. * rii i i i . . . : . i I OFT ORNL P 3189 11 ST ..--. . . , rej, 1 cm . . . 1 ' : . dos 11:25 114 11.6 MICROCOPY RESOLUTION TEST CHART NATIONAL BUREAU OF STANDARDS-1963 4 i * ** HT M ORNL 2318 Con*- 6707145 Ciwan 30 $3.00, ww.65 ACTID H: S M .G CONSEQUENCES OF INTERNAL HEAT FLOW IN RADIOISOTOPE HEAT SOURCES* LEGAL NOTICE AUG 22 1967 J. C. Posey Isotopes Development Center Oak Ridge National Laboratory Post Office Box X Oak Ridge, Tennessee 37830 This raport me 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, expressed or implied, with respect to the accu- racy, completeness, or usefulness of the information coatined in this roport, or that the use of any information, apparatus, method, or process disclosed in this repor may not Infringe privately owned righto; or B. Assumro any liabilities with respect to the use of, or for damages rcouting from the use of any information, apparatus, method, or process disclosed in this report. As used in the above, "por son acting on behalf of the Commission" includes any em- ployee or contractor of the Commission, or employee of such contractor, to the extent that such employee or contractor of the Commission, or employee of such contractor prepares, illo seminates, or provides access to, any information purevant to his employment or contract with the Commission, or his employment with such contractor. ABSTRACT from the heat source and the size of some sources are limited by the maximum a lowable internal temperature. Equations relating the maximum internal tempera- tures of various-shaped fuel forms and other source parameters are given. By using calculated results, the use of cerniets is compared with the use of oxide-metal laminar structures as methods of decreasing the resistance to heat flow in the interior of heat sources and achieving higher sur- face heat fluxes without exceeding maximum allow- ab.le internal temperatures. The laminar composite fuel form is moderately superior. This report gives basic equations for the predic- tion of these limitations for simple cases. It is shown that the maximum available surface heat flux can be increased by the use of cermets or laminar metal structures when radioisotope compounds of poor thermal conductivity are used. The expected vapor pbase migration and equilibrium distrivution of a volatile radioactive fuel inside a heat source capsule is described. Redistribu- tion does not always result in serious problems and can reduce the cost of source fabrication. The existence of temperature differences within the capsule also leads to volatile transfer of radio- active material. The factors which determine the equilibrium distribution of the material ere dis- cussed, and a mathematical analysis is given for a simple case. EQUATIONS FOR FUEL FORMS OF SIMPLE GEOMETRIC SHAPE INTRODUCTION A radioisotope heat source is generally considered to consist of a quantity of radioactive fuel and its container. The radioactive fuel can be in the form of a single compound of the radioisotope, or it can be associated with a matrix material of better thermal conductivity. Equations relating the difference between the sur- face temperature and the maximum internal tempera- ture to various parameters for fuel forms of simple geometric shapes are given in Table 1. The symbols used in the equations are defined as follows: AT = difference between the maximum allowable internal temperature and the surface temperature, P = power density (rate of heat generation per unit volume) of the fuel, Large temperature differences can exist between the suriace and the interior of the radioactive fuel (defined as the radioactive material with or without a diluent or matrix material) in heat sources. These gradients are created by the flow of heat, which is generated throughout the radio- active material, to the surface. Very high inter- nal temperatures can result. h = distance from surface to plane of maximum temperature in a planar fuel form, k = thermal conductivity of the fuel, q = total rate of heat production by the source, There are no specific rules for setting the maxi- mum allowable internal temperature for a heat, source. It must be set on the basis of the prop- erties and use of the particular source. The melting point of the fuel has often been set as the maximum allowable temperature. Certainly, melting can in some cases result in a volume change which can Qamage the source. In other cases, it can ai.low an undesirable movement of A = surface area through which heat leaves the fuel form, D = diameter of a cylindrical or spherical fuel form, .. .. .. - TI J. C. Posey Isotopes Development Center Oak Ridge National Laboratory Post Office Box X Oak Ridge, Tennessee 37830 Huwa ROT London States, nor the Commission, nor any person acting on betalt of the Commission: A. Makes my warranty or ropresentation, expressed or implied, with respect to