure Figure 3 shows the control control panel used with the test tested. test equipment. equipment. A detailed detailed descripdescriptest system system components components together together with some operating tion of the test operating description description is given [in the appendix. lin Graaff Test Test System System Van de Graaff Irradiation of organic organic liquids liquids in the Van Van de Graaff Graaff accelerator accelerator has been found Irradiation found useful useful in establishing the relative relative stability stability of the liquids liquids as measured measured by gas establishing gas evolution evolution and viscosity viscosity change.* A sketch sketch of a test test system system devised devised for use with the GE-ANPD Van de Graaff change.* Graaff accelaccelerator is shown in Figure Figure 4. A detailed detailed description description of the test system is given in the erator test system appendix. ·This work is is discussed discussed further further in two reports reports issued issued by the General General Electric ·This Electric Aircraft Aircraft Nuclear Nuclear Propulsion Propulsion Department: V. P P.. Calkins Calkins, , "Radiation "Radiation Damage Damage to Non-Metallic Non-Metallic Materi Materials," Department: als," APEX-167, APEX-167, August August 1954; G. Collins Collins and V. P P.. Calkins Calkins, , "Radiation "Radiation Damage Damage to Elastomers Elastomers, , Organic Organic Liquids, Liquids , and Plastics," Plas tics, " C. G. APEX-261, September APEX261 , Se ptember 1956.
9
10
Fig. 2 - A typical typical hydrocarbon hydrocarbon recirculating recirculating loop used used at the the Low Intensity Intensity Fig. Test Reactor Reactor (with side side of housing housing removed) Test
..
11 11
"
Qi
'"
c..
] o '" U I CO>
12
W ET- TEST WET· TEST METER METER
CONDENSER
VAN DE DE GRAAFF GRAAFF VAN ELECTRON BEAM ELECTRON BEAM
1·MIL AI
7.5 CM
I
Fig. 4 - A typical typical test test cell cell for for electron electron irradiation irradiation of liquids Fig. liquids
Interpretation of Test Interpretation Test Data Data and General General Conclusion Conclusion A comparison comparison of the data from from the 300 30000F F reactor reactor irradiation irradiation tests tests indicated indicated that that alkylalkylbenzene basis of viscosity benzene 250 was more more radiation radiation stable stable than alkylbenzene alkylbenzene 350 350 on the basis viscosity change and gas evolution rate dosage, butwas rate as a function of dosage, but was notas not as stable stable as Dowtherm-A. Dowtherm-A. These These data are are presented presented in Table Table 1; 1; plots plots of gas evolution and viscosity viscosity versus versus dosage are are shown in Figures Figures 6, 7, and 8. When When alkylbenzene alkylbenzene 250was 250was subjected subjected to reactor reactor irradiirradiation tests that the physical tests at 50000F, it was found found that physical property property changes changes with radiation radiation dosage were were not markedly markedly different different from from those those measured measured in the 300 30000F F tests tests (see (see Table Table 3). search for liquids liquids usable usable at 60000F, Van de Graaff Graaff data indicated indicated that that Pentalene Pentalene 95, In a search Pentalene 195, 195, and number number 290 showed stability stability at these these temperatures. temperatures. Of Of the three three Pentalene liquids tested tested to date, date, number number 290 appears appears most most promising. promising. A study of hydrogen conliquids tent and over-all over-all radiation radiation stability stability is given in Tables Tables 8 and 9 and in Figures Figures 23, 24, tent 25, and 26.
13 13
Operation of of Test Systems Systems Operation reactor irradiation irradiation engineering engineering tests tests on organic organic liquids liquids were Nine reactor were conducted conducted in the HB-2 facility of the LITR. In the initial initial tests tests alkybenzene alkybenzene 350, alkylbenzene facility alkylbenzene 250, and Dowtherm-A Dowtherm-A were tested tested for radiation radiation stability stability at an operating operating temperature temperature of 30000F. Alkylbenzene were Alkylbenzene 250 subjected to additional additional testing testing at temperatures temperatures up to 50000F. Gas evolution was subjected evolution was measmeasured irradiation temperature temperature and dosage. dosage. A run was also ured as a function of irradiation also conducted at 45000 -- 50000F to determine determine the heat heat transfer transfer characteristics characteristics of alkylbenzene 450 alkylbenzene 250 as a funcirradiation dosage. dosage. tion of irradiation Approximately 85 85 irradiations irradiations were were performed performed in the Van de Graaff Approximately Graaff accelerator accelerator using using large variety variety of organic organic liquids. liquids. Twenty-five Twenty-five screening screening tests a large tests were were performed performed using using varvartypes of liquids liquids to determine determine general general radiation radiation stability.* stability.* Approximately ious types Approximately 60 organic organic liquids, shown by the screening screening tests tests to be the most promising liquids, promising radiation-stable radiation-stable types, types, were subjected to high temperature temperature - high dosage dosage tests. tests. were subjected A detailed detailed description description of the irradiation irradiation test test rigs rigs and a summary summary of the data data obtained obtained from the reactor reactor irradiation irradiation and Van de Graaff Graaff tests tests are from are given in the Appendix. ·Other screening screening tests tests were described described in a report by V. P. Calkins Calkins, , "Radiation "Radiation Damage to Non-Metallic ·Other Non-Metallic Materials," General Elecuic Electric Aircraft Aircraft Nuclear Nuclear Propulsion Propulsion Department, Department, APEX-172, August Materials," August 1954, p. 39.
15 15
Appendix Appendix Details of Test Test Systems, Details Operation, and and Results Results Operation, Reactor Irradiation Irradiation Tests Tests Reactor schematic diagram diagram of a typical typical hydrocarbon-recirculation hydrocarbon-recirculation loop for reactor reactor irradiation A schematic irradiation testing is shown shown in Figure Figure 5. A modified Chemco canned rotor rotor pump was used testing used to avoid the problem of mechanical mechanical seals seals and stuffing boxes. boxes. On On elevated-temperature elevated-temperature tests problem tests a small small portion of the pump discharge discharge is fed through a cooling coil in which which the liquid temperature portion temperature remote-indicating viscosity reduced to 100<> 100<>- 150 15000FF and then through the Viscoson, a remote-indicating is reduced viscosity sensor, which continuously measures measures the viscosity viscosity and and transmits transmits the values values to a recorder sensor, recorder control panel. over the pump bearings bearings and back into the on the control panel. The cooled liquid flows over inlet line. line. The main discharge discharge from the pump flows through a heater heater to the reactor. pump inlet reactor. heater consists consists of a noninductively-wound double double coil of stainless stainless steel steel tubing, both The heater which are are electrically electrically grounded. By By means of a center center electrical ends of which electrical tap, an electric electric current is passed passed through the tubing in two two parallel parallel circuits. circuits. The heat generated generated in the wall current transferred with high efficiency to the test test liquid, which flows through of the tubing is then transferred the tubing.
Fig. 5 - Hydrocarbon Hydrocarbon recirculation recirculation loop for for reactor reactor irradiation irradiation tests tests Fig.
17
18
The liquid discharged discharged from the heater heater flows to a container container that that is located located in the HB-2 test hole of the LITR approximately test approximately 13 13 feet in from the outer outer shield shield face fac e of the reactor. reactor. This container place by a sealed, water-cooled aluminum probe probe from which it container is held in place sealed, water-cooled thermally insulated insulated by Refrasil Refrasil insulation. insulation. Small-diameter Small-diameter tubing carries carries the test test is thermally reactor to and from the external external pumping system. system. The pressurized liquid in and out of the reactor pressurized this external external loop is located located close close against against the face of the reactor, reactor, as housing containing this shown shown in Figure Figure 2. A C02 atmosphere atmosphere is maintained maintained within the box and throughout throughout the rereactor probe to minimize actor probe minimize fire fire hazards hazards in the event of a test-loop test-loop leak. leak. The irradiated passes through a filter irradiated test test liquid coming out of the reactor reactor first first passes filter to reremove any solids or flow passes solids that that might foul foul the test test loop loop or flow meter. meter. The filtered filtered liquid then passes through the flow-measuring discharged into the sump, where gaseous flow-measuring device and is discharged gaseous decomposition products formed by the reactor composition products reactor irradiation irradiation are are released released by the liquid. liquid. The slight pressure (2 pass through slight pressure (2 inches of water) developed by this action , causes causes the gas to pass a wet-test wet-test meter meter which which is connected to the top of the sump. After being metered, metered, the disdischarged charged gas either either is collected collected by water water displacement displacement in sample sample bottles bottles for subsequent subsequent analysis analysis or or is carried carried off through the reactor reactor vacuum exhaust system. system. The photograph shown shown in Figure Figure 3 was taken while the alkylbenzene alkylbenzene 250 was being tested tested at 50000 FF and shows the instrumentation proinstrumentation required required for the test test facility. facility. This equipment prometering, totalizing, recording, and controlling controlling facilities facilities for the test test apparatus. apparatus. In vides metering, totaliZing, recording, these instruments instruments control control units units of safety safety circuits circuits interconnected interconnected with the addition, most of these alarm system system and the reactor reactor fast-setback fast-setback or or scram scram controls. controls. LITR alarm engineering reactor reactor irradiation irradiation tests facility of the LITR The nine engineering tests conducted in the HB-2 facility using variations variations of the experimental experimental loop are are described described in the following following sections. sections. using
SCALE A SCALE A SCALE B SCALE
140
2
33
4
6
4
5 10
Gamma dosage dosage for for alkylbenzene olkylbenzene 250 Scale A: A : Gamma
fr-
ond Oowth.rm·A Dowth.rm·A and Scale B: Gamma Gamma dosage for alkylbenzene alkylbenzene 350 Scale
120
II .~ .~ ':;; ~ .~ .~ z·
100
II
,,.
