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NONDESTRUCTIVE TESTING
OF NUCLEAR GRAPHITE
A symposium
presented at the
Seventieth Annual Meeting
AMERICAN SOCIETY FOR
TESTING AND MATERIALS
Boston, Mass., 25-30 June, 1967
ASTM SPECIAL TECHNICAL PUBLICATION NO. 439
List price $8.00; 20 percent discount to members
published by the
AMERICAN SOCIETY FOR TESTING AND MATERIALS
1916 Race Street, Philadelphia, Pa. 19103
(PDVSA Los Teques) pursuant to License Agreement. No further reproductions authorized
BY AMERICAN SOCIETY FOR TESTING AND MATERIALS 1968
Library of Congress Catalog Card Number: 68-16730
NOTE
The Society is not responsible, as a body,

for the statements and opinions
advanced in this publication.
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Foreword
The papers in the Symposium on Nondestructive Testing of Nuclear

Graphite were presented at the Seventieth Annual Meeting of ASTM
held in Boston, Mass., 25-30 June 1967. Co-sponsors of this symposium
were Committees C-5 on Manufactured Carbon and Graphite Products
and E-7 on Nondestructive Testing. G. H. Tenney and G. G. Hoffman
of the Los Alamos Scientific Laboratory presided as co-chairmen.
Related
ASTM Publications
Effects of High-Energy Radiation on Inorganic Sub-

stances, STP 400 (1966), $5.25
The Effects of Radiation on Structural Metals, STP

426 (1967), $52.00
(PDVSA Los Teques) pursuant to License Agreement. No further reproductions authorize
Contents
Introduction 1
Infrared Testing of Bonds Between Graphite and Protective Coatings—
D. R. GREEN AND C. K. DAY 4
Nondestructive Testing of Graphite at the Los Alamos Scientific Labo-
ratory—B. L. BLANKS, N. B. EDENBOROUGH, D. E. ELLIOTT, AND
R. M. FORD 18
Application of Alcohol Penetrant for Evaluation of Surface Porosity
of Graphite Inserts for Rocket Nozzles—j. A. HENDRON 37
Discussion 47
Prediction of Strength of Graphitic Material by Nondestructive Test
Techniques—L. H. FANELLI AND R. D. MCKOWN 48
Contact Microradiography of Graphite—L. R. BUNNELL 61
A Novel Infrared Nondestructive Testing Technique for Determining
the Thermal Conductivity of Graphite—A. w. SCHULTZ 70
Strength Predictions for Graphite: A Review of Prior Work at AVCO
SSD—C. H. HASTINGS 87
Low Voltage Radiographic and Microradiographic Techniques for
Graphite—R. w. MCCLUNG 97
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Introduction
It is indeed a gratifying assignment to write these introductory remarks

to the Special Technical Publication which contains the papers pre-
sented at the Symposium on Nondestructive Testing of Nuclear Graphite
in Boston, Mass., during the 1967 Annual Meeting of ASTM on 27
June 1967. The fact that the American Society for Testing and Mate-
rials decided to publish the proceedings in book form constitutes probably
the most satisfying reward for the chairman who tried his best to make
such a symposium successful. It is, therefore, with gratitude and appre-
ciation to ASTM and each author when writing these remarks as chair-
man of this symposium.
To us who have been working on this topic in many laboratories
throughout the country for many years it appeared to be urgent and
justifiable to recommend that such a symposium be held in order to
prove to the technically interested public the need for combined efforts.
Because of the great need of reliable and reproducible graphite in the
space and nuclear industry, it became apparent that the fundamental
physical characteristics of this material and its behavior and up to that
time unorthodox environmental conditions have actually not been
known. It furthermore became visible that many of the parameters in-
fluencing the characteristics of graphite during the production processes
were also not known. The reason for this existing gap is, of course, very
simple. Prior to the nuclear and space age graphite was primarily used in
the crucible and steel industry, and the qualitative characteristics of the
mass-produced graphite satisfied the demand.
This generally accepted condition became completely unsatisfactory
practically overnight when the demand for materials of high thermal
conductivity, high density, more specific coefficients of linear thermal
expansion, and uniformity—to mention a few—became of paramount
importance.
It is well realized that in the last few years many means of dissemina-
tion of knowledge on this subject have been utilized in order to spread
the obtained data expeditiously. Technical publications, in the form of
text and reference books, classified and unclassified technical papers in
this and other
Copyright by ASTMcountries, andMonsymposia
Int'l (all rights reserved); and
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private industryby and government agencies, dealt with specific subjects
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1
2 NUCLEAR GRAPHITE
within the rapidly growing field of graphite technology. The graphite

manufacturing industry has been and is being continuously exposed to
new and stringent specifications as demanded by potential users. As a
matter of fact, in many instances this industry has become familiarized
with new data dealing with the characteristics and behavior of graphite
which were obtained in technical and scientific laboratories.
In all these research and development activities nondestructive testing
has become a very important source of information. It can well be
realized that nondestructive testing had to study and evaluate its own
test methods as applied to the inspection of graphite. Many test methods
had to be refined in order to cope with many, from this point of view,
undesirable features of this material. The high degree of scattered radia-
tion caused by graphite when exposed to penetrant radiation, the grain
size and orientation when using ultrasonics, and the nonuniform
porosity when applying radiation gages are just but a few of those prob-
lems that had to be solved within the nondestructive testing laboratories,
prior to applying them to graphite evaluation. In many cases special non-
destructive testing instruments had to be designed and manufactured in
these laboratories, criteria established, and specifications developed, com-
posed, and accepted.
These efforts and activities have reached such a plateau that the rec-
ommendation by Committees C-5 and E-7 for scheduling such a sym-
posium were approved by the American Society for Testing and Mate-
rials. The very satisfactory attendance, the lively discussions following
each paper, and the interest in the proceedings as expressed by lab-
oratories and industry in this country and abroad influenced the ASTM's
decision to publish this Special Technical Publication.
It is well realized, of course, that a one-day symposium cannot cover
all the activities, work, and aspects on this subject. On the other hand
it demonstrated the need for more knowledge, for better dissemination
of the respective findings, and, last but not least, for establishing a basis
for possible specifications and standards dealing with nondestructive
testing of nuclear graphite. This publication, therefore, should be con-
sidered to be a technical progress report on this subject and to be a
spark plug for more coordinated activities in this field. Producer and
consumer have to realize that in this field only joint forces can overcome
the major obstacles that are still facing us in this endeavor.
It is indeed my hope that all the efforts by ASTM, the authors, the
Technical Review Committee, the co-chairman, and, last but not least,
those of the chairman have not been in vain. If only a part of those
goals just listed can be reached in the foreseeable future, then I consider
this publication a success. It is up to the potential readers of STP 439 to
study the published papers in this spirit and to apply the purpose of this
INTRODUCTION 3
publication to their own efforts in the interest of a large technical com-

munity and progress in this field.
G. H. Tenney
Technical advisor on nondestructive testing,
Los Alamos Scientific Laboratory,
Los Alamos, N. Mex.; symposium co-chairman
D. R. Green1 and C. K. Day1
Infrared Testing of Bonds Between

Graphite and Protective Coatings*
REFERENCE: Green, D. R. and Day, C. K., "Infrared Testing of