the accu- racy, complotoners, or wrotulnost of the laformadon contained in this roport, or was the wo of any information, apparatus, morbod, or process disclosed lo this romi may not infrico privately owned righta; or B. Assumos any liabilities with respect to the use of, or for damages resulting from the use of any information, apparatus, wethod, or 0. OCOss disclosed in this roport. As usod in the above, "por son acting on behalf of the Commission" includes any 60- ployoo or contractor of the Commission, or omployee of such contractor, to the extent that such omployee or contractor of the Commission, or ployee of such contractor prepares, disseminates, or provides access to, any information pursuant to bilo employment or contract with the Commission, or his employment with such contractor. ABSTRACT from the heat source and the size of some sources are limited by the maximum allowable internal temperature. Equations relating the maximum internal tempera- tures of various-shaped fuel forms and other. source parameters are given. By using calculated results, the use of cermets is compared with the use of oxide-metal laminar structures as methods of decreasing the resistance to heat flow in the interior of heat sources and achieving higher sur- face heat fluxes without exceeding maximum allow- ab.le internal temperatures. The laminar composite fuel form is moderately superior. This report gives basic equations for the predic- tion of these limitations for simple cases. It is shown that the maximum available surface heat flux can be increased by the use of cermets or laminar metal structures when radioisotope compounds of poor thermal conductivity are used. The expected vapor phase migration and equilibrium distribution of a volatile radioactive fuel inside a heat source capsule is describea. Redistribu- tion does not always result in serious problems and can reduce the cost of source abrication. The existence of temperature dil'ferences within the capsule also leads to volatile transfer of radio- active material. The factors which determine the equilibriun distribution of the material are dis- cussed, and a mathematical analysis 18 given for a simple case. EQUATIONS FOR FUEL FORMS OF SIMPLE GEOMETRIC SHAPE INTRODUCTION A radioisotope heat source is generally considered to consist of a quantity of radioactive fuel and its container. The radioautive fuel can be in the form of a single compound of the radioisotope, or it can be associated wita a matrix material of better thermal conductivity. Equations relating the difference between the sur- face temperature and the maximum internal tempera- ture to various parameters for fuel forms of simple geometric shapes are given in Table 1. The symbols used in the equations are defined as follows: AT = difference between the maximum allcwable internal temperature and the surface temperature - P = power density (rate of neat generation per unit volume) of the fuel, Large temperature differences can exist between the surisce and the interior of the radioactive friel (defined as the radioactive material with or without a diluent or matrix material) in heat sources. These gradients are created by the flow of heat, which is generated throughout the radio- active material, to the surface. Very high inter- nal temperatures can result. h = distance from surface to plane of maximum temperature in a planar fuel form, k = thermal conductivity of the fuel, q = total rate of heat production by the source, A = surface area through which heat leaves the fuel form, There are no specific rules for setting the maxi- mum ai.lowable internal temperature for a heat source. It must be set on the basis of the prop- erties and use of the particular source. The melting point of the fuel has often been set as the maximum allowable temperature. Certainly, melting can in some cases result in a volume change which can damage the source. In other cases, it can allow an undesirable movement of material within the capsule. However, in other applications, melting in the interior of the radioactive mass of material does no barm. The maximum surface heat flux which can be obtained D = diameter of a cylindrical or spherical fuel form, 1 = length of a cylindrical fuel form, q/A = surface heat flux. *Research sponsored by the U. S. Atomic Energy Commission under contract with the Union Carbide Corporation. DISTRIBUTION OF THIS DOCUMENI S UNDIALULUI per These equations were derived under the assumption that P and k are constant throughout the fuel and that the surface temperature is constant. Heat losses from the edges of planar fuel fcrus and from the ends of cylindrical fuel forms are neglected. It can be seen that the maximum heat output of a spherical fuel form is limited by ATmax, The total power is not limited for flat or cylindrical fuel forms since the area or length respectively can be increased. The