'"«-c'"C>
"
•
II
11
ALKYLBENZENE ALKYLBENZENE 250 250
,, ,
/
1/
//
60
II
11 11
11 ,11
80
/ I
J
ALKYLBENZENE 350 ALKYLBENZENE 350
00
i= :::l :::l ...J -' 00 > > w
,/ ,I
/ I
/ I
40
,/ ,/ 1 20
0
'/ '/ II• 1/ I· I' 0.2 0.2
DOWTHERM·A DOWTHERM-A
--
0.4 0.4
- 0-1 -1-00--- --00 -0-j-10.6 0.6
0.8 0.8
1.0 1.0 18 18
FAST DOSAGE, 10 FAST NEUTRON NEUTRON DOSAGE,
1.2 1.2
__.•... .....
1.4 1.4 2 2
neut,ons / cm neutron./cm
Fig. 6 - Gas Gas evolution evolution alkylFig. from alkylbenzene 350, alkylbenzene alkylbenzene benzene 350, 250, and Dowtherm-A Dowtherm-A as as funcfunc250, tions of of combined combined reactor reactor tions radiation (fast (fast neutron neutron plus radiation plus gamma dosage) dosage) at at 30000 FF gamma
19 19 Screening Tests Tests at 3000F - In In these these tests tests a 700-milliliter 700-milliliter aluminum container Screening container was used in the reactor reactor irradiation irradiation test test loop, and and alkylbenzene alkylbenzene 350, 350, alkylbenzene alkylbenzene 250, and Dowtherm-A irradiated in succession. succession. During the course course of the tests were irradiated tests the LITR LIT R power level level was increased from 1900 1900 kilowatts to 3000 3000 kilowatts, kilowatts, and a variety variety of flux levels increased levels was used to dosages and and data shown shown in the 300 30000F irradiation irradiation test summary, Table 1. give the dosages test data summary, Figures 6, 7, and and 8 compare compare gas evolution rates rates and viscosity viscosity changes Figures changes for the three three neutron dosage. liquids as functions of fast neutron Stability of Alkylbenzene 250 250 at 450 45000 -- 500 50000FF - For Radiation Stability For this this experiment experiment the 700milliliter stainless stainless steel steel container container was located located to support support the test milliliter test liquid in a position position 3 11 inches inches from the end of the HB-2 hole. A 1/ 1/4-inch-thick inches through 11 4-inch-thick aluminum plate, plate, which seals seals the end end of this this test test hole, is positioned positioned against against the reactor which reactor fuel elements. elements. The average fast-neutron-flux fast-neutron-flux component (0.5 Mev Mev and above) above) of the reactor average reactor radiation radiation for this this 12 position with the reactor reactor at the 3000-kilowatt 3000-kilowatt operating operating level level is approximately position approximately 6.48 6.48 x 1012 13 n/cm n/cm22-sec, thermal-neutron-flux component is approximately n/cm -sec, and the thermal-neutron-flux approximately 1. 7 x 1013 n/cm22-sec. A flux diagram diagram showing showing the complete complete spectrum spectrum of the radiation sec. radiation field versus versus position pOSition measured from the 1/ 1/4-inch inner plate plate of the HB-2 facility facility is shown shown in Figure measured 4-inch inner Figure 9. The values given are are for a reactor reactor power level of 1500 1500 kilowatts. kilowatts. With a flow 800 cubic cenvalues flow of 800 centimeters of test test liquid per per minute through the reactor, reactor, a heater timeters heater input of approximately approximately 2 maintained the irradiated irradiated liquid at 480 48000 -- 500 50000F. The temperatures kilowatts maintained temperatures of other other parts parts test loop loop under these these conditions are shown in Table Table 2. of the test are shown The test test liquid in the reactor reactor can is heated an additional additional 35 F during irradiation 35 00F irradiation as a result approximately 500 500 watts of nuclear nuclear heating. heating. result of approximately 18 18
GAMMA DOSAGE, DOSAGE, 10 GAMMA
y/em y/ em2
2
4
SCALE A SCALE
SCALE SCALE B
5 10
4
Scal. A: Gamma Gamma dosage dosage for alkylben::tene alkylben::tene 250 _ Scol. 250 1400 1400
r"-
and Dowth.rm Dewtherre-A and ~A
Sccle B: Gamma Gamma dosage for for olkylbenzene olkylbenzene 350 ,I Scal.
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1200 1200
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1000 1000
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DOWTHERM-A DOWTHERM-A
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1.0 1.0
18 18
FAST NEUTRON DOSAGE, 10 FAST NEUTRON DOSAGE,
1.2 1.2
1.4 1.4
neutrons/em neutrons / em
2 2
Fig. . 7 - Vi Viscosity (at 100oF lOOoF)) of Fig sco si t y (at of alkylbenzene 350, alkylbenzene 350, aalkyllk ylbenzene 250,, and and Dowthe Dowtherrn-A benz ene 250 rm-A as func functions combined as tions of combined reactor radiation (fast t neure a ctor radi ation (fas neutron plus plus gamma gamma dosage) dosage) at tron at 3000F 300°F
20 20
TABLE 1 TABLE EXPElUMENTAL PHYSICAL PROPERTY PROPERTY CHANGES CHANGES OF OF ORGANIC EXPEIUMENTAL PHYSICAL LIQUIDS WITH WITH IRRADIATION IRRADIATION LIQUIDS Alkylbcnzene (Mol. Wt. Alkylbenzene (Mol. Wt. 350) Ir-radiated+ a Control Control Irradiated
Alkylbenzene (Mol. (Mol. Wt. Wt. 250) 250) Alkylbenzene Control Control Irradiatedb b Irradiated
DOWTHERM-A DOWTHERM-A bb Control Control Ir Ir radiated radiated
Flasil point, point, () ()F F Vlasil
340
245
280
255
240 240
190
Ire point, point, ()()F J' Ire V
355
290
295
NDc
260 260
225
Test Test
!km;ity, glee licnsi tv , g/cc 770F ;11: 770F 100 200 300 400 450 500 Viscosity, e Viscosity, c eut istokcs celltistokes 1000F at: 1000F 300 450 500
D.n7] 0.!171 0.863 0.863 0.827 0.827 0.790 0.790 (0.76J)d (0.76J)d (0.74B) (0.74B) (0.738) (0.738)
0.914 0.914 000905 905 0.868 0.868 0.835 0.835 0.807 0.807 (0.795) (0.795) (0.786) (0.786) 0
25.1 25.1 1.7 1.7 (0.4) (0.4) (0.4) (0.4)
974.0 974.0 9.3 9.3 « « 5) « 5) «
0.865 0.865 0.860 0.860 0.824 0.824 0.785 0.785 0.748 0.748 (0.737) (0.737) (0.726) (0.726)
0.934 0.934 0.925 0.925 0.888 0. 888 0.858 0.858 0.814 0.814 (0.808) (0.808) (0.797) (0.797)
6.56 6.56 1. 04 «« 1) « 1) «
1658 13.8 13.8 ( < 10) « 10) «
1. 058 1. 050 050 1.003 1.003 0.954 0.954 0.905 0.905 0.878 0.878 0.851 0.851
2.51 2.51 0.63 0.63 (0.3) (0.3) (0.3) (0.3)
1. 101 1.092 1.092 1. 049 000 1 000 0.945 0.945 (0. (18) (0.918) (0.888) (0.888) 0 0
45.1 45.1 2.51 2.51 « 1) « « 1) «
Maximum Maximum testin['; testing' tempel-at ternperatu u I-e, re,
°F °F Hydrogen content content Hydrogen hydrogen atoms!c.c atoms z'cc hydrogen at: 77 00 FF 100 200 200 300 400 450 500
500
300
0
0
0.54x101818 0.54x10
Vapor pressure pressure Vapor at 45000 1', atm atm
<1 <1
Precipitation Precipitation or sludging studgi ng or
ND
Film formation formation Film
22 38x1022 6. 38x10 22 22 6.3x10 6.3x10 6.1x102222 6.1x10 5.9x102222 5.9x10 22 5.6x1022 5.6x10 22 22 (5.5x10 ) ) (5.5x10 (5.4x102222 ) ) (5.4xl0
(0.47)f (0.47)f (0.57) (0.57) (0.65) (0.65) (0.67) (0.67)
156
Maximum radiation radiation Maximum testing dosage, dosage, testing 2 fast neutrons/cm neutrons/cm fast
300
6.30x102222 6.30x10 6.3xl02222 6.3x10 6.0x102222 6.0x10 22 5.7x1022 5.7x10 5.4xl02222 5.4x10 (5.4x102222 (5.4x10 (5.3xl02222 ) ) (5.3xl0
(0.47)£ (0.47)£ (0.57) (0.57) (0.65) (0.65) (0.67) (0.67)
Gas evolution evolutiong g Gas
Container Container materials materials
6.33x102222 6.33x10 603x1022 3x1022 2222 0xl0 6600xl0 5.8x102222 5.8x10 5.6xl02222 5.6x10 (5.5x102222 ) ) (5.5x10 (5.4xl02222 ) ) (5.4xl0
6.76x102222 6.76x10 6.7xl02222 6.7xl0 6.4xl022 6.4xl022 6.1x102222 6.1x10 (5.9xl02222 ) ) (5.9x10 (5.8x102222 ) ) (5.8x10 (5.7x102222 ) ) (5.7x10
Specific heat, heat, Specific cal/g-OC cal/g-OC 0 F at: 100 1000F 300 450 500
500
<1 <1
500
300 300
3.0x1022 3.0x1022
22 3. 78x10 78x1022 22 22 3.7x10 3.7x10 306xl0 3 6xl02222 3.4x10 3.4x102222 2222 3.2xlO 3.2xlO 22 (3.1x10 (3.1x10 22 2222 (3.0x10 ) ) (3.0x10
0.40 0.40f f 0.50 0.50 0.60 0.60 0.63 0.63
(0.40)f (0.40)f (0.50) (0.50) (0.60) (0.60) (0.63) (0.63)
3.72x1022 3.72x1022 22 22 3.7x10 3.7x10 22 3.5x10 3.5x1022 22 22 3.4x10 3.4x10 22 22 3.2x10 3.2x10 2222 3.1xl0 3.1xl0
0
98
7
18 5x1018 1. 5x10
18 1. 5x10 5x1018
<1
< 11
<1
ND
ND
ND
ND
ND
Not tested tested Not
Not tested tested Not
Not Not tested tested
Not tested tested Not
Not tested Not tested
Not Not tested tested
Stainless steel steel Stainless or aluminum aluminum or
or Al SS or
or Al SS or
or Al SS or
SS or or Al
SS or or Al Al
2 18 fast Actual Dosage Dosage - O. O. 54x10 54x1018 fast neutrons/cm neutrons/cm2 plus 3. 7x1018 7x1018 gammas/cm gammas/cm2 2 a Actual plus 18 18 2 18 Actual Dosage Dosage - 1. 5xl0 5xl0 fast neutrons/cm ncutrons /c mf plus plus 4. 9xl0 9xl018 gammas/cm gammas /cm- 2 fast b Actual None detected detected c ND _ None Values given given in parentheses parentheses are estimated estimated d Values are v iscoo itv in ill c:elltistokes c cntrstokcs x density density x 6. 72x10 72x10-4 Viscosity in lb/(ft-sec) lb/(ft-sec) e Visc:o:;ity - 4 = Viscosity Based on iinfoorat.ioll nfo r n.a tio n furnished furnished by suppliers. suppliers. Irradiation should not not change change these these properties properties significantly. f Based Irradiation should significantly. Liters per per liter liter pCI' pet' 1 1OIU fast neutrons/cm neutrons/cm2 2 l4l4 Liters OUl fast
<1
21 GAMMA DDSAGE, 10
SCALE SCALE B
ffo-
y/cm
2
2
SCALE A SCALE A
14
18
4
2
4
6
I
I
I
5
,
10
I
l-- {-
Scale A: Gamma 250 Scale Gamma dosage dosage for olkylbenzene alkyl benzene 250 and and Dowtherm-A. Dowtherm-A.