Bonds Between Graphite and Protective Coatings," Nondestructive Test-
ing of Nuclear Graphite, ASTM STP, 439, American Society for Test-
ing and Materials, 1968, pp. 4-17.
ABSTRACT: A nondestructive infrared method has been developed for
testing bonds between coatings and graphite. Application of a special
digital dual-scan technique makes the test independent of the specimen
surface emittance (often called emissivity). In addition, this method does
not require contact with the specimen, and can be automated for pro-
duction testing. Heat was applied during tests by projecting a hot jet of
helium onto the specimen surface. A commercial infrared radiometer
was used to sense the resulting surface temperatures. This paper de-
scribes the theory and equipment, and some of the experimental results
from tests on bonds between graphite and thin columbium carbide
coatings.
KEY WORDS: nondestructive testing, infrared, coatings, bonds, graphite,
emittance digital systems
Nuclear graphite components are often required to conduct a large

heat flux in a hostile environment. Such applications require protective
coatings to prevent erosion or corrosion of the graphite. These coatings
must be well bonded to give good mechanical strength and to provide
uniform heat transfer between the graphite and the environment. Just
as in ordinary metal coating processes, graphite components having
poorly bonded coatings will sometimes be produced regardless of the
precautions taken. This paper describes the theory and equipment for
a nondestructive infrared method that has been developed for testing
bonds between coatings and graphite. Infrared test results obtained on
bonds between graphite and columbium carbide coatings are also de-
scribed. Application of a special technique made the test independent of
* This paper is based on work performed under U.S. Atomic Energy Com-
mission Contract AT-(45-l)-1830.
1
Senior research scientist and development engineer, respectively, Applied
Physics and Electronics Department, Pacific Northwest Laboratory, operated by
Battelle Memorial
Copyright Institute
by ASTM for rights
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4 Agreement. No further reproductions authorized
GREEN AND DAY ON INFRARED TESTING OF BONDS 5
the specimen surface emittance (often called emissivity). Emittance in-

dependence is important in infrared tests on metal specimens, since the
emittance can vary from one point to another. Such variations would
give false indications of bond defects unless their effects were eliminated.
The basic procedure for carrying out an infrared thermal test is to
apply heat to the test piece and record the temperature response with
an infrared radiometer. By properly analyzing this response, internal
characteristics of the test piece can be determined. The infrared method
used in the present work was based on a previously investigated dual
radiometer method2 that required an expensive continuous tape loop time
delay unit. In the present work, however, tests were carried out by
making two scans with a single radiometer. Measurements in this appli-
cation needed only to be made at a few discrete points on each test
piece. This made it possible to use a relatively inexpensive digital method
to record the infrared outputs at each desired point, and eliminated the
need for a tape loop time delay. The digital data were converted to an
emittance independent test output by means of a computer. To further
automate the test, data could be sent to a computer by means of a
telephone line. However, this refinement was considered too costly for
the present feasibility study.
Discussion
Theory and Selection of Temperature Ranges

Basically the theory of emittance independent infrared testing is
simple. Heat deposited on the surface of a test piece flows inward at a
rate that depends on the thermal resistances of bonds through which it
must pass. As the heat flows inward, the surface temperature of the test
piece decreases. The transient surface temperature is thus related to the
quality of bonds within a test piece. A ratio of temperatures at two dif-
ferent times during the transient gives a good index of bond quality, pro-
vided the times are properly selected.
Practical application of the emittance independent method is not
quite so simple. Proper selection of the test conditions to avoid practical
limitations imposed by saturation, noise, and response time within elec-
tronic components, and to avoid excessive temperature changes within
the specimens is essential. Although an analytical approach to selection
of the test conditions is often a useful guide, empirical evaluation is
necessary for their final determination.
The output signal of an infrared radiometer is a function of the tem-
perature and emittance of the surface it is viewing. The emittance of
metal surfaces often varies from one location to another, and it is neces-
2Copyright by ASTM Int'l (all rights reserved); Mon Dec 26 20:58:32 EST 2011
Green, D. R., "Emissivity Independent Infrared Thermal Method," Materials
Evaluation, Vol. 23, Feb.by1965*, pp. 79-85.
Downloaded/printed
(PDVSA Los Teques) pursuant to License Agreement. No further reproductions authoriz
6 NUCLEAR GRAPHITE
FIG. 1—Radiometer output, E, versus temperature, T, of specimens having

three different emittances.
FIG. 2—Eo versus
Downloaded/printed by TD for specimens at TA = 54 and 44 C.
GREEN AND DAY ON INFRARED TESTING Of BONDS 7
sary to eliminate its effect to obtain the most meaningful results from an
infrared thermal test. Green2 has shown that an emittanee independent
ratio of a function of test piece temperature at two different times can
be approximated from the infrared radiometer output voltages as
where TA sad TD are the temperatures of any given point on the test
piece surface, E* and £s are the corresponding radiometer output volt-
ages, and C is a constant. The accuracy of this approximation depends
«pon how well the test meets the conditions that; (1) emittance of the
FIG. 3—E» versus T» for specimens at T» = 39 C,
test piece surface does not vary rapidly with temperature and infrared
wavelength; (2) the range of specimen temperatures and range of wave-
lengths permitted to enter the radiometer are small; and (3) the ra-
diometer is appreciably cooler than the test piece. These conditions are
met reasonably well for metals in the small range of test piece tempera-
tures and infrared wavelengths involved in the present work. The value
of C was determined empirically by methods described in the selection
entitled "Bench Standard Test Piece."
The optimum range of each test condition is related to other condi-
tions and is not easy to express in general form. A study of the effect of
test piece temperatures, assuming other conditions were constant, was
carried out to assure selection of the proper test conditions for the pres-
ent Copyright
application.byThis
ASTMwasInt'l
done graphically
(all as shown
rights reserved); inDec
Mon Figs.
261,20:58:32
2, and 3.EST 2011
Figure 1 shows the radiometer
Downloaded/printed by output voltage as a function of test piece
(PDVSA Los Teques) pursuant to License Agreement. No further reproductions
8 NUCLEAR GRAPHITE
temperatures and surface emittance. Data from Fig. 1 were used to com-
pute the values for E0, shown in Figs. 2 and 3. Figure 2 shows E0 versus
TD with TA equal to 44 and 54 C. If the test results were truly emittance
independent, the value of E0 at a given TA and TD would be precisely
the same for all emittances. Hence, the three curves for each of the TA
values in Fig. 2 would be coincident. This is approximately true for
values of TD down to 39 C. However, values of TD less than 39 C gave
too small a value for the denominator of Eq 1, and this caused large
errors due to normal errors in the measurement of ED . Hence, it was
necessary to maintain TD above 39 C in the tests. Figure 3 shows the
effect of varying TA with TD held at 39 C. Here again, emittance inde-
FIG. 4—Emittance independent infrared bond test.
pendence is shown by approximate coincidence of the three curves.

Although no restrictions on TA are apparent from Fig. 3 it should be
recalled that TA must be greater than the infrared detector temperature
for Eq 1 to be valid. The actual values of emittances in Figs. 1, 2, and 3
were not important as long as they were constant and different, and,
hence, they were not measured. The low emittance surface was bare
aluminum, and the medium and high emittances were produced by
spraying on thin coats of black "Krylon" lacquer. The range of emit-
tances used in Figs. 1, 2, and 3, thus, was between about 0.1 and 0.9.
This is much larger than the range that would normally be encountered
in practical specimens.
General Procedure and Arrangement of Equipment