surface heat flux, q/A, is limited for all fuel forms. Table 2 gives the maximum surface heat flux for fuel forms composed of an optimum laminar combina- tion of tungsten metal and various radioactive materials. These data were calculated using the thermal conductivity of Jun and Hoch(4) for tung- sten. Power densities were taken from references 5 and 6. · The thermal conductivities of the radio- active materials were all assuned to be 0.03 watt/cm°c. This value has little influence on the thermal conductivity of the composite fuel and exact values for many radioactive materials are not obtainable at the temperatures under considera- tion. The value of ATmax is determined by the application in which the source is useä as well as ty the na- ture of the fuel materials. The surface tempera- ture of the source is an important design parameter in such applications as thermionic and thermo- electric generators and is set in the design of the equipment. Since the required surface tempera- ture may be quite high, ATmax will be seriously restricted unless the melting point of the fuel material is very high or interior melting is allowed. The proportional increase in the maximum surface heat flux of a laninar composite fuel form as com- pared to a pure radioactive material fuel form depends on the relative thermal conductivities of the metal and radioactive material. As an example, an increase of 3.5 fold could be achieved with a fuel of strontium oxide in combination with tung- sten while an increase of only 2.9 fold could be achieved with one of curium sesquioxide and tung- sten. This calculation assuues thernal conduc.. tivities of 0.02 and 0.03 watt/cm °C, respectively, for the oxides. The value for strontium oxide was obtained from E. E. Ketchen and that for curium sesquioxide was estimated. The maximum curface beat flux is an important parameter in certain beat source applications. It has been a limiting factor in the design of thermi- onic generating units. These units require a high heat flux delivered at a high temperature. The“ surface temperature of the fuel must be at least a little greater than the temperature at which the heat is delivered. THE EFFECTS OF VOLATILITY IN THERMIONIC HEAT SOURCES It can be seen that the maximum surface heat flux, 9/A, is proportional to (KP)1/2. Consequently, high thermal conductivity and high power density are desirable, There are limited data which indicate that certain radioactive fuels are moderately volatile under the proposed conditions of use. Consequently, there has been concern that these materials may leave the desired location by volatile transfer to other parts of the capsule. IMPROVEMENT OF THE THERMAL PROPERTIES OF HEAT SOURCES TE . . . . It will be shown that this volatility will cause no severe probleins with regard to the heat flow characteristics of a well designed source form and that volatile transfer will, in fact, tend to create a distribution of radioactive material with- in the capsule similar to the ideal distribution regardless of the initial physical form of the radioactive material. However, this does not pre- clude other problems caused by volatility such as the plugging of helium vents. The product KP can be improved for fuel of poor thermal condutivit bestibo addition of a metal of high conductivity. This can be cone in two ways: . (1) a cermet can be produced, drià (2) oriented conductors of metal can be introduced into the body of the radioactive material. .! Ei The effectiveness of these methods in increasing the thermal conductivity is shown by the calculated curves in Figure 1. These curves assume that the thermal conductivity of the radioactive material is very small compared to that of the metal. Both phases are assumed to be 100% dense. The thermai conductivity of the ceimets was calculated using three different equations to chosen from the many that various people have derived for the con- ductivity of aggregates. The oriented conductors give moderately better results. Recognition of this phenomenon can lead to a worth- while reduction in the cost of fabrication of many sources. The material can be encapsulated as a loose powder instead of as a fabricated form. It will distribute itself in approximately the desired manner. Figure 2 is a chart which aids in the rapid calcu- lation of KP for any coübination of a highly con- ducting metal and a poorly conducting radioactive material providing the values of k and P for the Figure 3-B shows a thermionic heat source which is typical of many proposed designs. The useful heat flow leaves through one end of the cylindrical container, The rest of the container is assumed to be insulated so as to reduce extraneous heat losses to a low level. The radioactive material is attached to the inner surface of the cylinder at the end from which the useful heat flow passes. a . :: . ::* * : ---- It