,
Scale B: Gamma dosage for 350. Scale B: Gamma dosage For alkylbenzene olkylbenzene
12
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FAST NEUTRON NEUTRON DOSAGE, 10 FAST DOSAGE,
DOWTHERM-A DOWTHERM-A
I
I
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Fig. 8 - Viscosity Viscosity (at (at 300oF) alkylbenzene 350, alkylbenzene alkylbenzene 250, and Fig. F) of alkylbenzene functions of combined combined reactor reactor radiation radiation (fast (fast Dowtherm-A as functions 0 neutron plus plus gamma dosage) dosage) at 300 300°F neutron F
early part this test, test, the gas that that evolved as a result result of radiation radiation damage During the early part of this test liquid in the 700-milliliter 700-milliliter container container was generated generated at a rate rate of 1.5 1.5 liters liters per per to the test hour. However, However, as the experiment experiment continued, continued, the evolution rate rate steadily steadily decreased decreased and hour. 0.8 liter liter per test. The relationship relationship between gas fell to a value of 0.8 per hour by the end of the test. evolution and radiation radiation dosage of the test test liquid is shown in Figure Figure 10. Total Total gas evolution plotted as a function of the fast fast neutron neutron (~ (~ 0.5 0.5 Mev) Mev) component of the mixed reactor reactor is plotted radiation dosage dosage received received by the liqUid. liquid. Similar Similar data from from previous previous experiments experiments conconradiation 30000F irradiation irradiation temperature temperature also also are are plotted this figure figure to show the ducted at the 300 plotted in this difference in the rates rates of gas evolution at the two two temperatures. temperatures. Except Except for the tempertemperdifference
TABLE 2 TYPICAL TEMPERATURE PROFILE OF REACTOR REACTOR IRRADIATIONTEST LOOP FOR A 49000F LIQUID LIQUID IRRADIATION TEST LOOP IRRADIATIONTEMPERATURE TEMPERATURE IRRADIATION Thermocouple Location Location Thermocouple or heater heater inlet inlet Sump or Heater wall (inlet) Heater Heater wall (outlet) Heater Heater outlet outlet Heater inlet Can inlet Can Discharge to sump Discharge
Temperature, 0ofF Temperature,
290 350 515 515 475 475 465 465 490 415 415
22 22
Thermal neutrons/ em 2_sec Thermal neutrons/em 2_sec
Gammas/ Gammas/emem 2_sec 2_sec Fast neutrons/ neutrons/emem 2_sec 2_sec Fast
0.027 0.027
ev ev
DISTANCE DISTANCE FROM BLANK BLANK END OF HB·2, HB·2, inches inches
Fig. Fig. 9 - Radiation Radiation spectrum spectrum of the the HB·2 hole
23
ature test gas evoluevoluature differences, differences, test conditions conditions were were the the same. same. This This relationship relationship between between gas tion is in the the tion rate rate from from alkylbenzene alkylbenzene 250 and irradiation irradiation temperature temperature is further further discussed discussed in following before and and following section. section. A summary summary of the the physical physical properties properties of alkylbenzene alkylbenzene 250 before after after irradiation irradiation is presented presented in Table Table 3. The F, increased increased with with The viscosity viscosity of the alkylbenzene alkylbenzene 250, originally originally 7 centistokes centistokes at 10000F, irradiation at first hours of the the test. test. irradiation first very very slowly slowly and then then very very rapidly rapidly during during the the last last 10 hours The the alkylbenalkylbenThe data data plotted plotted in Figure Figure 11 11 show the the relationship relationship between between the the viscosity viscosity of the zene and the the liquid liquid zene 250 test test liquid liquid at various various temperatures temperatures the radiation radiation dosage dosage to which which the was is was exposed. exposed. Only the the fast fast neutron neutron ( ~ 0.5 0.5 Mev) component component of the the reactor reactor radiation radiation is plotted. were from the the plotted. The The viscosity viscosity measurements measurements were obtained obtained from from specimens specimens removed removed from test system system periodically periodically during the course of the the experiment. experiment. Independently of these test during the course Independently these measurements measurements a continuous continuous record record of the the viscosity viscosity changes changes produced produced in the the test test liquid liquid was was also the the also obtained obtained by means means of a Viscoson Viscoson instrument, instrument, the probe probe of which which was was located located in the test-liquid from this this inintest-liquid stream stream after after the the bypass bypass cooler. cooler. The The continuous continuous record record obtained obtained from strumentation showed with strumentation showed that that the the viscosity viscosity of the the test test liquid liquid increased increased only only periodically periodically with radiation near steady-state conditions These radiation and that that near steady-state conditions lasted lasted for for considerable considerable periods. periods. These steady-state periods were were especially especially noticeable noticeable during during the the last last half half of the the test test and steady-state periods and are are the the 0F cause F test the curve curve cause of the the break break in the the 5000 test curve curve shown shown in Figure Figure 11. 11. Comparison Comparison of the for 50000 FF test changes for previous previous 30000 tests tests with the the corresponding corresponding test data data shows shows that that viscosity viscosity changes 0 0 are than Therare less less severe severe at the the higher higher irradiation irradiation temperature temperature than at the the 300 FF temperature. temperature. Thermal may the difference. difference. mal degradation degradation of large large molecules molecules at the the higher higher temperature temperature may account account for for the 99 DOSAGE, 10 rods DOSAGE, 10 rods
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Fig, 10 10 - Total Total gas evolution evolution for for alkylbenzene alkylbenzene 250 250 versus versus the fast fast neutron neutron dosage dosage component component of the combined reactor reactor radiation radiation and total total energy absorption absorption
I"" I""
24
TABLE TABLE 3 PHYSICAL PHYSICAL PROPERTIES PROPERTIES OF OF ALKYLBENZENE ALKYLBENZENE 250 BEFORE BEFORE AND AFTER AFTER IRRADIATION IRRADIATION AT 300°F 300°F AND 500°F 500°F Test Test Flash point, OF Flash point, Density, cc Density, g/ g/cc at 1000F 1000F at 2000F 2000F 300°F 300°F 400°F 400°F 450°F 450°F 5000F 5000F
Control Control
Irradiated Ir radiated= a at at 3000F 3000F
Ir radiatede a Irradiated at at 5000F 5000F
280
255
205
0.860 0.860 0.824 0.824 0.785 0.785 0.748 0.748 (0.730)b (0.730)b (0.713) (0.713)
0.925 0.925 0.888 0.888 0.858 0.858 0.814 0.814 (0.797) (0.797) (0.779) (0.779)
0.910 0.910 0.884 0.884 0.846 0.846 0.809 0.809 (0.791) (0.791) (0.773) (0.773)
Viscosity, centistokes Viscosity, centistokes at at 100°F 100°F 200°F 200°F 300°F 300°F 4000F 4000F 5000F 5000F A verage molecular Average molecular weight weight
7 2 1 « 1) « ( < 1) « 250 250
1658 59 14 < 10 < 10 467
Hydrogen Hydrogen content, content, weight percent weight percent
12.1 12.1
11. 4 11.4
11. 8
6.3 6.3 6.0 6.0 5.8 5.8 5.5 5.5 5.2 5.2
6.3 6.3 6.1 6.1 5.9 5.9 5.6 5.6 5.4 5.4
6.5 6.5 6.3 6.3 6.0 6.0 5.8 5.8 5.5 5.5
Hydrogen Hydrogen content, content, 22 (H atoms / cc) x 10atoms/cc) 10-22 at at 100°F 100°F 200°F 200°F 300°F 300°F 400°F 400°F 500°F 500°F Vapor Vapor pressure, pressure, atmospheres atmospheres at 5000F 5000F at Gas Gas evolution, evolution, liters/literliters/liter5.8 5.8 x 109 rads radsc c
< 1
30 7 2 <2 <2 < 2 320
<1 <1
<1 <1
98
198
aMixed aMixed reactor reactor radiation radiation of the the HB-2 HB-2 hole hole of LITR LITR - energy energy absorbed absorbed 8.7 <-, 8.7 x 109 rads rads <; bValues in parentheses parentheses are These bValues are estimated. estimated. These values values reflect reflect more more rerefined of the presented in fined extrapolations extrapolations the density density data data than than those those presented Table Table 1 c5.8 c5.8 x 109 rads rads is is equivalent equivalent to a mixed mixed reactor reactor radiation radiation dosage dosage of the the HB-2 HB-2 hole hole of the the LITR LITR having having a f',0. ~O. 5-Mev 5-Mev fast fast neutron neutron component component of n/cm2 2 1. 0 x 1018 n/cm
\\
25 25 ? 'I DOSAGE, DO SAGE . l() 1{) rods f<'Hh
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~-----------4------------41~----------+_----_1~--,
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neutron$/ cm neutrons/em
2
Fi g. 11 Vi s co sity of alkylbenzene alkylb enz e ne 250 us the th e fast fast neutron dosage dos age Fig. 11-- Viscosity 250 vers versus component combined compon ent ooff the th e combin ed reactor reactor radiation radi a tion and total tota l energy e nergy ab s orpti on absorption