Basic equipment to carry out the digital dual scan infrared tests com-
prised a specimen
(PDVSA scanner,
Los Teques) an infrared
pursuant to Licenseradiometer, a digital
Agreement. No voltmeter and
further reproductions authorized.
printer, and a heat source. A functional diagram of the system is shown

in Fig. 4.
At the beginning of each test, the test pieces were placed near a pre-
heater block at one end of the scanner, as indicated in Fig. 4, to bring
them to a uniform temperature above that of the radiometer. After
coming to equilibrium with the pre-heater, the specimens were passed
under a fixed spot heat source and an infrared radiometer. Spot heating
on the test piece surface was provided by means of helium gas that was
heated by passing it through a length of electrically heated inconel tubing.
The gas was projected onto the specimen surface from a nozzle. Care was
taken to ensure that the field of view of the radiometer was located at
the point of maximum heating in the heated spot. This was necessary
FIG. 5—Test piece scanner and associated equipment.
since thin coatings have a low heat capacitance per unit area. Tempera-
ture differences, resulting from bond defects under thin coatings on
graphite, rapidly decay below their minimum detectable value after the
bond defects have passed beyond the heated zone. Thus, they would not
be detected unless viewed during or immediately after heating. The scan
made with the spot heat source turned on gave values of TA . Values of
TD were obtained by returning the specimens to the pre-heater for a fixed
length of time and then making a scan with the spot heat source turned
off.
Scanning System
The scannerbyemployed
Copyright ASTM Int'lthe
(all bed
rightsof a smallMon
reserved); screw
Deccutting latheEST
26 20:58:32 as 2011
the
basicDownloaded/printed
unit. Test pieces bywere mounted on the tool carriage which was
driven with the
(PDVSA Losoriginal lead screw
Teques) pursuant at a speed
to License of approximately
Agreement. 1 in./s. authori
No further reproductions
10 NUCLEAR GRAPHITE
Figure 5 shows the scanner logic circuits. The pre-heater block, gas
heating furnace, and the infrared radiometer can also be seen.
Trigger pulses, to command digital printout of the radiometer output
at discrete locations along the specimen, were generated by a wheel
fastened on one end of the scanner lead screw. A photocell placed on
one side of the wheel viewed a light source on the other side once per
revolution through a hole drilled near the rim of the wheel. The wheel
and photocell assembly can be seen on the right end of the lead screw in
Fig. 5. Each revolution of the lead screw advanced the specimen ^ in.
Pulses from the photocell were passed through electronic logic circuits
to give an output of one pulse per one, two, or four photocell pulses,
depending on a selector switch setting. Hence, the digital printout was
actuated at intervals of ^, 34> or /^ m- along the specimens. The re-
producibility of these locations was estimated to be better than ±0.005 in.
Constancy of the scanning speed is essential for meaningful test re-
sults. Logic circuits were used to blank out the pulses commanding the
printer and thus allow an initial scanning distance of 5 in. for the scanner
to reach full speed before starting the data printout. The test piece
carriage mount was drilled to reduce its weight and ensure that full speed
would be reached prior to the beginning of data output.
A timer was provided to assure a uniform time between the TA and
TD scans; startup for the TD scan was automatic. The same relative time
along the temperature transient was used in different tests to ensure the
absolute ratio outputs, E0 given by Eq 1, were meaningful indexes for
comparing bond quality in different batches of test pieces.
The pre-heater block, used to bring the test pieces to the desired initial
temperature, can be seen above the ways on the left end of the lathe
bed in Fig. 5. This block was held at a temperature of 69 C during the
tests. The initial temperature of the test pieces was approximately 44 C
due to their proximity to the block.
Radiometer and Digital Recording System

A Barnes model R8T1 infrared radiometer was used to detect test
piece surface temperature changes. This unit employs a germanium im-
mersed bolometer as the infrared detector and has a noise equivalent
temperature of approximately 0.05 C for a black body target at 25 C.
An area about !/8 in. in diameter on the specimen surface was viewed
by the radiometer. The band-width used in the present tests was about
10 Hz, as determined by a low pass filter on the output of the radiom-
eter. An internal focusing lamp which projected a light spot on the
specimen at the location being viewed by the radiometer was found to
be convenient in aligning the radiometer and heated region on the test
pieceCopyright
surface.by ASTM Int'l (all rights reserved); Mon Dec 26 20:58:32 EST 2011
Output of the radiometer
Downloaded/printed by was passed from the 10-Hz low pass filter
into a digital voltmeter which was triggered by pulses from the scanner.
The voltmeter output was fed into a digital printer capable of printing
five 6-digit readings per second. Printed output of this unit gave in-
stantaneous radiometer output voltages corresponding to discrete data
points along the test piece surfaces.
Heat Source and Alignment Method
The heat source used in these studies was a jet of helium gas pro-
jected at 27 cfh from a nozzle that had a %6 in. inside diameter and was
placed about % in. from the specimens. Heating of the gas was accom-
plished by passing it through 10 ft of |4 in. outside diameter inconel
FIG. 6—Infrared system for testing bonds between graphite and its coating.
tubing maintained at 765 C. Heat was supplied to the tubing by passing

a current of approximately 90 A through its entire length. The tempera-
ture of the gas impinging on the specimen was about 250 C, as measured
with a thermocouple placed in the stream near the nozzle. This heating
method was inexpensive and was found to be reasonably uniform and
steady when the gas flow was laminar. A pivoted cover was attached to
the gas nozzle to deflect the flow during the TD scan; shutting off the gas
flow completely was found undesirable due to resulting changes in the
heater tubing temperature.
Alignment of the heat source and radiometer was accomplished using
a graphite block coated with U.S. Radium Corp. thermographic phos-
phor. Illumination of the phosphor with an ultraviolet lamp causes it
to fluoresce, and
Copyright by ASTMheating therights
Int'l (all phosphor
reserved);extinguishes this fluorescence
Mon Dec 26 20:58:32 EST 2011
untilDownloaded/printed
it is cooled again.
by To carry out the alignment, the graphite block
12 NUCLEAR GRAPHITE
was placed in the position normally occupied by the surface of the test
pieces. Heat supplied from the gas jet caused darkening of a spot on
the phosphor in the heated zone. The light spot, projected from the
radiometer to mark its field of view, was focused hi the middle of the
heated zone. Figure 6 shows an overall view of the equipment during
alignment.
FIG. 7—Emittance independent bond test of standard which has three defects
and a high emittance area: (top) photograph of standard, (middle) radiometer out-
put, and (bottom) emittance independent plot.
Bench Standard Test Piece

Due to changes in instrument conditions, it was necessary to determine
the value of C in Eq 1 during each test scan. In addition, it was desirable
to provide an index of test sensitivity of each scan to assure that all
equipment was functioning properly. A bench standard test piece, having
both emittance differences and bond defects, was fabricated to fulfill
these requirements.
The bench standard
Downloaded/printed by test piece comprised a 0.005-in.-thick stainless
steel sheet bonded to a massive piece of graphite with W. T. Bean type

RTC epoxy. Bond defects were produced by embedding l/& and lA-in.2
pieces of O.OOl-in.-thick Teflon in the epoxy layer. A defect was also
manufactured by producing a %6-in.-diameter pit approximately % 2
in. deep hi the graphite surface. This pit subsequently filled with epoxy
to produce a low conductivity zone in the graphite. Inadvertant differ-
FIG. 8—Emittance independent bond test of standard which has three built in
defects and randomly spaced high emittance areas: (top) photograph of standard,
(middle) radiometer output, and (bottom) emittance independent plot.
ences in the bond at other locations were detected during subsequent

infrared tests on the standard. The largest of these occurred on the left
end of the standard. Data from tests on this region of the standard were
ignored since they do not represent known conditions.
Emittance differences were produced on the surface of the standard by
spraying black "Krylon" paint in localized areas. Hence both high and
low Copyright
emittanceby areas, as well
ASTM Int'l as bonded
(all rights and
reserved); unbonded
Mon areas,EST
Dec 26 20:58:32 were viewed
2011
by the radiometer during any given scan on the test piece.
14 NUCLEAR GRAPHITE
Test Results
Scans that were made on the standard, to determine the value of C and
to test the sensitivity and emittance independence of the equipment,
yielded the results shown in Figs. 7 and 8. The surface of the standard
with various high and low emittance zones is pictured at the tops of the
figures. Strip chart records of the electrical signals out of the infrared
radiometer during the EA and ED scans are shown in the middle of the
figures. The EA record is, of course, the output one would obtain from an
infrared test without emittance independence. Emittance independent
ratio outputs, computed from the digital data taken at the points indi-
FIG. 9—Emittance independent plot of data resulting from bond tests on