can be seen that the maximum heat output of a spherical fuel form is limited by ATmax. The total power is not limited for flat or cylindrical fuel forms since the area or length respective.ly can be increased. The surface heat flux, q/A, is limited 5 and ú. The thermal conductivities of the radio- active materials were all assumed to be 0.03 watt/cm °C. This value has little influence on the thermal conductivity of the composite fuel and exact values for many radioactive materials are not obtainable at the temperatures under considera- tion. The proportional increase in the maximum surface heat flux of a laminar composite fuel form as com- pared to a pure radioactive material fuel form depends on the relative thermal conductivities of The value of ATmay is determined by the application in which the source is used as well as by the na- ture of the fuel materials. The surface tempera- ture of the source is an important design parameter in such applications as thermionic and thermo- electric generators and is set in the design of the equipment. Since the required surface tempera- ture may be quite high, ATmax will be seriously restricted unless the melting point of the fiel material is very high or interior melting is allowed. an increase of 3.5 fold could be achieved with a fuel of strontium oxide in combination with tung- sten while an increase of only 2.9 fold could be achieved with one of curium sesquioxide and tung- sten. This calculation assumes thermal conduc- tivities of 0.02 and 0.03 watt/cm °C, respectively, for the oxides. The value for strontium oxide was obtained from E. E. Ketchen (T) and that for curiwn sesquioxide was estimated. The maximum surface beat flux is an important parameter in certain heat source applications. It has been a limiting factor in the design of thermi- onic generating units. These units require a high beat flux delivered at a high temperature. The“ surface temperature of the fuel must be at least a little greater than the temperature at which the heat is delivered. THE EFFECTS OF VOLATILITY IN THERMIONIC HEAT SOURCES There are limited data which indicate that certain It can be seen that the maximum surface heat flux, q/A, is proportional to (kP)2/2. Consequently, high thermal conductivity and high power density are desirable. the proposed conditions of use. Consequently, there has been concern that these materials may leave the desired location by volatile transfer to other parts of the capsule. TMPROVEMENT OF THE THERMAL PROPERTIES OF HEAT SOURCES p U : It will be shown that this vclatility will cause no severe problems with regard to the heat flow characteristics of a well designed source form and that volatile transfer will, in fact, tend to create a distribution of radioactive material with- in the capsule similar to the ideal distrivution regardless of the initial physical form of the radioactive material. However, this does not pre- clude other problems caused by volatility such as the plugging of helium vents. ++ +2 I aht: V 1.. A ?",-* .. ..*. * *76... . . . . The product KP can be improved for fuel of poor thermal conduntivi da tela. Addition of a metal of high conductivity. This can be done in two ways:: (1) a cermet can be produced, and (2) oriented conductors of metal can be introduced into the body of the radioactive material. . The effectiveness of these methods in increasing the thermal conductivity is shown by the calculated curves in Figure 1. These curves assume that the thermal conductivity of the radioactive material is very small compared to that of the metal. Both phases are assumed to be 100% dense. The thermal conductivity of the ceimets was calculated using three different equations (+2) chosen írom the many that various people have derived for the con- ductivity of aggregates. The oriented conductors give moderately better results. Recognition of this phenomenon can lead to a worth- while reduction in the cost of fabrication of many sources. The material can be encapsulated as a loose powder instead of as a fabricated form. It; will distribute itself in approximately the desired manner. Figure 2 is a chart which aids in the rapid calcu- lation of kP for any combination of a highly con- ducting metal and a poorly conducting radioactive material providing tbe values of k and P for the pure materials are known. Figure 3-B shows a thermionic heat source which is typical of many proposed designs. The useful heat flow leaves through one end of the cylindrical container. The rest of the container is assumed to be insulated so as to reduce extraneous heat losses to a low level. The radioactive material is attached to the inner surface of the cylinder at the end from which the useful heat flow passes. The temperature of this end of the container is "Superior numbers refer to similarly-numbered references at the end of this paper". 