The removed from tes t loop were s ubjected to The specimens specimens removed from the the test loop during during the the experiment experiment were subjected laboratory analysis. analysis. The results results of these these studies studies are are shown shown in Table Table 4 in comparison comparison with laboratory The with values obtained obtained from from studies studies of unirradiated unir radiated alkylbenzene alkylbenzene and alkylbenzene alkylbenzene irradiated values irradiated at at 0 0 300 F. F. Effect Temperature on Gas 250 - Two Effect of Irradiation Irradiation Temperature Gas Evolution Evolution from from Alkylbenzene Alkylbenzene 250 separate runs were were made made in this this second second experiment. experiment. the first first run run alkylbenzene alkylbenzene 250, separate runs In the 250, which previously previously had been been subjected subjected to mixed mixed reactor reactor radiation radiation so that that the the fast fast neutron which neutron 18 n/c (~ 0.5 Mev) dosage dosage component component amounted amounted to 0.5 0.5 x 10 18 n/cm was charged charged into the test test (~0.5 m22, , was into the 0 F, loop F, and 50000 F. F. For loop and circulated circulated at at 3000F, 3000F, 4000 For the the second second run run the the same same experiexperimental mental conditions conditions were were used, used, but the the test test liquid liquid was was alkylbenzene alkylbenzene 250, previously previously irradiirradiated ated for for 3 times times the the dosage dosage of the the liquid liquid tested tested in the the first first run. run. The data data shown shown in Table Table 4 record record the the gas gas evolution evolution rates rates per per hour hour from from the the 700-milliliter 700-milliliter The container of alkylbenzene alkylbenzene under irradiation irradiation at the the various various temperatures. temperatures. Very little little container 250 under at Very time conditions were time was was required required to obtain obtain equilibrium equilibrium conditions whenever whenever test test temperatures temperatures were changed. changed. For For this this experiment experiment the the average average fast fast neutron neutron (~ (~ 0.5 0.5 Mev) flux component component of the the 18 n / cm 2 -sec. The .reactor reactor radiation radiation was was 6.48 6.48 x 10 1018n/cm2-sec. The compositions compositions of the the gases gases obtained obtained from from the are the liquids liquids at the the various various test test temperatures temperatures are shown shown in Table Table 5. Analysis Analysis of the the results results showed s e data showed excellent excellent agreement agreement between between the these data and those those obtained obtained from from previous previous constantconstanttemperature experiments temperature experiments. . Moreover, Moreover, radiation radiation damage damage to alkylbenzene alkylbenzene 250 as as determined determined by hydrogen Higher hydrogen evolution evolution appears appears to be generally generally independent independent of temperature. temperature. Higher total total
;; ~ ------------------------~============----~-----=========~~~---------------------------------
26
TABLE TABLE 4 GAS EVOLUTION EVOLUTION FROM FROM 700 MILLILITERS MILLILITERS OF ALKYLBENZENE ALKYLBENZENE GAS 250 AT VARIOUS DOSAGE LEVELS LEVELS AND TEMPERATURES TEMPERATURES - CONSTANT CONSTANT FLUX FLUXaa
Temperature, of Temperature, of
Gas Gas Evolution Evolution Rate, Rate, Liters Liters per per hour hour 22 Dosagebb 0.5 0.5 x 1018 n/ n/cm Dosage'?b 1. 5 x 1018 n/cm Dosage cm Dosage n/ cm2 2 1. 04 1. 1.27 1.27 1.47 1.47
300 400 500
0.90 0.90 1. 03 1. 1.18 1.18
aAverage aAverage fast fast neutron neutron flux flux component component of the the reactor reactor radiation: radiation: 6.48 6.48 x 1012 2 -sec n/ cm2-sec n/cm bFast / cm2)2 ) component radibFast neutron neutron ( ~ ~ O. 5 Mev) dosage dosage (n (n/cm component of the the reactor reactor radiation ation
TABLE TABLE 5 CHEMICAL CHEMICAL ANALYSIS OF OF THE THE GAS GENERATED GENERATED BY REACTOR REACTOR IRRADIATION IRRADIATION OF OF ALKYLBENZENE ALKYLBENZENE 250 250 AT VARIOUS TEMPERATURES TEMPERATURES Values Reported Reported as Values as Volume Volume Percent Percent TemperaTemperature, of of ture,
Dosage Dosageaa 18 10-18 x 10-
150 300 300 500 500 500
0.5 0.5 0.5 0.5 1.5 1.5 0.5 0.5 1.0 1.0 1.5 1.5
H2 61.4 61.4 62.0 62.0 66.0 66.0 46.2 46.2 48.7 48.7 52.2 52.2
ComCombustiblesb b bustibles 24.1 24.1 20.0 20.0 12.0 12.0 27.3 27.3 22.1 22.1 21.7 21.7
IllumiIllumiCC nants nants
CO
CO2
02 02
Inerts Inerts
11.8 11.8 14.0 14.0 16.0 16.0 18.3 18.3 18.3 18.3 18.7 18.7
0.9 0.9 4.0 4.0 6.0 6.0 5.8 5.8 8.7 8.7 6.1 6.1
0.9 0.9 0.0 0.0 0.0 0.0 0.8 0.8 2.2 2.2 1.3 1.3
0.9 0.9 0.0 0.0 0.0 0.0 1.6 1.6 0.0 0.0 0.0 0.0
0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0
aFast 0. 5 Mev) dosage dosage of test aFast neutron neutron (£ (~o. test liquids liquids at at the the time time of gas gas sampling sampling bCombustible hydrocarbons bCombustible saturated saturated hydrocarbons cnluminants (unsaturated cnluminants (unsaturated hydrocarbons) hydrocarbons) dThe dThe residue residue remaining remaining (N2 or or He) after after removing removing all all reactive reactive components components
d
27 27
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40o-~~+-----4-----1-----1------r-----r--
30t---~~~~~---t----i-----t-----r-
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Constant temperature: 150°F
6
10
12
DISTANCE FROM OF I-'B-2 HOLE, DISTANCE FROM HOT HOT END END OF f'B-2 HOLE, ;nches Inches
Fig. Fig_ 12 - Comp>l.rison Comparison of gas gas evolution evolution mte rate from from alkyl alkylbenzene benzene 250 at at various various positions within within the the 1lB-2 HB-2 hole hole of the the LITR LITR with the the flux pattern pattern positions vf the the hole "f
gas evolution rates rates at the higher higher temperatures temperatures are are attributed attributed to the probability probability that that more more of the products products of radiation radiation damage are are volatile volatile at the high temperatures. temperatures. Effect Effect of Flux on Radiation Damage to Alkylbenzene Alkylbenzene 250 - With minor minor exceptions exceptions the general test facility used general testfacility used for this this test test was as described described for previous previous experiments. experiments. In In place place of the large large container container used for previous previous tests, tests, a small small 100-milliliter 100-milliliter aluminum container container 3-inch 3-inch ID by 11inch inch long, was used for this this test. test. Probe Probe connections connections were were such that it was possible possible to move this this can with the test test liquid circulating circulating through it while the reactor reactor was active. test liquid could be supported active. Thus, Thus, the test supported in any position position in the range range 1/2 112 inch to 15 15 inches inches from the end of the test test hole. It was not necessary necessary in this this test test to use use the heater heater since since the test test liquid was circulated circulated at ambient ambient temperatures. temperatures. During the first first run of this this experiment, experiment, the LITR was held at the 3000-kilowattoperating 3000-kilowattoperating level level while the can containing containing the Circulating circulating alkylbenzene alkylbenzene 250 test test liquid was held for four hours positions within the test hours at each of 15 15 different different positions test hole, starting starting 1/2 1/2 inch from from the core core end of the hole. In the second run this repeated, but in the reverse this test test was repeated, reverse order, order, starting starting 15 15 inches inches from the core core end. At each location location gas evolution data were were obtained. obtained. It was found found that steady-state steady-state conconditions ditions could be obtained obtained in less less than 1 hour after after each move. The measured measured gas evolution rates rates from the 100-milliliter 100-milliliter container container ranged ranged from 0.76 0.76 liter liter per per hour at an average average distance distance of 1 inch from from the core core end of the test test hole to 0.07 liter liter per per hour at the 15-inch 15-inch position. The relationships position. relationships between gas evolution rates rates at these these various various pOSitions positions and the flux levels positions are levels of the various various radiation radiation components components at these these positions are shown in Figure Figure 12. These These data show show that changes changes in gas evolution rates rates with pOSition position closely closely follow follow the fast fast neutron and gamma gamma flux profile profile in this this test test hole. neutron In the third third run of this this experiment, experiment, the power level level of the reactor reactor was decreased decreased from 3000 3000 kilowatts kilowatts to 1500 1500 kilowatts kilowatts and gas evolution measurements measurements were were made at various various positions in the HB-2 hole as in previous positions previous runs. runs. It was found found that that gas evolution evolution rates rates at the lower power level percent of the rates level were were 50 50 percent rates obtained obtained at the 3000-kilowatt 3000-kilowatt level. level.