columbium carbide coated graphite.
cated, are shown in the lower part of Figs. 7 and 8. Note that the change
from high to low emittance regions causes little change in E0, while
signal changes resulting from defects do cause E» to increase.
Numerous scans on columbium carbide coated test pieces showed the
necessity of an emittance independent infrared method. Natural emit-
tance differences on the test piece surfaces often gave differences in
radiometer output voltage, EA , that were equivalent to those caused by
bond defects. The emittance independent test output, E0, was not in-
fluenced by these natural emittance variations in the practical test pieces
and thus gave valid indications of bond quality regardless of the surface
emittance variations.
Computations of the values of E0 and C were carried out on a Univac
1107 computer.
Copyright Data
by ASTM were
Int'l (all transferred
rights reserved); to 26
Mon Dec punched cards
20:58:32 EST 2011 rather than
being submitted directly
Downloaded/printed by to the computer on punched tape. This was more
FIG. 10—Columbium carbide coated graphite (X750).
16 NUCLEAR GRAPHITE
economical for the small number of test pieces in the present study since
a longer setup time would have been required for a punched tape com-
puter input. A more convenient arrangement would be to employ a
small built-in "desk-top" computer or to send the data directly into the
memory of a large computer and obtain return computations via tele-
phone lines. This would give nearly real time values for E0. Such an
arrangement would be a necessity for economically handling large
numbers of test pieces.
Practical columbium carbide coated graphite test specimens were
tested using the emittance independent infrared system. Bond defects
were found in some specimens. Figure 9 shows the emittance independent
output, Eo, for the bench standard and two of the columbium carbide
coated graphite specimens. A line drawn through the minimum E0 level
in the standard was used as the unbond threshold level. Specimens show-
ing much higher E0 levels than the threshold were considered to be
poorly bonded. Hence, the E0 values for Specimen 1 indicated that it was
well bonded, whereas Specimen 2 was not.
Destructive metallographic examination on several test specimens gave
bond quality results that agreed with the nondestructive digital dual scan
infrared results. However, it must be pointed out that even the interpreta-
tion of metallographic results on bond quality is not infallible. Photomi-
crographs of the bonds in Specimens 1 and 2 are shown in Fig. 10. These
micrographs indicate that Specimen 1 was well bonded, whereas Specimen
2 was found to have an unbond approximately 0.0001 in. thick. Independ-
ent destructive analyses on other test specimens were carried out at Los
Alamos Scientific Laboratory. Their results also appeared to support the
digital dual scan infrared test results.
Conclusions
An emittance independent digital infrared method was developed for
nondestructively testing bonds between graphite and protective coatings.
The equipment required for the digital method was less expensive than
equipment for the analog method employed in the past. Correlation was
found between the infrared test results and metallographic destructive
analyses on the bonds. Automation of the method for economical pro-
duction application is possible.
A cknowledgments
This program was funded by the Space Nuclear Propulsion Office and
was coordinated through the Los Alamos Scientific Laboratory by G. H.
Tenney.
The authors gratefully acknowledge Dr. Tenney's efforts in defining
the Copyright
scope ofbythis
ASTMwork
Int'land in arranging
(all rights for Dec
reserved); Mon the 26
test20:58:32
specimens. We also
EST 2011
wishDownloaded/printed
to thank R. J. byAusere, E. W. Wallace, and W. H. Payzant who de-
veloped the scanner; W. H. Gray, L. H. Fischer, R. D. Breneman, and

E. F. Perrizo who assisted in the experiments; E. M. Woodruff and
D. H. Parks who vacuum impregnated metallographic specimens in prep-
aration for the bonding studies; and L. H. Hartcorn who supervised the
metallographic work.
B. L. Blanks,1 N. B. Edenborough,1 D. E. Elliott,1
and R. M. Ford1
Nondestructive Testing of Graphite at the

Los Alamos Scientific Laboratory*
REFERENCE: Blanks, B. L., Edenborough, N. B., Elliott, D. E., and

Ford, R. M., "Nondestructive Testing of Graphite at the Los Alamos
Scientific Laboratory," Nondestructive Testing of Nuclear Graphite,
ASTM STP 439, American Society for Testing and Materials, 1968, pp.
18-36.
ABSTRACT: The Los Alamos Scientific Laboratory has investigated and
used radiography, ultrasonics, sonics, eddy current, radiation gaging, and
beta-backscatter gaging for the inspection of graphite and its protective
coatings. Some applications and limitations of these techniques are re-
viewed. The use of ultrasonics, sonics, eddy current, and radiation gaging
to determine physical characteristics, aside from the normal flaw detec-
tion, shows promise in the inspection of graphite. Electron microscopy
has proved to be a valuable tool for the evaluation of the findings of
nondestructive testing.
KEY WORDS: nondestructive testing, graphite, ultrasonics, sonics, eddy
current, radiation gaging, beta backscatter, electron microscopy, physical
properties, moduli, sound velocity, grain orientation, protective coatings
When the Los Alamos Scientific Laboratory started to use graphite

in its experimental nuclear reactor programs, the need for more knowl-
edge of the material was evident. One natural need was how to inspect
it. Nondestructive testing is, of course, one of the inspections needed for
any structural material and for the components made of it.
The safety and economic aspects inherent in nuclear reactor tech-
nology justify a more thorough investigation of all aspects of testing than
in other potential fields.
Therefore, an extensive investigation of possible means of nonde-
structive testing of graphite has been and is being conducted. Most of
the methods used on the more conventional structural materials have
been investigated, and various innovations have been devised. The search
* Work done under the auspices of the Atomic Energy Commission.

1
Alternate group leader, staff member, group leader, and staff member, re-
spectively,
CopyrightGroup
by ASTMGMX-1, Los
Int'l (all rights Alamos
reserved); Mon Scientific Laboratory,
Dec 26 20:58:32 EST 2011 Los Alamos, N.
Mex.Downloaded/printed by
18
BLANKS ET AL ON NONDESTRUCTIVE TESTING OF GRAPHITE 19
has not been confined to the normal flaw-detection approach but has been
extended to a search for methods of nondestructively determining physi-
cal constants which might have bearing on the utility and suitability of
the part. The methods investigated are covered topically along with
the findings for each.
Methods
Radiography
Radiography was one of the earliest methods of nondestructive testing
to be investigated. The findings were reported thoroughly in a previous
article [I].2 Radiography is currently used for the inspection of a num-
ber of reactor components fabricated by, and for, the Laboratory and
is used for flaw detection. The establishment of meaningful specifications
TABLE 1—Relative ultrasonic attenuation factors of various graphite types.
Graphite Type Manufacturer" Relative Attenuation
Factor6
331 1 1
AUC 2 4.5
H4LM 3 49
CS312 2 80
CSBS.. 2 120
ATL 2 210
SX5 4 310
AGOT 1 370
" 1. Stackpole Div., Pure Carbon Co.
2. National Carbon Co.
3. Great Lakes Carbon Co.
4. Speer Carbon Co.
6
These values are approximate.
for these inspections is a continuing process based on the performance

of the parts.
Ultrasonics and Sonics

Graphite was found very early in the investigation to be a poor con-
ductor of ultrasonic energy. Only relatively thin sections can be in-
spected for discontinuities with the normal pulse-echo techniques. A
large variation in the degree of attenuation among the various types of
graphite which have been tested is illustrated by the data in Table 1.
These data were obtained by using a transmitted wave (two transducer)
technique at 2.25 MHz. The relative attenuation factor is that amount
of gain necessary to bring the received pulse height to that of Type 331
graphite.
* The italicbynumbers
Copyright in (all
ASTM Int'l brackets refer toMon
rights reserved); the Dec
list 26
of 20:58:32
references
EST appended
2011 to this
paper.
20 NUCLEAR GRAPHITE
FIG. 1—Model 721 Reflectoscope setup for determining longitudinal sound