2 - PAh. set in the design of the apparatus. The volume of the container is appreciably greater than the vol- ume of the radioactive material in order to allow space for the helium released by the radioactive decay of an alpha emitting radioisotope. @ @ or h = 9/ where q = rate of heat flor, A = area, It is assumed that the radioactive material vapor- izes and, condenses without change in its proper- ties. It is also assumed that all of the heat is generated within the radioactive material. Thus, the reasoning will not necessarily apply if an appreciable fraction of the energy is emitted as gamma rays. P = power density, h = thickness of radioactive layer. The thickness is directly proportional to the rate of heat loss per unit area. The volatile radioactive material will distribute itself in a continuous layer covering the inner surface of the capsule. No part of the surface OI' the capsule can remain bare so long as at least some heat escapes from all parts of the outer sur- fece. This results from the fact that heat can flow only from a higher to a lower tempereture. Furthermore, the heat leaving a bare surface can cožie only from radioactive material which must, therefore, be at a higher temperature than the bare surface. Transport of volatile material from the hotter to the cooler surface will occur. Application of the equation from Table 1 for the maximum internal. temperature of a planar source form leads to Equation 3, which relates the outer surface of the radioactive layer to the constant inner surface temperature. To = Te - Pn2/2 k (3) where T - tenperature of the outer surface of the radioactive layer, Tg = temperature of the inner surface, The temperature of the inner surface of this layer wiil be uniform at equilibrium. The reason for this uniformity is apparent when one considers that if a difference in temperature did exist material would vaporize from the hotter surface and condense on the cooler surface. k = thermal conductivity of the fuel. The other symbols have been defined. Equations 2 and 3 can be combined to produce Equation 4. (4) 2 Pk For thin layers essentially all of the beat loss from any part of the radioactive layer passes . through the outer surface of the layer. This rate of loss is essentially equal to the rate at which heat is generated within that part of the layer. It can be seen that T will vary and will be at a maximum when (g/A) is at a minimum. Thus, the outer surface of the radioactive material layer will be botter for the well insulated parts of the capsule than at the end from which the thermionic heat flow occurs, This equality exists because of the lack of other significant modes of heat loss or gain. The radioactive material layer cannot gain or lose heat by conduction or thermal radiation across the interior of the capsule because of the uniform inner surface temperature. Conduction within the layer parallel to the surface will be small as compared to flow from the outer surface of the layer so long as the thickness of the layer is small compared to the dimensions of the capsule. One consequence of the uniformity of the interior temperature, Te, is that the lowering of T, at any point will result in a general lowering of T, throughout the source at equilibrium. One method of accomplishing this is to introduce oriented metallic conductors into the radioactive material layer on the thermionic end of the capsule (see Figure 4). It is apparent that the layer will be thick at the end from which the thermionic heat flow occurs and thin on the surfaces corresponding to the well insulated parts of the capsule. Thus, the radio- active material will tend to locate itself in the desired manner. The change in T, produced by this method can be of great practical importance as is shown by the following example. If the radioactive material layer at the thermionic end of the capeule is assumed to consist of pure 244 Cm203 and the values of 50 watts/cm2, 26.4 watts/cm®, and 0.03 watts/cm °C are used for q/A, P and k, respectively, Ti will exceed To by 1580°C according to Equation 4. If To is fairly high, part of the Cm203 will be The thickness of this laver can be predicted mathe- matically by simple equations for the case in which the thickness of the layer of radioactive material is small as compared to the diameter and length of the capsule. This will se tho 0250 wie??. ?oore- - . . . 