2 - UNCLASSIFIED ORNL PI 150 TOFI The First Time 25200 . .. ;, Keto- 12 .. , LEGAL NOTICE This report was prepared as an account of Government sponsored work. Neither the United States, nor the Commission, nor any person acting on behalf of the Commission: A. Makes any warranty or representa- tion, expressed or implied, with respect to the accuracy, completeness, or usefulness of the information contained in this report, or that the use of any information, appa- ratus, method, or process disclosed in this report may not infringe privately owned rights; or B. Assumes any liabilities with respect to the use of, or for damages resulting from the use of any information, apparatus, method, or process disclosed in this report. As used in the above, "person 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, disseminates, or provides access to, any information pursuant to his employ- ment or contract with the Commission, or his employment with such contractor. . . . . Si. . 2 . - . i T: + 2Y ital !1i ... . 24 1 DTIE MICROCARD ISSUANCE DATE 9/14 h961 " ' YER . X . ' + -. - - W kilicor , CONF-638-2 DTIE s 2. note Aid to 83564 เue 11 Pimyo This note 18 an addendim to RN -3556 and was prepared to ailow presenta- tion of the most rece!. rad: seat flow apparatus measurements at the Nationa i Prys :51 Labor-story fer .cc on Thermal Conductivity, Teddington, Engia :., Juny J.., 962. 19 antert " SISTER morietun d. iii . . .. ... ... reimininkrimmersteiro..-.. en THERMO :38 ES OF GRADE CGB CEAPHITE* J. D Mourc, I. G. Gorlfer and D. L MCEIRO Metals Cer' s Divin. Tak R: .. Jati di laboratory as. Piqe, nessee, USA . i... . :": Facsimile Price s . interior Microfilm Price $_ Ro LEGAL NOTICE - This report as prepared sa un acoma of Government sponsored work. Nothout the United Hatos, marline Comuni, war wy porma muy bonit of the commandon: A. Wake my warranty or reputation, emprend or implied, we repect to the sur- racy, complement, or weters of the winnmathow contain the report of that when we of way lubormation, manau, worth a proces declared that this report may not matters printly a nd rights; n. A way that staa wa rast to the web, w for tempo read the tren the w of way intor matiem, apuram, with or part dechowed to the reports Am vend then the whova, sperma actiung an d of the commen" besteden wury we shery o choc ad the Commis, et v oy a cha cunctor, When out that a employee or contractor of the Contest w staplegue at wwch cpretrun tor prepares, docrinales, or awhing across any motormation par le do employment or coorrect what the Comminosou, or we empiment with much contractor. , wit Available from the Office of Technical Services Department of Commerce Washington 25, D. C. ..;) Selim Rikom . *Research sponsored by contract with the Union Carc. U. ). Atomic Energy Commission und Cc :oration. ... . . 2 .,. - - THERMAL PROPERTIES OF GRADE CGB GRAPHITE J. P. Moore, T. G. Godfrey, and D. L. McElroy SPECIMEN CHARACTERIZATION Grade CGB graphite is a nuclear graphite which is basically an extruded petroleum coke bonded with coal tar pitch. No carbon blacks are used and the low-permeation graphite is finished through a series of impregnations and heat treatments with a final heat treatment of all components to 2800°C. The graphite is produced by the Carbon Products Division of Union Carbide Corporation as 2 1/4-in.-square by 72-in.-long bars with an average bulk density of 1.85 g/cm3. One bad feature of the graphite is its cracked condition which 18 caused by the structure of the graphite being 80 dense that hydrocarbons produced through pyrolysis of the impregnants cannot escape via the pores during fabrication. In general, these cracks are 0.001 to 0.002 in. thick, 1/8 to i 1/4 in. wide, and less than 3 in. long. The bar stock was machined into 2 1/8-in.-diam by l-in.-thick disks for the radial heat flow specimens and radiographs or these were used to select two crack-free measuring disks. These speci- mens, which had a measured density of 1.824 g/cm", permitted thermal con- ductivity measurements with heat flow normal to the extrusion axis, which is the low k directior.. The axial core heater hole was made only 3/8 in. in diameter in order to allow the largest practical value of lo rz/rı (12 was 0.969 in. and i was 0.315 in.) and hence the largest possible st. A 1/4-in.