velocity.
FIG.by 2—Block diagram of resonance test.
Downloaded/printed
Sound transmission measurements have not been used much for flaw
detection, but they are useful in establishing sound velocity in the speci-
mens. Sound velocity is of interest because of its connection with other
physical attributes of the material.
Various moduli of a material can be determined from its sound
velocity and density. The relationships between sound velocity and
physical properties are given in a number of references, for example,
the Nondestructive Testing Handbook [2]. The density can be determined
nondestructively with radiation gages which will be discussed later. Many
have investigated methods of determining sound velocity [3].
FIG. 3—Bar charts sound velocity versus cracking of modules.
The through-transmission, elapsed-time method of determining sound

velocity is applicable to most graphites. A Sperry 721 reflectoscope
shown in Fig. 1 is generally used. The thickness of the specimen is
limited to about 2 in. due to the attenuation. Greater thicknesses could
be measured with a more powerful pulser. In most cases alcohol is used
as a couplant since it leaves little contamination.
The resonant frequency technique has also been used to measure
sound velocity—in this case, the extensional velocity. A small, lightweight
disk of magnetic material is attached to one end of the specimen. The
disk is excited by an electromagnet driven by a variable frequency gen-
erator. A ceramic pickup attached to the opposite end of the specimen
generates a signal
Copyright by voltage
ASTM proportional
Int'l (all to the
rightsenergy it receives.
reserved); Mon TheDec 26
specimen is supported by
Downloaded/printed at its first and third quarter-length points as
(PDVSA Los Teques) pursuant to License Agreement. No f
22 NUCLEAR GRAPHITE
shown in Fig. 2. To insure that the lowest resonant frequency has been
found, the specimen is momentarily clamped in the center to severely
damp the fundamental frequency. The specimen must have a length at
least ten times its smallest cross-sectional dimension for this technique.
A similar setup can be used to determine the torsional velocity. The
driving disk and the pickup are mounted on the circumference rather than
at the ends of the specimen. Velocities have been determined in graphite
specimens up to 5 ft long in this manner. We have been able to sort
many graphite components into different manufacturing batches using
these methods. In some instances, correlation indicated that the sound
velocity had a bearing on the serviceability of the part. Figure 3 is a
FIG. 4—Block diagram of high power wave generation experiment.
graph showing cracking as a function of sound velocity in a group of

components from a reactor test.
Although conventional electronic pulsing circuits are now available
to produce considerably higher power than the reflectoscope, we are
investigating sources with even more power to penetrate reasonable sec-
tions of low-density graphite. A block diagram of the first attempt is
shown in Fig. 4. The spark gap produces a very strong shock front which
can be received by a standard ultrasonic transducer. The 1 /*/ capacitor
bank in the block diagram was charged to about 3000 V and discharged
through a thyratron.
Although this apparatus produced a shock wave capable of pene-
trating 3.5 in. of graphite having a density of 1.01 g/cm3, the dis-
persion of energy through the couplant, and echoes from the walls of
the container precluded use because of the reduced signal-to-noise ratio.
We believe the device can be refined by collimating and focusing the
source and coating the container walls with sound-attenuating materials.
Eddy Current
Primarily, eddy current inspection has been used for near-surface flaw
detection in graphite. However, conductivity measurements have con-
tributed other useful information. Such measurements have been used
to sort graphites either as a function of composition or treatment, often
FIG. 5—Block diagram of the Universal eddy current tester.
FIG. 6—Small diameter eddy current probe.
a useful step in the fabricating sequence. They have also been used to
determine grain orientation, as will be discussed later.
Our primary tool for eddy current inspection is a system which we
assembled and named the "Universal eddy current tester." A block
diagram of this unit is shown in Fig. 5. The design is such that a coil
may Copyright
be drivenbyatASTM
any frequency from
Int'l (all rights 0.020 Mon
reserved); to 1.5
DecMHz. The search
26 20:58:32 coil
EST 2011
signalDownloaded/printed
can be balanced by to a null in a chosen set of surroundings with the
24 NUCLEAR GRAPHITE
bridge circuit. The imbalance in the bridge, caused by changes in the

coil impedance due to its surroundings, is amplified and displayed both
on an oscilloscope and on a digital voltmeter.
The system can drive coils with a wide variety of designs. The smallest
coil employed for routine inspection is 0.082 in. in diameter. This probe
for inspecting graphite with a small diameter hole is shown in Fig. 6.
With this coil and the system, we have consistently detected discontinui-
FIG. 7—Calibration curve for conductivity measurements, Universal eddy

current unit.
ties equivalent to a 0.035-in.-diameter hole extending 0.025 in. radially

from the bore surface.
The procedure for utilizing the system is as follows:
1. The bridge is adjusted to zero with the coil in air or with a cali-
bration specimen.
2. The amplifier gain is set at a selected voltage level with the coil
in a standard containing a discontinuity of a known size.
3. Routine inspection proceeds on the premise that discontinuities
producing voltages equal to or greater than that of the standard are
worthy of consideration.
The tester has also been used to detect the presence of protective coal-
ings, specifically columbium carbide (CbC) about 0.001 in. thick, on
graphite. The bridge is nulled with the coil on bare graphite. The ampli-
fiers are then adjusted to a 5-V level on a specimen with the greatest ex-
pected coating thickness. Components producing signals below 2 V are
rejected for insufficient coating.
Although the frequency range of the tester, 0.020 to 1.5 MHz, has
been adequate for most graphite inspections, we are now in the process
of increasing the upper limit to 180 MHz. We hope that this extended
range will prove useful in the inspection of very thin protective coatings.
At the higher frequencies, it should be possible to inspect the coatings
with negligible energy penetration into the graphite substrate.
The Universal eddy current tester is also used to make conductivity
measurements. In this application, it is more flexible than a Magnaflux
TABLE 2—Typical conductivity measurements with a rectangular eddy current

probe to determine grain orientation.
Apparent Conductivity, % IACS*
Graphite Type Manufacturea
XY Plane XZ Plane YZ Plane
E24 1 0.047 0.045 0.051

EP192 2 0.080 0.085 0.084
SX^l 1 0 225 0 225 0 170
PO3 3 0.110 0.115 0.142
SX-5 1 0.152 0.150 0.152
0 1. Speer Carbon Co.
2. Poco.
3. Stackpole Div., Pure Carbon Co.
6 Probe dimensions were 0.125 by 0.25 in.
Magnates! FM-102. The range of conductivities which can be measured

with this commercial equipment extends to a minimum of only 0.8 per
cent of the International Annealed Copper Standard, a conductivity
greater than that of most of the types of graphite used by the Los Alamos
Scientific Laboratory. Furthermore, the FM-102 is relatively limited as
to the type of probe which can be used with it.
The Universal eddy current tester is calibrated with specimens of
known conductivity for making conductivity measurements according to
the following procedure:
1. The bridge is adjusted to some convenient level.
2. Standards of known conductivity are placed beneath the probe and
the output voltages of the tester are noted.
3. The output voltages are plotted as functions of the conductivities
of the specimens to form a calibration curve.
4. Copyright
The output
by ASTMvoltages
Int'l (all rightsfrom unknown
reserved); Mon Dec 26 specimens are converted to
20:58:32 EST 2011
conductivities through
Downloaded/printed by the calibration curve.
26 NUCLEAR GRAPHITE
A typical calibration curve is shown in Fig. 7. Conductivities as low

as 0.003 per cent International Annealed Copper Standard (IACS) can
be measured with the equipment. The low conductivity standards are
fabricated from graphite carefully inspected to insure uniformity; their
conductivities are determined by standard laboratory methods.
To detect grain orientation in graphite by conductivity measurements,
a rectangular coil 0.125 in. wide and 0.25 in. long was constructed. The
conductivity of a specimen parallel to the longer dimension of the coil
contributes the major portion of the signal from the coil. The change of
FIG. 8—Radiation gage for measuring graphite density.
conductivity as the coil orientation is changed has been found to be a