4 + 1 17 A = area, ***IT 18 assumed "that the radioactive material vapor izes and, condenses without change in its proper- ties. It is also assuned that all of the heat is generated within the radioactive material. Thus, the reasoning will not necessarily apply if an appreciable fraction of the energy is emitted as gamma rays. P = power density, h = thickness of radioactive layer. The thickness is directly proportional to the rate of heat loss per unit area. : The volatile radioactive material will distribute itself in a continuous layer covering the inner surface of the capsule. No part of the surface of the capsule can remain bare so long as at least some heat escapes from all parts of the outer sur- face. This results from the fact that heat can flow only from a higher to a lower temperature. Furthermore, the heat leaving a bare surface can come only from radioactive material which must, therefore, be at a higher temperature than the bare surface. Transport of volatile material from the hotter to the cooler surface will occur. Application of the equation from Table 1 for the maximum internal temperature of a planar source form leads to Equation 3, which relates the outer surface of the radioactive layer to the constant inner surface temperature. T. = T; - Ph2/2 k (3) where I = temperature of the outer surface of the radioactive layer, T, = temperature of the inner surface, The temperature of the inner surface of this layer will be uniform at equilibrium. The reason for this uniformity is apparent when one considers that if a difference in temperature did exist material would vaporize from the hotter surface and condense on the cooler surface. k = thermal conductivity of the fuel. The other symbols have been defined. Equations 2 and 3 can be combined to produce Equation 4. To = Ti - 19/4) (4) .. For thin layers essentially all of the heat loss from any part of the radioactive layer passes. through the outer surface of the layer. This rate of loss is essentially equal to the rate at which heat is generated within that part of the layer. 2 Pk It can be seen that I will vary and will be at a maximum when (a/A) is at a minimum. Thus, the outer surface of the radioactive material layer will be hotter for the well insulated parts of the capsule than at the end from which the thermionic heat flow occurs. This equality exists because of the lack of other significant modes of heat loss or gain. The radioactive material layer cannot gain or lose heat by conduction or thermal radiation across the interior of the capsule because of the uniform inner surface temperature. Conduction within the layer parallel to the surface will be small as compared to flow from the outer surface of the layer so long as the thickness of the layer is small compared to the dimensions of the capsule. 40 that the lowering OI twe One consequence of the uniformity of the interior temperature, T., is that the lowering of T. at any point will result in a general lowering of T. throughout the source at equilibrium. One method of accomplishing this is to introduce oriented metallic conductors into the radioactive material layer on the thermionic end of the capsule (see Figure 4). It is apparent that the layer will be thick at the end from which the thermionic heat flow occurs and thin on the surfaces corresponding to the well insulated parts of the capsule. Thus, the radio- active material will tend to locate itself in the desired manner. The thickness of this layer can be predicted mathe- matically by simple equations for the case in which the thickness of the layer of radioactive material is small as compared to the diameter and length of the capsule. This will be the case won an appre- ciable void volume has been allowed to contain helium generated by alpha decay. In this case the layer can be treated as a flat plate and the . Iollowing equations from Table I will apply to any small area of the layer of radioactive mate- rial: The change in 1, produced by this method can be of great practical importance as is shown by the following example. If the radioactive material layer at the thermionic end of the capsule is assumed to consist of pure 244cm203 and the values of 50 watts/cm², 26.4 watts/cm®, and 0.03 watts/cm °C are used for q/A, P and k, respectively, Ti will exceed T, by 1580°C according to Equation 4. If T, is fairly high, part of the Cm203 will be molten. If an optimum combination of tungsten metal and 244cm203 is used, the temperature differ- ence will be only 187°C. A high value of Tz has three undesirable conse- quences: (1) The stored helium gas is at the temperature Ty and its pressure increases with temperature. (2) The metal wall of the capsule . .at a distance froin the thermionic surface tends to leads to weakening and accelerated deterioration. (3) The high temperature of the capsule walls also will cause an increase in the heat loss through the insulation. untoward situation will occur during the luigra- tion although the temperature in the center of a charge of loose powder might become very high. This would ordinarily do no more than cause rapid vaporization and migration to the cooler surfaces of the capsule. The material in contact with the capsule cannot reach a temperature much above the operating temperature because of rapid heat trans- fer to the capsule surface. So far, the temperatures and heat flow have rew ferred only