-diam spectrographic carbon rod was used for the core heater and 70% Pt-30% Rh wires were placed in shailow grooves to serve as voltage taps. THERMAL CONDUCTIVITY DATA A listing of the results obtained is given in Table 1. T. results at 51°C are considered questionable since the measured ar was jéis than 1/2°C. The results obtained at 704 and 602°C after heating to 910°C were 1% higher than those of the first cycle. This increase was caused by a slight contamination of the 90% Pt 10% Rh-Pt thermocouples at 910°C but was not sufficient to doubt the validity of the 910°C results. However, ,- - Table 1. Total Thermal Conductivity of Grade CB Graphite Normal to the Extrusion Axd8 28 Measured in the Radial Heat Now Apparatus t(°C) T(°K) (w oppi cm-2) (-762 cm) 51 1.0878 0.9610 101 2014 0.8786 295 397 500 324.2 374.2 477.2 568.2 670.2 773.2 875.2 977.2 1183.2 1288.2 876.2 0.920 1.040 1.138 1.247 1.403 1.522 1.611 1.769 2.023 1.924 1.368 0.8019 0.7129 0.6571 0.6020 0.5612 0.4944 0.51966 0.73210 602 704 910 · 1015 603 & Accuracy of 51°C data is questionable because of very small at across specimen. Disregard because of severe thermocouple instabilities. the results obtained at 1015°C should be disregarded because of severe thermocouple instabilities. In addition, the electrical resistance of the core heater at 603°C indicated the thermocouples bad a -10 to -15°C error which is sufficient justification to disregard the 603°C data. po. AUXILIARY MEASUREMENTS In addition to the thermal conductivity measurements in the radial heat flow apparatus, electrical resistivity measurements and low-temperature thermal conductivity measurements were made normal and parallel to the extrusion axis of the same CGB graphite stock. ". . - . i . .: : Electrical Resietivity Measurements Electrical resistivity measurements were made by the four-probe potentiometric method under a vacuum of 1005 to 10-6 torr, between 23 and 1000°C. The results were reproducible to 10.1% and accurate to +0.25%. The results listed in Table 2 were taken from a smooth curve drawn through the data plotted in Fig. 1. This figure also shows the temperature varia- tion of the ratio of the electrical resistivities in the normal and parallel directione. The electronic portion of the thermal conductivity was calcu- lated using the Wiedemann-Franz-Lorenz relation. Table 2. Electrical Resistivity and Electronic Portion of Thermal Conductivity of CGB Graphite Perpendicular to Extrusion Axis Parallel to Extrusion Axis p . ke (uohm-cm) (w ºr em 2) p t(90) T("K) (uohn-cm) (w ºk?cm-2) 23. 100 200 300 400 296.2 373.2 473.2 573.2 673.2 773.2 873.2 973.2 1073.2 1173.2 1273.2 1232 1132 1045 993.2 962.7 945.4 937.3 936.5 941.5 948.8 960.8 0.0059 0.0081 0.0112 0.0142 0.0171 0.0200 0.0228 0.0254 0.0279 0.0303 0.0325 583.4 538.0 501.5 480.5 469.0 463.5 463.5 467,8 474.0 482.0 490.0 0.0124 0.0170 0.0231 0.0292 0.0352 0.0409 0.0461 0.0510 0.0555 0.0596 0.0637 2.11175 .. 2.10408 2.08375 2.06701 2.05266 2.03969 2.02222 2.00192 1.98629 1.96846 1.96082 60 700 800 900 1000* Thermal Conductivity Measurements Thermal conductivity measurements were made in the range of 34 to 75°C in a longitudinal canparative type heat flow apparatus. This apparatus consisted of two l-in.-diam gold-plated Armco iron meter bars mounted coaxially in a vacuum chamber with the cylindrical disk specimen compressed - . . † between them. A temperature gradient was established along the meter bar's 8.nd the specimen by a Nichrome heater at the top of one meter bar and a water-cooled heat sink at the bottom of the other mater bar. The tempera- ture at known positions along the meter bars was determined with Chranel-P/Constantan thermocouples. The temperature gradient along each meter bar was extrapolated to the meter bar specimen interface to determine the temperature drop across the specimen. The measured t:"nperature gradi- ents along the meter bars were used with the known thermal conductivity of the iron meter bars to calculate the amount of ineat flowing through the specimen. Interracial resistance was minimized with l-mil-thick indium foils and by careful lapping of the specimen and meter bar surfaces. This apparatus was evaluated using an Armco iron specimen and yielded data with a repeatability of better than 1/4% and a probable mccuracy of +3%. The thermal conductivity measurements listed in Table 3 were made with this apparatus on a 0.8-in.