function of grain orientation in graphite.
Various types of graphite exhibit different degrees of grain orientation.
In some types, very little grain orientation is observed, while others show
grain orientation in only one plane and some show it in all three planes.
Some typical values of measured conductivity with the directional eddy
current probe are shown in Table 2. A change greater than 0.01 per cent
IACS appears to be indicative of significant grain orientation.
Radiation Gaging
One use of radiation gages is the determination of densities of speci-
mens. For this
Copyright application,
by ASTM Int'l (all it hasreserved);
rights been found that26high
Mon Dec energy
20:58:32 radiation
EST 2011
(about 1 MeV) is desirable because the absorption coefficients are more
FIG. 9—Close-up of radiation gage showing detector collimator.
nearly a function of density at that energy level. The Los Alamos Scien-
tific Laboratory pioneered in the development of this type of gage and
has published several articles on it [4-6].
The densities of graphite specimens up to 4 in. thick have been deter-
mined with such a transmission gage using the gamma radiation from a
cobalt-60 source. As in previously reported work, the gage was empiri-
callyDownloaded/printed
calibrated usingbygraphite standards, the densities of which had been
measured
(PDVSAbyLos
standard
Teques) means.
pursuant to License Agreement. No further reproductions authorized.
28 NUCLEAR GRAPHITE
The gage used for this work consists of a one curie cobalt-60 source
mounted in a uranium shield, primary and secondary collimators de-
signed to restrict the radiation beam to a diameter of approximately % a
in., a stage for scanning the graphite specimen between the two colli-
mators, a gamma detector utilizing a sodium-iodide (thallium activated)
scintillating crystal and photomultiplier tube, and a d-c signal amplifi-
cation and recording system. Basically, the relative transmission of
FIG. 10—Typical scanning trace from radiation gaging of a graphite cylinder.
gamma rays through the specimen is the measured variable in the equa-
tion:
where:
r = per cent transmisssion (ratio of transmitted gamma intensity to
initial gamma intensity),
in = mass absorption coefficient,
p = material density, and
t = specimen thickness.
For a given material, n is constant and t can be measured. Therefore p
can be related to the measured T through the calibrated standards. These
standards are selected from graphites of different densities machined to
size Downloaded/printed
and accurately weighed.
by
The overall error in the density measure-
ments(PDVSA
of suchLos
standards is of the toorder
Teques) pursuant of ±0.25
License per cent.
Agreement. No further reproductions autho
Since a two-dimensional scanner is normally used to position speci-

mens in the beam of radiation, it is possible to determine density varia-
tions within the specimen. A wide variety of scanning patterns can be
selected to cover specimens with simple geometrical shapes. Figure 8
shows the gage described, and named DXT gage since it measures
density times thickness. Figure 9 is a close-up of the unit showing the
detector collimator. Figure 10 is a reproduction of the results of a typical
scanning trace from the unit.
Density measurements have been made on a number of graphite
FIG. 11—Schematic beta-backscatter probe for accessible surfaces.
specimens in the research program of the Laboratory. The total error

in the instrumentation and the calibration standards has been observed
to be about d=0.5 per cent.
Beta Backscatter
As previously mentioned, much of the graphite used in the Los Alamos
Scientific Laboratory's programs is protected from corrosive atmospheres
by suitable coatings. The nondestructive testing of these coatings must be
as exacting as the inspection of the graphite. Beta particle scattering
gages have been used extensively for the determination of the thicknesses
of these coatings.
Copyright Although
by ASTM the principle
Int'l (all rights has Dec
reserved); Mon been26 covered in the
20:58:32 EST 2011 litera-
ture [7-9], some of our engineering accomplishments to adapt the method
30 NUCLEAR GRAPHITE
FIG. 12—Schematic beta-backscatter probe for small diameter bores.
FIG. 13—Calibration chart for beta-backscatter coating thickness measure-

ment.
to particular configurations are worthy of recording along with the im-

provements in accuracy achieved.
When materials are bombarded by beta particles, a portion of the par-
ticles are reflected or scattered back. The amount of reflection or scat-
tering is a function of the atomic number of the materials upon which
the beam impinges (directly proportioned to Z2 and to density). The ap-
plication of this method
Downloaded/printed by to measurement of coating thickness is dependent
FIG. 14—Electron micrograph of extruded graphite (X6000).
on the existence of an appreciable difference in the atomic numbers of

the coating material and the graphite, a condition easily met by the ma-
terials normally used by the Laboratory.
Most of the work has been done so far using strontium-yttrium-90
beta sources and scintillating detectors coupled to photomultiplier tubes.
These gages have been made to inspect the coatings on the bores in small
diameter holes
Copyright by as well Int'l
ASTM as to(allinspect coatings Mon
rights reserved); on easily
Dec 26accessible surfaces.
20:58:32 EST 2011
A cross-sectional schematic
Downloaded/printed by diagram of a beta probe for inspecting easily
32 NUCLEAR GRAPHITE
FIG. 15—Electron micrograph of pyrocarbon deposit (X6000).
accessible surfaces is shown in Fig. 11. Figure 12 is a similar view of a

small diameter bore probe. A quartz light pipe is used to couple the scin-
tillator to the photomultiplier in these probes. The scintillator is shielded
against direct radiation from the source by a 0.015-in. gold foil so that
only the scattered radiation can contribute to the signal.
In the routine inspection of CbC coatings about 0.001 in. thick on a
graphite substrate, it has been found that accuracies of from ±3 to ±10
per cent can be achieved depending on the material and conditions.
Again, an empirical
Copyright by ASTM calibration
Int'l (all rightsofreserved);
the instrument is made
Mon Dec 26 20:58:32for each
EST 2011coat-
FIG. 16—Electron micrograph of adherent coating on graphite (X6000).
ing and substrate. This is accomplished in two ways: (1) by the intro-
duction of foils of the coating material and (2) by metallographic meas-
urement of coatings measured. A typical calibration chart is shown in
Fig. 13.
Electron Microscopy
The data obtained from nondestructive tests are frequently not com-
pletely understandable,
Downloaded/printed by particularly in cases where new materials are in-
volved. We have
(PDVSA frequently
Los Teques) resorted
pursuant to various
to License destructive
Agreement. tests to evalu-
No further reproductions authorized.
34 NUCLEAR GRAPHITE
FIG. 17—Electron micrograph of nonadherent coating on graphite (X6000).
ate the findings of nondestructive tests. Electron microscopy has been

found to be a very useful tool in these efforts. The measurements from
such tests as eddy current and ultrasonics can be explained sometimes
by the fine structure of the material revealed by the electron microscope.
Figure 14 is such a picture of a specimen of nuclear graphite of the type
normally used by the Laboratory, that is, an extruded graphite made of
graphite flourby with
Copyright ASTMa Int'l
binder. The reserved);
(all rights flake structure
Mon Decin26the specimen
20:58:32 is the
EST 2011
flourDownloaded/printed
and the granular by regions are the graphitized binder. The orientation
of the grains can easily be detected. Figure 15, an electron micrograph