to the layer of radioactive material. When it can be assumed that the flow of heat along ühe capsule walls parallel to the surface is negli- gible, (g/A) can be considered to be the heat flow from the surface of the capsule. However, in many cases this assumption will involve considerable error. In many sources, the rate of volatile migration will not be rapid enough for an equilibrium dis- tribution to be established during the life of the source, although at least some movement toward this distribution will always occur. The avail- able vapor pressure data for most heat source compounds are not adequate for good estimations of migration rates. In the common case of a thick-walled metal capsule, the conduction of heat by the walls to the low temperature end of the capsule will have a sub- stantial leveling effect on To, 9/A, and h. The heat flow, q/A, from the radioactive material layer in any part of the hotter (insulated) part of the system will now equal the sum of the heat lost through the insulation and the heat conducted along the capsule walls. This greater flow of heat requires a thicker deposit of radioactive material to hold T, constant. This is illustrated in Fig- ure 4. It should be noted, however, that the overall effects of the thermal conductivity of thick cap- sule walls are beneficial. The heat flowing along the wails flows to thermionic surface and is not lost. Heat losses are, in fact, reduced since the temperature of the insulated parts of the capsule are lowered towaad that of the thermionic end which is fixed by the design of the device. This lowering of the temperature will also result in greater strength and less deterioration for the capsule metal. The movement of radioactive mate- ria away from the thermionic surface also reduces the thickness of the layer on this surface. Since To is fixed, this thinning of the radioactive lever causes a lowering of T, which is the temperature of the helium storage volume. Thus, the pressure exerted by a given quantit reduced. iven quantity of heli Although this discussion was directed toward thermionic heat sources, the basic conclusions wil). apply qualitatively to any capsule geometry. The material will tend to concentrate on the surfaces from wnici the greatest heat flow occurs and T., will be constant at equilibrium. The characteristics of the ideal capsule for a volatile radioactive material in applications where . internal temperature is a limiting factor can be summarized as follows: (1) It should have thick wails of a highly conducting metal. (2) Internal metallic heat paths should be used to conduct the heat to the desired surface. A desirable distribution can be obtained even if So far, the temperatures and heat flow have re- ferred only to the layer of radioactive material. When it can be assumed that the flow of heat along the capsule walls parallel to the surface is negli- gible, (q/A) can be considered to be the beat flow from the surface of the capsule. However, in many cases this assumption will involve considerable error. In many sources, the rate of volatile migration will not be rapid enough for an equilibrium dis- tribution to be established during the life of the source, although at least some movement toward this distribution will always occur. The avail- able vapor pressure data for most beat source compounds are not adequate for good estimations of migration rates. . I is In the common case of a thick-walled metai capsule, the conduction of heat by the walls to the low temperature end of the capsule will have a sub- stantial leveling effect on To, q/A, and h. The heat flow, q/A, from the radioactive material layer in any part of the hotter (insulated) part of the system will now equal the sum of the heat lost through the insulation and the heat conducted along the capsule walls. This greater flow of heat requires a thicker deposit of radioactive material to hold Ti constant. This is illustrated in Fig- ure 4. is . . think t It should be noted, however, that the overall effects of the thermal conductivity of thick cap- sule walls are beneficial. The heat flowing along the walls flows to thermionic surface and is not lost. Heat losses are, in fact, reduced since the temperature of the insulated parts of the capsule are lowered toward that of the thermionic end which is fixed by the design of the device. This lowering of the temperature will also result in greater strength and less deterioration for the capsule metal. The movement of radioactive mate- rial away from the thermionic surface also reduces the thickness of the layer on this surface. Since To is fixed, this thinning of the radioactive laver causes a lowering of T; which is the temperature of the helium storage volume. Thus, the pressure exerted by a given quantity of helium will be. reduced. na l idad necesibi Although this discussion was directed toward