-high by 1.00-in. -diam .CGB graphite speri- men cut so that the heat flow wes normal to the extrusion ads. Also listed in Table 3 are similar measurements on an 0.8-in.-high by 1.00-in.- diam CGD graphite specimen cut so that the heat flow was parallel to the extrusion axis. Table 3. Thermal Conductivity of Type CGB Graphite as Determined from Measurements in the Longitudinal Heat Flow Apparatus Direction of Heat Flow +(°C) T°K) (w or I com-2) Normal to extrusion axis Normal to extrusion axis Parallel to extrusion axis Parallel to extrusion axis Parallel to extrusion axis 307.2 348.2 307.2 326.2 348.2 1.087 1.058 1.942 1.921 1.884 DISCUSSION OF RESULTS The total thermal resistivity, 1/k, values for the axis normal to extrusion that are tabulated in Table 1 are plotted as a function of the absolute temperature in Fig. 2. The lattice component, ktor of the thermal conductivity was calculated by subtracting the electronic component, ke, as determined from appropriate electrical resistivity data and the Wiedemann-Franz-Lorenz relation, from the total thermal conductivity. These calculated lattice component values are also plotted in Fig. 2. Above its Debye temperature, the lattice component of the thermal resistivity of an electrically insulating solid should depend linearly on the absol'te temperature. The lattice component values in Hg. 3 are all within 14% of the linear equation, 1/1 = R1 = 0.48812 + 1.4060 x 10-3 T, where k = w ºk?cm-, and T - K. The electronic component of the thermal conductivity is shown in Fig. 2 with the appropriate scale on the right. The numbers in parentheses above the ke line at 200°K increments indicate the percentage of the total thermal conductivity which is electronic in nature. Since the thermal conductivity of graphites varies so widely with composition and manu- facturing technique, no attempt was made to selectively compare these results with those of other investigators. The results obtained from the longitudinal heat flow apparatus are limited in temperature range but are very useful since they provide a check on the radial results for k in the normal direction and allow com- parison between the values of k along the two principal axes of the graphite. The results from this apparatus are tabulated in Table 3 and are plotted in Fig. 3. The results from the radial apparatus are also shown on this figure and the intercomparison of the two methods is very good. At these temperatures, the thermal conductivity ratio of the axis parallel to extrusion and the normal axis is 1.74. CONCLUSIONS Theoretical considerations based on three-phonon umklapp processes predict an inverse relationship between the lattice component of the thermal conductivity and the absolute temperature for temperatures above the Debye temperature of the solid. The results from this work show that this inverse relationship holds for graphite over the wide temperature range from 323 to 1183°K. This entire temperature span 18 well below the Debye temperature for graphite. e, 1300 . UNCLASSIFIED ORNL-DWG 6:1-5879 12.16 ELECTRICAL RESISTIVITY COB GRAPHITE Tod TO EXTRUSION DIRECTION 2.14 ::|| TO EXTRUSION DIRECTION PllPro 2.12 .- - - -. --- -- 2... - 2.10 -- - -. . 2.08 P. ELECTRICAL RESISTIVITY (M.2-cm) ....-- ... 12.06 lid, To ... -- .. . 2.04 ..-. .- 2.02 2.00 400 . . . . - + - o 1.96 200 400 600 800 1000 TEMPERATURE (°C) Fig. 1. The Electrical Resistivity of Grade CGB Graphite Along the Principa). Axes. UNCLASSIFIED ORNL-DWG 64--5877 -- ..... • Vkl o Vk 1.8 ----------- A ke VK THERMAL RESISTANCE (w-Ok cm) Ke, ELECTRONIC THERMAL CONDUCTIVITY (W OK-4 cm) (6.5%) (4.7%) (3.3%) oom, L:6199) — (4.9%) ...! (0.9%) - 0.8l. 300 400 500 600 700 800 900 TEMPERATURE (°K) 1000 1100 1200 1300 Fig. 2. Therma). Resistivity in the Normal to Extrusion Direction of Grade CGB Graph::from 300 to 1200^K us Measured in the Radial lleut Flow Apparatus. UNCLASSIFIED ORNL-DWG 64-5878 A PARALLEL TO EXTRUSION AXIS O NORMAL TO EXTRUSION AXIS O RESULTS FROM RADIAL APPARATUS K, THERMAL CONDUCTIVITY (w OK-'cm') 0.8 300 310 320 360 370 380 330 340 350 TEMPERATURE (°K). Fig. 3. Thermal Conductivity Results on Grade CGB Graphite Obtained in a Low-Temperature longitudinal Heat Flow Apparatus and From the Radial lcat Flow Apparat:18. END