of a carbide coating on a pyrocarbon matrix, illusrtates the lamellar na-
ture of pyrocarbon deposits, explaining the vastly different nature of
signals returned from nondestructive testing as compared to those from
conventional graphite. Electron microscopy is indispensable in the evalu-
ation of our protective coating results. Figures 16 and 17 are micro-
graphs showing adherent and nonadherent columbium carbide coatings
on graphite, respectively. Note the intrusion of the adherent coat into the
open pores in the graphite matrix. All these micrographs were made from
shadowed replicas of metallographically prepared specimens.
Conclusion
This paper describes some of the work which has been done in de-
veloping and applying nondestructive testing methods to graphite at the
Los Alamos Scientific Laboratory. Radiography, ultrasonics, sonics, eddy
current, radiation gaging, and beta-backscattering methods are described.
Further development of most of these methods continues. An area which
must be explored more thoroughly is the appraisal of the findings from
these methods. This is perhaps the most difficult portion of the general
field of nondestructive testing. In most instances, it involves a tremendous
amount of very tedious correlation of data to extract the significant in-
formation.
The nondestructive determination of the mechanical properties of
graphite is an area of much promise which is also being pursued by other
workers [10]. It appears to have more applicability to graphite than to
most of the more conventional materials of construction.
Much work remains in the development of nondestructive tests for
graphite, but meaningful tests are now available.
A cknowledgments
The authors wish to express appreciation to their colleagues of Group
GMX-1 of the Los Alamos Scientific Laboratory who have contributed
to the work described in this paper, as well as to many from other labo-
ratory groups who have cooperated in the program.
The contributions of former members of the Group, P. D. Edwards in
the ultrasonic and electromagnetic portions of the work, and G. H. Ten-
ney, now technical advisor on nondestructive testing for the laboratory,
are especially appreciated.
References
[1] Elliott, D. E., Stokes, J. L., and Tenney, G. H., "Radiographic Behavior of
Graphite and Beryllium," Nondestructive Testing, Vol. XX, No. 3, May-June
1962, p. 161.
[2] Copyright
McMaster,by R. C., Nondestructive
ASTM Testing Handbook,
Int'l (all rights reserved); Mon Dec 26 II, Ronald
Vol.20:58:32 EST Press,
2011
New York, 1963, Chapters
Downloaded/printed by 43, 45, and 51.
[3] Kaufman,
(PDVSA Los D. E., "Finding
Teques) Ultrasonic
pursuant Velocity,"
to License Electronics,
Agreement. No furtherJune 1960.
reproductions authorized.
36 NUCLEAR GRAPHITE
[4] Berman, A. I. and Harris, J. N., "Precision Measurement of Uniformity of

Materials by Gamma Ray Transmission," The Review of Scientific Instru-
ments, Vol. 25, No. 1, Jan. 1954, p. 21.
[5] Taylor, G. M., "A High Precision Density Times Thickness Gage," Sym-
posium on Nondestructive Tests in the Field of Nuclear Energy, ASTM STP
223, American Society for Testing and Materials, 1958, p. 231.
[6] Harris, J. N. and Megill, L. R., 'Techniques Used in Measuring Uniformity
of Materials with Gamma Radiation," Nondestructive Testing, Vol. XI, No.
6, July 1953, p. 9.
[7] Basl, G. J. and Soffa, L. L., "Beta Ray Backscatter Techniques and X-Ray
Emission-Film Thickness Measurement," Materials Evaluation, Vol. XXIII,
No. 10, 1965, p. 493.
[8] Zumwalt, Lloyd R., "Absolute Beta Counting Using End-Window Geiger-
Mueller Counters and Experimental Data on Beta-Particle Scattering Ef-
fects," AECU-567, 1950.
[9] Brownell, G. L., "Conference on Absolute Beta Counting," National Re-
search Council, Oct. 1950, pp. 35-44.
[10] Lockyer, G. E. and Proudfoot, E. A., "Nondestructive Determination of
Mechanical Properties of Refractory Materials," Bulletin of the American
Ceramics Society, Vol. 46, No. 5, May 1967, pp. 521-526.
(PDVSA Los Teques) pursuant to License Agreement. No further reproductions autho
J. A. Hendron1
Application of Alcohol Penetrant for

Evaluation of Surface Porosity of
Graphite Inserts for Rocket Nozzles
REFERENCE: Hendron, J. A., "Application of Alcohol Penetrant for

Evaluation of Surface Porosity of Graphite Inserts for Rocket Nozzles,"
Nondestructive Testing of Nuclear Graphite, ASTM STP 439, American
Society for Testing and Materials, 1968, pp. 37-47.
ABSTRACT: Detection of defect conditions in rocket nozzle graphite
components, using clear alcohol as a penetrant, is described as an in-
spection method. Procedure and acceptance criteria used for graphite
with densities of 1.60 to 1.80 are given. Porosity and density evaluation
using standard test blocks is discussed relative to rocket test firing results.
It is concluded that this method is the most valuable single inspection
technique for graphite in this density range when the technique is com-
pared to other common nondestructive tests.
KEY WORDS: graphite, rocket nozzle graphite, alcohol penetrant, de-
fect detection graphite, density measurement graphite
Graphite erosion by hot gases is common to rocket nozzles, high-tem-

perature gas-cooled power reactors, and nuclear rocket reactors. Expe-
rience accumulated in the chemical rocket field for measuring and evalu-
ating discontinuities in graphite may well be useful in the field of nuclear
rockets.
Erratic erosion of graphite components was a major problem in the
initial stages of its use in solid rocket nozzles. Of prime importance, was
the development of an economical and reliable nondestructive test proce-
dure for selection of acceptable material, with broad capability both
qualitatively and quantitatively. The large size of the graphite stock from
which nozzle inserts are cut makes it impossible to expect perfect ho-
mogeneity (Fig. 1).
Defects Which Must Be Detected

Gross porosity (Figs. 2 and 3), wide density variations (Fig. 4), large
inclusions and cracks of any size (Fig. 5) are the most commonly en-
1
Nondestructive testing
Downloaded/printed by engineer, Aerojet-General Corp., Sacramento, Calif.
(PDVSA Los Teques) pursuant to License
37Agreement. No further reproductions authorized.
38 NUCLEAR GRAPHITE
FIG. 1—Normal graphite—Appearance as alcohol drys. Even mottling occurs

as it is near dry.
FIG. 2—Porous area—Appearance as alcohol drys. Affected area remains wet

longer.
HINDRON ON APPLICATION OF ALCOHOL PENETRANT 39
FIG. 3—Porous area—Appearance magnified while dry (same porous area

shown with alcohol in Fig. 2).
FIG. 4—Density
Copyright by ASTMvariation—Appearance
Int'l (all rights reserved); as
Monalcohol
Dec 26 is near dry.
20:58:32 Low density
EST 2011
area Downloaded/printed
remains wet longer.by
40 NUCLEAR GRAPHITE
countered defects. The size and degee of each of these conditions, and its
location in the part, must be evaluated in order to determine whether it
is a rejectable defect. Responsibility for this evaluation commonly falls
to the purchaser. If the purchaser were to insist that the graphite manu-
facturer supply stock with no defects, the cost of the material would be-
come prohibitive. There is a cost advantage in buying large graphite
FIG. 5—Cracked graphite—Appearance as alcohol drys. Cracks visualization

enhanced by lingering wetness around crack as it is near dry.
billets from which multiple nozzle blanks may be cut with occasional
blanks being rejected. This advantage can be exploited if the purchaser
has a reliable method of detecting detrimental defects. Reliability is in-
creased, also, by performing this evaluation on the machined surfaces of
sections or parts rather than on a billet of stock material.
Alcohol Penetrant Most Economical Method

Methyl
Copyrightorbyisopropyl
ASTM Int'lalcohol penetrant
(all rights reserved); testing
Mon Decis26the fastest,
20:58:32 ESTmost
2011 in-
formative nondestructive test used in production inspection of nozzle
HENDRON ON APPLICATION OF ALCOHOL PENETRANT 41
insert blanks and finish-machined graphite parts by Aerojet-General

Corp. Production inspection experience gained over a period of seven
years with no deleterious effects, well establishes this test as nondestruc-
tive.
On a piece of graphite wetted with alcohol, cracks remain wet a little
longer than the surrounding areas, making it possible to see them. Cracks
are often too small to be seen without some type of penetrant fluid, and
common penetrants are not nondestructive in graphite. Starting with al-
cohol as a crack detection practice, an accumulation of observations on
porosity, density variations, and inclusions grew into a knowledge of
graphite characteristics. Other methods of testing were generally found
to be too costly, impractical, destructive, time consuming, or less relia-
ble. Alternative tests are now seldom used except to further examine con-
ditions detected by the alcohol penetrant test.
Procedure for Alcohol Inspection