thermionic heat sources, the basic conclusions will apply qualitatively to any capsule geometry. The material will tend to concentrate on the surfaces from which the greatest heat flow occurs and Ti will be constant at equilibrium. highest sisteminin insatisfacer 1 The characteristics of the ideal capsule for a volatile radioactive material in applications where · internal temperature is a limiting factor can be summarized as follows: (1) It should have thick walls of a highly conducting metal. (2) Internal metallic heat paths should be used to conduct the heat to the desired surface. is there mandamientation with now and A desirable distribution can be obtained even if the radioactive material is encapsulated as loose lumps or powder when comparatively fast migration toward the equilibrium distribution occurs. No initiation artistice is isitioning m REFERENCES Russell, H. W., Principals of Heat Flow in Porous Insulators, J. Am. Cer. Soc. 18: 1-5 (January 1935). Rayleigh, Lord, On the Influence of Obstacles Arranged in Rectangular Order Upon the Prop- erties of a Medium, Phil. Mag. 34: 481-507 (1892). Bruggeman, D. A. G., Dielectric Constant and Conductivity of Mixtures of Isotropic Mate- rials, Ann. Physik 24: 636-79 (1935). (4) Jun, C. K. and Hoch, M., Thermal Conductivity of Tantalum, Tungsten, and Tantalum-Tungsten Alloys, Technical Rpt. AFML-TR-65-191, University of Cincinnati (May 1965). Rohrman, C. A., Radioisotopic Heat Sources, USAEC Rpt. HW-76323, Hanford Atomic Products Operation (February 1963). (6) Rimshaw, S. J., Ketchen, E. E., and Burnett, J. L., private communication, Oak Ridge National Laboratory (March 1966). (7) Ketchen, E. E., private communication, Oak Ridge National Laboratory (June 14, 1967). ILLUSTRATIONS Figure 1. Comparison of the Thermal Conductivities of Laminar Composite Fuels and Cernets. Figure Comparison of Surface Heat Flux Factors of Laminar Composites and Cermets Fuels. Figure 3. Distribution of Radioactive Material Inside Capsule. Figure 4. Qualitative Representation of Fuel Distribution in Three Models, Table 1. Equations for Fue). Forms of Simple Geometric Shape Parameter Flat Plate Solid Cylinder Solid Sphere Pha PD2 PD2 16k 2k 24K IPD3 PAN A(zkParmax) 1/2 414IKATmax max = (a/A)max = (2kPaTmax) 1/2 (KPATmax) 1/2 (akoppimax )/2 Table 2. Maximum Surface Heat Fluxes of Laminar Composite Planar Fuel Forms Radioactive Compound Surface Temp., Power Density, watts/cc Melting Point, Maximum Surface Heat Flux, watts/cm2 90sro 2.08 2430 1250 1500 1800 147Pm203 2.36 2350 1250 1500 1800 244cm203 26.4 1950 1250 1500 1800 232002 2176 1250 1500 1800 2000 228Thoz 1270 3050 1250 1500 1800 2000 2050 070 860 780 ORNL-DWG 66-11423 !! SELL'S -LAMINAR COMPOSITE OF METAL AND OXIDE, HEAT FLOW – PARALLEL TO STRATA I CERMET WITH METAL PHASE CONTINUOUS, FROM RUSSEL'S EQUATION - CERMET WITH METAL PHASE CONTINUOUS, FROM RAYLEIGH- | MAXWELL OR EUCKIN EQUATION+ CERMET WITH METAL PHASE CONTINUOUS FROM BRUGGEMAN'S EQUATION, r -CERMET WITH OXIDE PHASE CONTINUOUS, FROM BRUGGEMAN'S EQUATION Et RELATIVE THERMAL CONDUCTIVITY, k/KMETAL 0 .0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 VOLUME FRACTION OXIDE Comparison of the Thermal Conductivities of Laminar Composite Structu.ces and Cermets. FUELS . . .-... ". " t .. - h.com .--- . . w - . ..... h the mou i . .. e thin .. . .. . . . . - . . . ORNL-DWG 66-49422 PARALLEL STRATA OF METAL AND OXIDE 7 MAXWELL-RAYLEIGH OR EUCKEN EQUATION, CERMET GWITH METAL PHASE+ CONTINUOUS 0.2 RUSSEL EQUATION, CERMET WITH METAL PHASE CONTINUOUS SURFACE HEAT FLUX FACTOR (kP) = [KMETAL * Poxide) BRUGGEMAN EQUATION, CERMET WITH METAL PHASE CONTINUOUS BRUGGEMAN EQUATION, CERMET WITH OXIDE PHASE CONTINUOUS 0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 4.0 VOLUME FRACTION OXIDE Comparison of Surface Heat Flux Factors of Laminar Composites and Cermets, Fw · · - : : .. ..... . . . .. . .. ....... ............ A. IDEAL - DISTUBUTION .. .. VR! HEAT FLOT ..commons Tweede IT .. . ........ k CAPSULE MATERIAL RADIOACTIVE. : Fig. 3. MATERIAL INSIDE CAPSULE DISTRIBUTION OF RADIOACTIVE · .. ' juccana.comcommon. mind .. s ·licacione ...... C C B. EGUILIBRUM DISTRIBUT/01/ Pallatih? HVERT 201! - - . ARRO:YS IND:CATE DIRECTION OF HEAT FLOW. OXNL-DWG. 67-268 To:TEMPERATURE AT TSE FUEL-CAPSULATE FACE (MAXI.. AT VEDICATED 2011T) T::TEMPERATURE AT THE INTER SURFACE OF THE FUEL AT EQUIL:3RIUM To (4) > , < > a C ; 7; a) x 1; ) > 7 C) - CONSTANT *COMSTA:!T . Toa MAXIMUM Ti *50::START T AXIMUM COSTANT Work card V nennamen IL. PP dawkwambambamba - INSULATION SILT - CAPSULE CONDUCTORS A IN ww.rivite conductors FUEL 1 A. LATERAL HEAT FLOKI . S. LATERAL 1.2 LOMO!TLOKAL C.LATERAL AND 10RGITUDIA . HEAT FLOW WITH CONDUCTORS ::UEL Fig. Qualitative Representation of Fuel Distribution in Three Models. !! !! ! ! N . . . H END 2 . 2 t . DATE FILMED 10 / 5 / 67 .. P . .. . . ... .. ... 2 . . .: - 11 - -