28 TABLE 6 TABLE PROPERTIES OF OF THE THE LIQUID CONDENSED CONDENSED FROM FROM PROPERTIES THE OFF-GAS OFF-GAS LINE IN ALKYLBENZENE ALKYLBENZENE 250 THE REACTOR IRRADIATION IRRADIATION TEST TEST EXPERIMENT EXPERIMENT REACTOR Viscosity, centistokes Viscosity, centistokes 0F at 1000 at F 0 2000FF 30000 FF
1. 46 0.76 0.76 0.51 0.51
Density, g/ml g/ml Density, at 1000F 1000F at 20000FF
0.816 0.816 0.775 0.775
Flash point point Flash Small cup, cup, of of Small
< 100
Average molecular weight weight verage molecular A
176
Effect of Irradiation Irradiation on the Heat Transfer Transfer Coefficient of Alkylbenzene Alkylbenzene 250 - A reactor reactor Effect the Heat Coefficient irradiation test was was run run in the the LIT LIT R using using alkylbenzene alkylbenzene 250 to establish establish further further the the effects effects irradiation test radiation fields fields on film film formation formation and heat heat transfer transfer characteristics. The test test eqUipequipof radiation characteristics. The ment was was similar similar to that that used used in previous tests except except that that additional additional instrumentation instrumentation was ment previous tests was used to give give more more accurate accurate heat heat transfer transfer data. data. The The alkylbenzene alkylbenzene 250 was was exposed exposed to a used mixed radiath:m r-adiation flux flux (per (per square square centimeter centimeter per second) second) of 1.8 1. 8 x 10 13 thermal thermal neutrons, neutrons, mixed per 13 gammaphotons; 9.4 x 1012 fast fast neutrons, neutrons, and and 2.3 2.3 x 10 1013 gammaphotons; the maximum maximum temperature temperature 9.4 the of the liquid liquid was was maintained at 4600 -- 50000 F. The experiment experiment was was operated operated a total total of 136 the maintained at F. The hours with with the the LIT R at at the the 3000-kilowatt 3000-kilowatt power level. The The experiment experiment was was terminated terminated at hours power level. at will and not because because of increased increased viscosity. viscosity. analysis of the the effect effect of radiation radiation dosage dosage will An analysis the heat heat transfer transfer characteristics characteristics is given given at at the the end end of this this appendix. appendix. on the is experiments, liquid specimens specimens and gas gas samples samples were were taken taken during during the the As in previous previous experiments, liquid course of the the test. test. However, However, in this this experiment experiment a trap trap was the off-gas off-gas line line to course was inserted inserted in the collect any any volatile volatile liquid liquid that that might might distill. distill. was found that that four four milliliters milliliters the collect It was of the liquid condensed condensed out out with with every every liter liter of gas gas evolved. evolved. Table Table 6 shows shows some some of the the properties liquid properties this low boiling boiling decomposition decomposition liquid. liquid. of this Graaff Testing Testing Van de Graaff The 2 --Mev Graaff electron electron accelerator accelerator was used evaluate radiation radiation damage damage The Mev Van de Graaff was used to evaluate several types types of organic organic liquids. liquids. Since Since the the Van de Graaff Graaff is is capable capable of imparting imparting energy energy to several materials rates as as high high as as 100 watts, watts, the the possibility equivalent damage damage to materials at rates possibility of producing producing equivalent liquids within within a much much shorter shorter time time than than that that needed needed for for irradiation irradiation testing seemed seemed useuseto liquids testing with respect respect to testing testing materials materials at high high temperatures temperatures high dosages. dosages. ful, particularly particularly with at and high The test test cell cell used used in the the Van de Graaff Graaff electron electron irradiation irradiation organic liquids liquids was was fabrifabriThe of organic cated of stainless stainless steel steel having having such such dimensions dimensions that that with with a liquid volume of 30 cm cm33, , a cated liqUid volume depth of 2.2 2.2 cm cm was was maintained. maintained. This depth depth was was approximately approximately twice twice that that necessary necessary to ababdepth This sorb 2-Mevelectrons. 2-Mevelectrons. The cell cell flange flange was was sealed sealed with with a 0.0006-inch 0.0006-inch aluminum aluminum window window and sorb The Buna N rubber rubber gasket. gasket. The The O. 0006-inch 0006-inch aluminum aluminum window window was was selected selected because because it it rerea Buna sulted in negligible negligible loss loss due to absorption absorption and negligible negligible scattering scattering of the the impinging impinging elecelecsulted trons. A thermocouple thermocouple well provided provided a means means of measuring measuring the the liquid liquid temperatu temperature re during during trons. well the test. test. The The volatile volatile gases gases formed formed during during irradiation irradiation were exhausted exhausted through through a water water- the were cooled condenser condenser and then then metered metered through through a wet-test wet-test meter. meter. All All samples samples were were magnetmagnetcooled ically stirred stirred to give give equal equal distribution distribution of damage damage throughout throughout the the material. material. sectional ically A sectional
29
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Fig. 13 - Comparison Comparison of of reactor, reactor, gamma, gamma, and electron radiation damage damage Fig. electron radiation benzene to benzene
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test system system is shown shown in Figure Figure 4. The tests tests using the Van Van de Graaff Graaff accelacceldrawing of the test erator are are described described in the following following sections. sections. erator Correlation of Electron Electron Irradiation Various Particle Particle Type Irradiations Irradiations - The extent Correlation Irradiation with Various electron irradiation irradiation damage to a material material is based based on the amount of energy energy absorbed absorbed of electron specific material. material. Since the beam current current and energy energy of the electrons electrons are are known, known, it by a specific calculate the amount of energy energy absorbed absorbed by by a material material during a definite exis possible possible to calculate posure. energy absorption absorption is termed termed a rad and is defined as 100 100 ergs ergs absorbed absorbed posure. The unit of energy per gram. Similarly, Similarly, with respect reactor irradiations, irradiations, if the intensity intensity and energy spectra spectra per gram. respect to reactor thermal neutrons neutrons are are known, known, it is possible possible to calculate calculate the amount of energ energvv of the fast and thermal absorbed by by a specific specific material. material. absorbed
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DOSAGE, .. rcdd.s DOSAGE,
Fig. 15 - Com Comparison reactor,r, ggamma, electron damage Fig. parison of reacto amma, aand nd electron damage to glycerin glyce rin
Experimental work on the correlation correlation of various various particle Experimental particle types types on the basis basis of energy energy absorption was devoted to the irradiation irradiation of benzene, absorption benzene, toluene, toluene, and glycerin. glycerin. The data shown in Table Table 7 and and Figures Figures 13, 14, and 15 15 indicate indicate that shown that for dosages dosages that that are are equal on the basis basis of energy energy absorption on absorption the damage from electron electron irradiation irradiation matches matches within a factor of 2 the damage from from gamma and reactor reactor irradiations. irradiations. Further factor Further correlation correlation has been established on on the comparison comparison of electron electron and LITR irradiation established irradiation of two alkylbenzene alkylbenzene mamaterials. Figure Figure 16 16 compares compares these these results. results. The accuracy accuracy of calculations calculations of dosages terials. dosages error by a factor factor of 2 because because of uncertainty uncertainty of flux and sample sample position may be in error pOSition during during reactor irradiation irradiation test. test. However, reasonably reasonably good good agreement agreement of the results the reactor results was obtained. The relative relative stability stability of the two two materials materials was the same same for both types tained. types of exposure. exposure. This comparison comparison of the effects effects of electron reactor irradiations elecThis electron and reactor irradiations indicated indicated that that electron irradiations irradiations could be used to advantage advantage in studying studying damage to organic tron organic liquids. liquids. Screening of Organic Organic Liquids for Possible Possible Moderator Moderator Materials screening of Screening Materials - In the screening organic liquids liquids using 2Mev electrons, electrons, several several types of materials organic 2 - Mev materials were were tested. tested. These These consisted of hydrocarbons, hydrocarbons, ethers, ethers, ketones, ketones, alkylated structures, and consisted alkylated benzene benzene ring ring structures, alkylated naphthalene structures. Of Of these these materials materials evaluated, alkylated naphthalene structures. evaluated, the longer longer chain comcomwere found found to be less less radiation radiation stable stable than the shorter shorter or branched pounds were branched chain compounds. compounds. Tests of such alkylated alkylated benzene ring ring compounds as alkylbenzene alkylbenzene 250 and alkylbenzene Tests alkylbenzene 350 350 alkylbenzene 250 250 to be more more radiation radiation stable stable than alkylbenzene showed the alkylbenzene alkylbenzene 350 at temtemperatures in the range range from from 3000 3000 to 500 50000F. Since the napthalene peratures napthalene ring ring is is more more radiation radiation stable than the benzene ring,, a mixture mixture of amylnaphthalenes amylnaphthalenes was evaluated stable benzene ring evaluated for radiation radiation temperature stability. stability. The amylnapthalenes amylnapthalenes tested tested were di-, and and temperature were mixtures mixtures of mono-, mono -, di-, polyamylnaphthalene. Studies Studies were continued in finding a naphthalene polyamylnaphthalene. naphthalene ring ring having tempertemper-
0 106 3 x 106 3 x 107 107 1. 5 x 1088 0 1066 3.2 x 10 3.2 x 107 3.2x107 1088 1. 6 x 10 0 3.2 x 1066 3.2 x 1077 1. 6 x 1088 1064 1013 1013 959 959 965 965
-
-
d
-
d
0.0 0.0 0.615 0.615 1.47 1.47 2.49 2.49 0.68 0.68 0.61 0.79 0.79 1.45 1.45 0.08 0.08 0.12 0.24 0.24 0.84 0.84
0 1066 1.1 x 10 9.9 x 1066 9.9 6.8 6.8 x 107 107 0 107 1. 9 x 107 88 1.1 x 10 1.1 9 1 x 10 0 1. 9 x 1077 1.9x10 1.1 x 10 1088 1.1 6.4 x lOB lOB 6.4 1329 1329 1312 1312 838 838 212 212
-
-
d
-
d
0.08 0.08 0.16 0.16 0.64 0.64 3.06 3.06
-
0.3 0.3 0.28 0.28 0.48 0.48 32 1. 32 0.58 0.58 0.483 0.483 0.64 0.64
Radiation Gamma Radiation Viscosity, c Viscosity, Iodine Dosage, Number rads rads centistokes centistokes
0 8.4 8.4 x 107 107 1. 7 x 1088 2.5 x 1088 2.5 0 8.4 x 1077 8.4 1. 7 x 108 3.4 x 10 1088 3.4 0 8.4 x 1077 8.4 1. 7 x 10 8 2.5 x lOB lOB 2.5
1259 1259 1079 1079 843 843 615 615
-
d
-
-
d
dViscosity changes changes in benzene benzene and toluene toluene at the indicated indicated dosages dosages were were within the experimental experimental error error of measuremeasuredViscosity therefore were were not included. included. ment and therefore
0 2.2 2.2 3.25 4.60 4.60 0.51 0.90 0.90 1. 59 59 2.54 2.54 0.0 0.0 06 1. 06 2.86 2.86 4.2 4.2
Electron Radiation Radiationbb Electron Viscosity, c Viscosity, Dosage, Dosage, Iodine Number centistokes centistokes rads rads
aReactor and gamma gamma irradiation irradiation data have been reported previously in APEX 11. aReactor reported previously bElectron irradiation irradiation was made with 30-gram 30-gram samples samples in Van de Graaff electron beam. beam. Operating Operating conditions conditions of the bElectron Graaff electron Graaff were were 50 /-La /la at 2 Mev; Mev; the non-scattered non-scattered beam beam impinging impinging on the sample sample was 42 42 /-La. /la. Van de Graaff CAt6BOF CAt6BOF
Glycerine Glycerine
Toluene Toluene
Benzene Benzene
Material Material
Reactor Radiation Radiation Reactor Dosage, Viscosity, c Viscosity, Iodine Number rads rads ccentistokes entistokes Number
CHANGESIN ORGANICLIQUIDSIN REACTOR, GAMMA, GAMMA, AND AND ELECTRON IRRADIATIONSa IRRADIATIONSa CHANGES IN ORGANIC LIQUIDS IN REACTOR,
TABLE 7
~
c..:l
aDetermined at 40000F aDetermined bDetermined at 30000F bDetermined
Dosage, rads rads Dosage, NH NH NH/density NH/density ratio ratio Viscosity, Viscosity, centipoises centipoises at 10000F 0F 3000F 300 Evolution, Gas Evolution, liters/liter liters/liter Temperature of Temperature irradiation, OF OF irradiation, 400
500
111.4 111.4 0.889 0.889 42.0 42.0
18.1 1.44 1.44
51. 0 2.34 2.34
14.2 45 1. 45
6.1 6.1
4.28x109 9 4.28x10 5.1a 5.1a
Irradiated Irradiated
30.0 30.0
6.4 6.4
6.0 6.0
5.9 5.9
5.2a 5.2a
Original Original
4.28 x 1099 4.28 5.3bb 5.3
Irradiated Irradiated
Pentalene 195 195 Pentalene
4.8aa 4.8
Original Original
Pentalene 95 95 Pentalene
6.29 6.29 0.864 0.864
7.2 7.2
5.7bb 5.7
Original Original
300 500
39.1 2.34 2.34
5.5 5.5
4.86 x 109 4.86 5.0bb 5.0
24.6 24.6
3.12 3.12 0.634 0.634
5.6 5.6
4.8bb 4.8
Mixture Mixture Alkylbenzene 250 Alkylbenzene and Dowtherm-A Dowther m-A 1:1 by weight 1:1 Irradiated Irradiated Original Original
30.7 30.7
7.82 0.75 0.75
7.1 7.1
1.2 x 1099 1.2
Irradiated Irradiated
Alkylbenzene 250 Alkylbenzene
PHYSICAL PROPERTY PROPERTY CHANGES CHANGES OF ORGANIC ORGANICLIQUIDS EXPERIMENTAL PHYSICAL LIQUIDS WITH VAN VAN DE DE GRAAFF IRRADIATION IRRADIATION WITH
TABLE 8
r..:I
t.)
33
~------~------~--------r-------~-------'
800 ~------~------~--------~------~-------,
··
...-"•
~~
600
· c u
u: u." 0 0
8~
400
tt-
-c <
>ttv;
00 U U v>
:; :;
200
99 DOSAGE, 10 rads rads DOSAGE,
Fig. 16 - Comparison Comparison of reactor reactor and electron electron irradiation irradiation of two alkylbenzenes alkylbenzenes Fig.
ature stability stability to 60000 F. mixture of polyamylnaphthalenes polyamylnaphthalenes having a boiling boiling pOint point of 62500 FF ature F. A mixture having was tested tested for for radiation radiation stability. stability. was High Temperature, Temperature, Dosage Evaluations Evaluations of Some Some Feasible Feasible Moderators Moderators - Since Since the the High High Dosage reactor irradiation irradiation results obtained obtained previously previously on alkylbenzene alkylbenzene could could be duplicated duplicated by reactor results Graaff irradiation, irradiation, the Van de Graaff Graaff was was used used for for additional additional studies studies of organic organic Van de Graaff the liquids. liquids. take partial partial advantage advantage of the the higher higher NH* of alkylbenzene alkylbenzene 250 (5.4 (5.4 at at 45000 F) and the the To take F) and stability of Dowtherm-A, Dowtherm-A, mixture of equal equal parts parts of the the two materials was irradiated irradiated stability a mixture materials was in the Van de Graaff Graaff accelerator. accelerator. The NH of this this mixture mixture was was approximately approximately 4.3. Figure Figure 17 the The 4.3. compares the the gas gas evolution evolution from from alkylbenzene alkylbenzene 250, 250, from from Dowtherm-A, Dowtherm-A, from a mixmixcompares and from ture of equal equal parts parts of the the two liquids liquids as as a function LITR and Van de Graaff Graaff radiation radiation ture function of LITR 0F dosage. Figure 18 compares compares the the viscosity viscosity at at 1000 the three three liquids liquids as as a function function of dosage. Figure F of the dosage, and Figure Figure 19 compares compares the the viscosities viscosities at 300oF. The curves curves suggest suggest that that the the dosage, at F. The mixture is is more more promising promising than than alkylbenzene alkylbenzene 250 as as a possible possible moderator moderator liquid liquid since since mixture viscosity change change in the the mixture mixture is less by a factor factor of apprOXimately approximately viscosity is less 20 selected organic organic liquids liquids that that are are stable stable at at high high temperatures temperatures were evaluated evaluated using using Two selected were -Mev electrons electrons from from the the Van de Graaff Graaff accelerator. accelerator. The liquids liquids are are mixtures mixtures of mono-, mono-, 2 -Mev The di-, and and polyamylnaphthalenes polyamylnaphthalenes are commercially commercially as Pentalene Pentalene di-, and are known as Pentalene 95 and Pentalene The Pentalene Pentalene 95 is is an undistilled undistilled mixture, mixture, whereas whereas the the Pentalene Pentalene 195 is is a distilled distilled 195. The mixture of amylnaphthalenes. amylnaphthalenes. Since the the naphthalene naphthalene ring ring is is more more stable stable to radiation radiation than than mixture Since the benzene benzene ring, ring, the the Pentalenes Pentalenes should should be quite quite radiation radiation stable. stable. the Experimental data obtained obtained from from the the electron electron irradiation irradiation these organic organic materials materials are are Experimental data of these given in Table Table 8. Gas Gas evolution evolution and changes changes of viscosity viscosity measured measured at at 10000 FF and 30000 FF are are given graphically compared compared in Figures Figures 20, 21, respectively. graphically 21, and 22 respectively. Pentalene 95 showed showed damage damage comparable comparable to that that of the weight mixture mixture of alkylalkylPentalene the 1: 1 by weight benzene 250 and Dowtherm-A. Dowtherm-A. The viscosity viscosity increase increase of Pentalene Pentalene 195 was was greater greater than than benzene The *N
-
H -
hydrogen atoms atoms/cc number cf hydrogen / cc atoms/cccc 10 22 hydrogen atoms/
34
so 80
.., -e
10
'0 '0
60
';'s .2' .2"
ALKTLBENZENE
,~ ~
250
1/
VAN DE1¥GRAAFF
') ';i 8.8.
50
.
'0
V
40
~ ~
7:
z00
VI
MIXTURE,
-'
VV
~NDEGRAAFF
20
'"< < o
V>
"
10
250 AND
DOWTHERM-A
30
i= ::> -' 00 > > w
(1,1 BY WEIGHT)
ALKYLBENZENE
/
I~
V
V
- .-
V
OOWTHERM-A
~
LITR~
7
9
DOSAGE, 10 rads rads DOSAGE,
Fig Gas evolution Fig. . 17 - Gas evolution from alkylbenzene alkylbenzene 250, 250, Dowtherm-A, Dowt herrn-A, and a mixture mixture of of alkyl alkyl benzene benzene 250 and Dowtherm-A Dowtherrn-A as as functions functions of LITR LITR and and Graaff radiation radiation Van de Graaff
MIXTURE, (1 :1 BY IGHT) MIXTURE, (U BY WE WEIGHT)
r---,----,----~--~
60 . 6o · r----n----~----~--~ALKY L BE~ZENE250A~D 70.5 CS.1 ALKYLBEI>IZENE 250 A"ID ALKYLBENZENE
··
.,.-"• ;;
· c u
SO ~o
I ---
I
250
I
DOWTI-I EFlM-A DOWTH EIlM-A
I
VAN DE GRAAFF'
I 1
-
40
u.: u. o0
~ ~ 0
30
I-
-c < >l-
l-
v; o0
V>
~ ~
20 ~---+----~----+---,L~--.-+~~-+--~
:; ;:
10
o0 L -__ o0
~
____L-__~____- ' -____L-__~__---'
9 9 nOSAGE, ['lOSAGE, 10 rads rads
Fig. 18 - Viscosity Viscosity at lOOoF of alkylbenzene alkylbenzene 250, Dowtherm-<\ Dowtherm-A, , and a Fig. at 250, mixture mixture of alkyl alkyl benzene benzene 250 and Dowtherm-A Dowtherm-A as as functions functions of of LITR and Van de de Graaff Graaff radiation radiation LITR
35 35
6
··
5
-•j
1
· •
.~ .~
ALKYLBENZENE 250 ALKYLBENZENE
4
II
u
IGHT) VMIXTURE, BY WE IGHT) VMIXTURE, (1:1 BY
VAN V AN DE DE GRA~ GRAA:I'
11.!L' 0o
..,g
0 o 0
ALKYL 250 AND ALKYL BENZENE BENZENE AND DOWTHERM-A DOWTHERM·A
tf-
< >t-
/ ./
f-
v; in 0o
V V
/V
~ ~
VAN I/GRAiFF D/GRAjFF VAN
'\
~ ~
LlTR LITR
_/ / I---~ ~~ERM-A
u u
V>
:; :;
~
~ ~ oo oo
/
»> ~ERM'A
I--~ ~
4
2
55
7
9 DOSAGE, DOSAGE, 10 rods rads
Fig. 19 - Viscosity Viscosity 30000FF of alkylbenzene alkylbenzene 250, Dowtherm-A, Dowtherm-A, and a Fig. at 300 250, mixture of of alkylbenzene alkylbenzene and Dowtherm-A Dowtherrn-A as as functions functions of mixture 250 and LITR and Van Van de Graaff Graaff radiation radiation LITR and
60
..,-e., 's ~
50
'0
.~ 40 .~
..
";i ';i 00
'0
~
~
;;
30
:i
00
i= ::>
20
...J -' 00
MIXTURE,
> w w
'" '" < <
"o
(1:1 BY WEIGHT)
ALKYLBENZENE AND ALKYLBENZENE 250 AND
10 t---f-7"E-/-'-----~r-::---+--t--f-7"E:r'----::;;ooI""'---+--DOWTHERM·A DOWTHERM-A
0 0
3
4
5
9 DOSAGE, 10 rods rods DOSAGE,
Fig. 20 - Gas Gas evolution evolution from alkylbenzene alkylbenzene 250, 250, a mixture mixture of alkylbenzene alkylbenzene Fig. and Dowtherm-A, Dowtherm-A, Pentalene Pentalene 95, and Pentalene Pentalene 195 as as functions functions and Graaff radiation radiation of Van de Graaff
36
120 120 //
.
M M
-"• ~~
.>t
100 100
ce
•u u
u.u.-
80
00 C> C>
!? !2 I-
-c < >lv;
60
00
U U V) V)
;; s
40
!:! ~ II-c < :J; :20 w w
z "
~
20
MIXTURE, (1: 1 IlY WEIGHT) A LK YL BENZ ENE 250 AND
1f-'7~-+-----17L---+----,7"''-1
ALKYL BENZENE 250 AND DOWTHERM-A DOWTHERM-A
00 00
2
4
3 99
DOSAGE, DOSAGE, 10 rad. rad.
Fig. Kinematic viscosity Fig. 2121- Kinematic viscosity at at lOOoF 1000F of of alkylbenzene alkylbenzene 250, 250, a mixture mixture of alkylbenzene 250 and Dowtherm-A, 95, and Pentaalkylbenzene Dowtherm-A, Pentalene Pentalene Pentalene 195 as lene as functions functions of of Van Van de de Graaff Graaff radiation radiation
4
M M
::
'0 a. ce ~
~
u.0 0 C> C> C> C> M M
I-
MIXTURE,
-e <
>>v;
,
ll-
\\
00
u u V)
(1:1 BY WEIGHT)
ALKYL 250 ALKYL BENZENE BENZENE 250 AND AND DOWTHERM·A DOWTHERM·A
V)
;; s
0
4
0
5
99 DOSAGE, 10 rads DOSAGE, rods
Fig. Fig. 22 - Absolute Absolute viscosity viscosity at at 30000 FF of alkyl alkyl benzene benzene 250, 250, a mixture mixture of alky.lbenzene 250 and Dowtherm-A, Dowtherm-A, Pentalene Pentalene 95, and PentaPentaalky.lbenzene 95, lene lene 195 as as functions functions of of Van de Graaff Graaff radiation radiation
37 37
60.-------.-------,--------r-------,--------.-------~------~
60.-------.-------,--------r-------,--------.-------,-------~
,,
50r-------+--------r-------+----~-1--------r-------+_------~ sOr-------+--------r-------+----~-1--------r-------~------~
--
-v 40 40~------+-------~--~~~----- ....'v «:.•..'" 'v' .~ i)1:>
~"V ~"V
~ ~ ;;i ~ 0
~ ::> :>
~'<; ~t,; .;.."'"
*-",,'V
~....,*"
30 f--______-t-_____ ""'VrF-____---7"1-_
30
~ ..J ~
o0 > > ur UJ
'" '" «-c (!)
o
20
20
I-----I~h._10 ~--_I~he_-
o~------~-------L------~------~--------~------~------~
o~------~-------L------~------~--------~------~------~ 4 oo 7 9 rads DOSAGE, 10 rads
Fig. 23 - Gas Gas evolution evolution from aalkylbenzene 250, Pentalene Pentalene 195, number Fig. lkylbenzene 250, 195, number 290,, and a mixture mixture of alkylbenzene alkylbenzene 290 250 and Dowtherm-A Dowtherm-A as as functions of Van de Graaff Graaff radiation radiation functions
Pentalene 95 95 by a factor factor of 2 at 100 1000oF; however, however, at 30000F the viscosity that of Pentalene viscosity of PentaPenta195 was less less than that that of Pentalene Pentalene 95 95 by a factor factor of approximately approximately 3. lene 195 materials that can be used used at temperatures temperatures up to 60000F has necessitated The need for materials necessitated irradiation studies studies of many new high temperature temperature organic organic liquids. liquids. Pentalene 195 was disirradiation Pentalene 195 distilled at 625 62500F so that the lower lower boiling boiling fractions fractions from from the original original material tilled material were were removed. removed. residue, termed termed number number 290, had an initial initial boiling boiling point point of 625 The residue, 625 00F. F. This This liquid was irradiated at 60000F in the Van Van de Graaff Graaff accelerator accelerator to determine determine the pertinent irradiated pertinent physical physical property changes electron radiation. radiation. The NH property changes as a function of 2-Mev erectron NH of number number 290 at the operating liquid moderator moderator temperature temperature of 60000F is 4.5 4.5 and is operating is comparable comparable to that that of alalkylbenzene 250 (NH (NH = = 4.8) 4.8) and water water (NH (NH = = 4.5) 4.5) at this this temperature. temperature. At a temperature kylbenzene temperature of 40000F, at which the main bulk of the shield shield liquid would would be operating, 400 operating, the NH NH of Pentalene Pentalene 5.06, that of alkylbenzene alkylbenzene 250 is is 5.4, 5.4, and that that of water water is 5.7. 290 is 5.06, is 5.7. Experimental data obtained obtained from the Van de Graaff Graaff electron electron irradiations Experimental irradiations of number number 290 are Table 9. Vi&cosities Viacoaities measured measured at 100 10000F and 30000F, and gas are given in Table gas evolution evolution are are compared in Figures Figures 23, 24, and 25 with those those of alkylbenzene alkylbenzene 250, Pentalene compared Pentalene 195, and mixture (by (by weight) of alkylbenzene alkylbenzene 250 and Dowtherm-A Dowtherm-A as functions the 50:50 mixture functions of radiradidosage. Figure Figure 26 is a plot of viscosity viscosity increase increase of number number 290 at 60000F as a funcation dosage. Van de Graaff Graaff radiation radiation dosage. dosage. tion of Van detailed study of Figures Figures 23, 24, 25, and 26 26 reveals reveals that that the evolution from A detailed evolution of gas from number 290 under under irradiation irradiation is less less than that that from from Pentalene Pentalene 195 195 or alkylbenzene nurr;.ber alkylbenzene 250. viscosity measured lOOoF of non-irradiated non-irradiated and irradiated irradiated 290 is The viscosity measured at lOOoF is higher higher than the
38
,,
r---------~--------~--------~--------~--------_r--------~--------~
800 BOO r---------~--------~--------~--------_r--------_r--------~--------~
I
.~ ~
•
~------~r_------~--------_+--------_r--------1_------~~_1----~
700 700
~------~r_------~--------_+--------_r--------1_--------J__I----~
600 600
~--------+_--------1_--------4_--------_r--------_+------~_I--------~
~--------+_--------1_--------1_--------_r--------_+------~~--------~
500 500
·0
0. 0.
C
~
~
!L0 0
0 0
:=
400 400
II-
«
>-
l-
v;
00 U U ~
~ >
300 300
OPERATING
200 200
~--------+_--------4_--------~~~----_r----_J~_+--------_+--------~
~--------+_--------1---------~~~-----r-----I~-r---------+--------~
100~--~-----+----------~--------~-100~--~----4_--------_r---------r--MIXTURE
(1:1 BY WEIGHT)
ALKYLBENZENE ALKYLBENZENE 250 250 AND AND DOWTHERM-A DOWTHERM·A
oo
7
99 DOSAGE, 10 10 ,ods reds DOSAGE,
Fig. . 24 - Absolute Absolute viscosity viscosity at lOOoF of number 195,, Fig at number 290, 290, Pentalene Pentalene 195 alkylbenzene 250, and a mixture mixture of alkylbenzene and Dowalkylbenzene 250, alkylbenzene 250 and Dow· therrn-A as as functions functions of Van de Graaff Graaff radiation therm·A radiation
39
~------~--------~---------r--~----~--------~--------~------~
2.4 2.4 ~------~--------~---------r--~----~--------~--------~------~
2.0 2.0
···
• -t~= ••uc
'0 '0
1.6 1.6
u
IL00
8 ..,8 •... -c -< >•... I-
1.2 1.2
I-
;;;
00 U U
:; '"'"s
0.8
~--------~-------+---------+--------~--------+---------+--------4
0.4 ~--------~-------+--------~--------~--------+---------+--------4 0.4
L~---- __ __~ ~------~~------~------~------~ oo L-______ ~---~______~------~--------~------~------~ 4 5 6 oo 7 9 rod. DOSAGE, 10 rad.
Fig. 25 - Absolute Absolute viscosity viscosity at 300 30000FF of nU!llber number 290, 290, Pentalene Pentalene 195, Fig. at 195, alkylbenzene 250, and a mixture mixture of alkylbenzene alkylbenzene 250 and and Dowalkylbenzene 250, therm-A as as functions functions of Van de Graaff Graaff radiation radiation therm-A
• 40 40
0.5
.::
0.4 0.4
OPERATING TEMPERATURE, TEMPERATURE, 600°F 600°F OPERATING
·0 ·0
... .~
.;:: e 0
~ ~
,.:1'.-
0.3 0.3
--
°0
..,8-c ... t< >... !::
;;; on
I"
0.2 0.2
-
~ ~
00 U U
V V
~ I---NUMBER 290 ~ ~UMBER290
-
0
~ ~
~ ~
> >
0.1
oo
oo
2
6
5
4
3
7
9 ,od. DOSAGE, 10 rod.
Fig. Absolute viscosity at function of Fig. 26 - Absol ute viscosity at 60000F of number 290 as a function Graaff radiation radiation Van de Graaff
...•..
1.0 L/ 1.0 v U
00
r--....
O~ O~ r---,..
---
----
-e.;...
00
. '"'" .., . ..,..,
..,. ..,e
<, .....
~ ~
00
0.8 0.8
0 -0
00 00
0.6 0.6
•
00
.., ..... ..,<,
0.4 0.4
00
h
-.L= -L= h
Ratio of eo eo Iculated Iculated heat heat tronsfer tronsfer coefficients coefficients Ratio
o{ o{ irradiated irradiated to unirradiated unirrodiated olkylbenzene olkylbenzene 250
u
Ratio of experimentally experimentally determined heottransf.r heottransf.r Ratio determined h --.!..::Z coefficient coefficient of irradiated irradiated to the the calculated calculated -...!..:Z h coefficient of unirrodiated unirrodiated alkylbenzene alkylbenzene 250 250 coefficient u
0.2 0.2
oo
oo
0.2 0.2
0.4 0.4
0.6
1.0
0.8 0.8
FAST NEUTRON NEUTRON DOSAGE, DOSAGE, 10 FAST
18
1.2 1.2
2 n/
Fig. 27 - Comparison Comparison of the the ratio ratio he he/hu the ratio ratio h/ h/huhu versus versus fast fast Fig. / hu to the neutron dosage dosage neutron
1.4 1.4
41 41 TABLE 9
or
PHYSICAL PROPERTY PROPERTY CHANGES CHANGESOJ;" EXPERIMENTAL PHYSICAL NUMBER 290 WITH WITH VAN VAN DE GRAAFF IRRADIATION IRRADIATION . NUMBER Original Original
6.5 6.5 x 109
Dosage, rads rads Dosage, NH value value at: NH
Irradiated Irradiated .
6.4 6.4 5.3 5.3 4.5 4.5
100°F 100°F 300°F 300°F 6000F
Density, grams grams/cc Density, / cc at: 100°F 3000F 600°F 600°F
0.956 0.956 . 0.878 0.878 0.750 0.750
0.919 0.919 0.835 0.713 0.713
Viscosity, centipoises centipoises at: Viscosity, 100°F 100°F 300°F 300°F 600°F 600°F
87.5 87.5 0.74 0.74 0.22
7?6.4 7?6.4 1.55 1.55 0.36 0.36
evolution, liters/liter liters/liter Gas evolution,
46.6 46.6
point, of of Boiling point,
625 625
670
Temperature of irradiation, irradiation, of of Temperature
600
10 TABLE 10 EFFECT OF IRRADIATION IRRADIATIONONTHE EFFECT ON THE HEAT TRANSFER CHARACTERISTICS OF ALKYLBENZENE 250 CHARACTERISTICS Fast Neutron Neutron Fast Dosage, Dosage, fn/cm fn/cm22
oo (Control)
16 5.6 x 1016 5.6 17 1. 65 x 10 1.65 10 17 17 2.57 x 10 1017 2.57 17 3.71 x 1017 17 5.65x 10 1017 5.65x 17 6.78 6.78 x 10 1017 17 1 9.09 x 10 10 7 9.09 9.93x101717 9.93x10 18 09 x 10 1018 1. 09 18 1.24 1018 1. 24 x 10 1.29 x 1018 1018 1.29 18 34 x 10 1018 1. 34
Density Density P ), (P Ib/ft3 Ib/ft3 45.5 45.5 45.7 45.7 45.9 45.9 46.1 46.4 46.4 46.8 46.8 47.0 47.0 47.4 47.4 47.6 47.6 47.8 47.8 48.1 48.1 48.2 48.2 48.2
hu
hi
h/hu hi/hu
he
he/hu he/hu
a (eat ceat Balance Balance' Q1 - Q2) Q2) 1009t Q1 Q1 0 Q1 0
228 231 231 230 223 223 226 226 228 235 235 223 223 242 242 233 232 232 231 231
235 235 236 236 230 217 217 210 207 207 205 205 191 191 205 192 192 190 191 191
1.0 1.0 1. 03 03 1. 02 02 1.0 1.0 0.973 0.973 0.924 0.924 0.908 0.908 0.871 0.858 0.858 0.847 0.826 0.820 0.820 0.815
227 227 224 221 221 212 212 210 190 190 195 195 187 187 189 189 186 186 162 162 172 172
0.99 0.99 0.97 0.97 0.96 0.96 0.95· 0.95 · 0.93 0.93 0.83 0.83 0.83 0.83 0.84 0.84 0.78 0.78 0.80 0.80 0.70 0.70 0.75 0.75
+3 +3 +3 +3 +3 +3 +3 +3 +2 +2 -8 -4 -4 -15 -6 -20 -23
Viscosity Viscosity (( J1 )) , lb/ft-hr lb/ft-hr
09 1. 09 01 1. 01 1. 04 04 1. 09 09 1.17 1.17 31 1. 31 39 1. 39 1. 54 54 1.60 1.60 1.66 1.66 76 1. 76 79 1. 79 1.82
Temperature = = 450°F 450°F Temperature Average Velocity Velocity ~ ';t 2fps Average aQ1 = = Electrical Electrical power power input; Q2 Q2 aQl thermocouple readings. readings. thermocouple
= WC WCpp ~T =
determined from as determined from measured measured flow flow and
42 42 viscosities viscosities of the three three other other liquids liquids studied. studied. However, the viscosity viscosity of 290 is lower than the viscosities viscosities of the alkylbenzene alkylbenzene liquids liquids after after initial initial irradiation irradiation when when measured measured at temtemperatures peratures ab0ve above 300 300o0F. A preliminary infrared absorption survey of the infrared absorption spectrum spectrum of the irradiated irradiated number number 290 preliminary survey indicated that no unsaturation unsaturation was present indicated that present in the sample. sample. This This was later later confirmed confirmed by a bromine number number determination. determination. The spectrum spectrum indicated indicated further further that that the functional functional groups groups bromine appeared appeared to be unaffected unaffected by irradiation irradiation except except for a slight slight change to the 2-mono-substi2-mono-substituted naphthalene. naphthalene. Analysis of of Heat Transfer Transfer Data Analysts
The heat transfer transfer coefficient coefficient of alkylbenzene alkylbenzene 250 was evaluated evaluated using the following rerelation: lation: h
0.8 ( 0.8
=A ~ ~ ( ~G ~G = )
~/l ~/l
) 0.4 0.4
where = = heat heat transfer transfer coefficient coefficient = tube inside inside diameter diameter = = fluid mass mass velocity velocity = = fluid specific specific heat heat /l = = fluid viscosity viscosity thermal conductivity conductivity K = fluid thermal A = constant constant
h D G Cp
Btu / hr-ft2 _oF Btu/hr-ft2_o F ft Ib / ft2-hr Ib/ft2 -hr Btu / lb-oF Btu/lb-oF lb / ft-hr Ib/tt-hr Btu/hr-ft-OF Btu/hr-ft-OF
Values of the heat heat transfer transfer coefficient coefficient h were were determined determined for the unirradiated unirradiated and irradiated irradiated liquid throughout throughout the heat transfer transfer test test described described earlier earlier in this this report. report. Ratios of the heat transfer transfer coefficients coefficients of the irradiated irradiated liquid hi to the unirradiated unirradiated Ratios liquid hu hu were were computed and are are shown in Table Table 10. Values for the experimentally experimentally determined determined heat heat transfer transfer coefficient coefficient he were were determined determined using the relation: relation:
where where Q = heat dissipated dissipated in test test section section AH AH = heated heated surface surface to test test section section f:.. TM= TM = mean wall-to-liquid wall-to-liquid temperature temperature difference difference in the test test section. section. /). The ratio / hu, based ratio he he/hu, based on experimental experimental values, values, shows a cumulative cumulative effect effect of fouling and viscosity on the heat heat transfer transfer coefficient. coefficient. viscosity Values of he and the ratio ratio are are given in Table Table 10. Figure / hu ratios Figure 27 27 is a plot of the hi/h hi/huu and he he/hu ratios as a function of fast fast neutron neutron dosage. dosage. A study of the curves curves indicates indicates that there there is no serious serious degradation degradation of the heat transfer transfer coefcoef18 n/cm ficient of alkylbenzene alkylbenzene 250 for fast fast neutron neutron dosages dosages up to 1. 4 x 1018 n/cm22• . The data ficient indicate that that the heat heat transfer transfer coefficient coefficient was decreased decreased by irradiation irradiation to approximately approximately indicate 18 fast 80 percent percent of the unirradiated unirradiated value when when subjected subjected to a dosage dosage of 1. 4 x 1018 fast 2•2 . neutrons / cm neutrons/cm