The alcohol inspection procedure is expressed in a shop specification
in the following words:
1. Brush, flood, or immerse the parts in the alcohol for 5 s min, 10 s
max.
2. Scan the parts as the alcohol evaporates. The presence of cracks
open to the surface will be indicated by a wet line, which is usually con-
tinuous, after the neighboring areas appear dry. Wide or deep cracks will
remain wet longer and will show a wider indication than narrow or shal-
low cracks. Voids open to the surface will cause an area to remain wet
after the surrounding surfaces have dried; the surface wetted will be
slightly larger than the true extent of the voids.
NOTE—If uneven evaporation occurs due to puddling, or the uneven
application of the alcohol, it is permissible to slightly wipe the sur-
face of the part once with a clean absorbent cloth to remove the excess
surface alcohol.
3. Record the results of the visual examination on the inspection re-
port and the location and types of discrepancies on the sketch.
4. Do not release parts for the next operation until parts are dry.
CAUTIONS—Alcohol is highly flammable. "Precautions shall be taken
to prevent fires and explosions."
It is important to train inspectors carefully for this inspection. Judg-
ment is a critical factor in this procedure.
Typical Acceptance Criteria

The acceptance criteria vary for different components and for different
grades of graphite. The same inspection procedure applies to all parts and
is referenced by one procedure number. The differing acceptance criteria
are detailed on each component
(PDVSA Los Teques) drawing.
42 NUCLEAR GRAPHITE
Typical acceptance criteria for two specific parts of different graphite

grades are:
Example I—Molded graphite shall contain no surface cracks, voids,
or inclusions with a major surface dimension greater than 0.060 in. Areas
of porosity shall not have a major surface dimension greater than 0.250
in.
Example II—Extruded graphite shall contain no cracks with a major
surface dimension greater than 0.250 in. Voids or inclusions with a ma-
jor surface dimension greater than 0.100 in. are not acceptable. Areas of
porosity shall not have a major surface dimension greater than 0.500 in.
These acceptance levels are tailored to certain parts relative to their
service. The actual service life (in firing) of the parts covered in these
examples is seldom more than 1 min.
FIG. 6—Alcohol drying appearance—On set of six standard density blocks,

ranging in steps from high density, 1.78 glen? on left to 1.58 g/cm3 on right;
high density blocks dry, low density still wet (all blocks having been wetted simul-
taneously).
Porosity and Density Variation Acceptance Criteria

The same alcohol application procedure applies to evaluation of po-
rosity and density variation. However, there is a difference in interpreta-
tion of results. In detection of discontinuities, the flaws are detected by
observing those distinct areas, or spots, which remain wet longer than
the surrounding material. In checking for density variation, the condition
is evaluated by noting the time of a specimen area to dry. This is com-
pared to the drying time of a standard block of known density; this block
being wetted at the same time as the part being evaluated.
This test is seldom needed. When it is, the inspector is aware of the
condition because of very slow drying time or a mottled appearance dur-
ing drying. In these rare cases, the evaluation for density is performed by
engineering personnel.
The test is best used to render a simple go-or-no-go decision on sus-
pect material. Judging a range of densities is unnecessary. When a part
takes less time to drybythan a standard block of minimum acceptable den-
Downloaded/printed
FIG. 7—Ultrasonic C-scan recording—On 27 graded density graphite standard

blocks. Note correlation between density and sound transmission capability.
Copyright
FIG. by ASTM
8—Alcohol Int'l time
drying (all rights reserved);
tests—On Mondensity
graded Dec 26 graphite
20:58:32 standard
EST 2011
blocks. Charts show closebycorrelation between density and drying time.
Downloaded/printed
(PDVSA Los Teques) pursuant to License Agreement. No further reproductions authoriz
44 NUCLEAR GRAPHITE
sity, it is acceptable. If it takes more time to dry than the specimen, then
the pore size and frequency is too great to resist erosion, and it is there-
fore rejectable.
Selection of Standard Density Test Blocks

Test blocks were procured with a graded series of densities (Figs. 6
and 7). Drying times versus apparent densities were determined for
various dwell time and conditions of ventilation. For densities above
1.65, in a still air environment, the drying rate is reproducible and cor-
relative (Fig. 8). Continued efforts to correlate the controlled alcohol
penetrant with the erosion of full scale inserts deteriorated with time be-
cause the graphite reference blocks change their absorption characteris-
tics with use. Ordinarily each lot of graphite would require new correla-
tion-calibration efforts.
There is a proposed alternative to replacement of test blocks. Contami-
nated test blocks may be cooked at 4000 F in order to remove foreign
materials. This could provide a means of rejuvenating valuable standard
blocks.
It does appear that the alcohol penetrant test can be standardized and
specified. It also appears that the test can reveal small, local areas of sur-
face porosity, and provide the basis for estimation of the erosion re-
sistance and probable functional life.
Studies Relating Density Variations to Erosion Rate

On large graphite sections such as nozzle entrance and throat inserts—
local erosion is the common occurrence, indicating a need for a nonde-
structive test method correlative with the pore spectra. Because alcohol
as a penetrant was studied as a method to detect and evaluate local varia-
tions in graphite, the accumulation of information about alcohol lends
itself to this needed development.
The first phase used a nozzle cap that exhibited a fourfol_d variation in
drying time when the alcohol was applied for 5 s and then blotted. Small
specimens were selected. The open pore spectrum was then measured by
the mercury intrusion method, and the bulk density was measured by the
procedure in ASTM Test for Density and Interconnected Porosity of
Sintered Powder Metal Structural Parts and Oil Impregnated Bearings
(B 328 - 60). The pore spectrum for the specimen with slow evaporation
resembled the spectra from specimens with high erosion rates. The con-
verse was observed for the fast drying, dense specimens.
A long term investigation dealing with the behavior of various grades
of graphite was conducted with subscale, end-burning motors, having a
2.00 by 2.20-in.bygraphite
Copyright nozzle
ASTM Int'l insert,
(all rights with aMon
reserved); throat
Decdiameter of EST
26 20:58:32 0.474 in.
2011
Four extruded and fifteen
Downloaded/printed by molded grades of graphite were included in
the evaluation. Test specimens were developed from the graphite mate-
rial adjacent to the blank from which the nozzle insert was made, to
evaluate the hardness, strength, bulk density, and the open pore spectrum
of the material. The bulk density was calculated from dimensional and
weight measurements, and the pore population was surveyed by the
mercury intrusion technique. From these data, the total volume of sur-
face connected pores and the volume fraction attributed to groups of pore
sizes can be determined.
Analysis of the total body of data showed a correlation of 78.5 per
cent erosion rate with the total pore volume and the volume with pores
having sizes in the range from 5 to 25 /mi. There was no significant cor-
relation with bulk density, hardness, or pore volume for sizes under 5 p.m.
The erosive attack results from chemical action on the binder, this at-
tack being accelerated by the presence of pores large enough to allow
diffusion and surface attack.
It has been suggested that, for different grades of graphite having dif-
ferent applications, it may be desirable to alter the penetrant test by
using a variety of fluids having different viscosities and surface tensions
as well as various methods of application (time, temperature, pressure).
Such an approach might be taken in application of this inspection method
to nuclear fuel elements.
Nondestructive Test Method Comparison

Alcohol penetrant is a surface test. It does not prove that material be-
low the surface is either good or bad. It is a statistical specimen, usually
representative of what would be found if the part were sliced and sec-
tioned. The alcohol will reveal conditions such as voids, inclusions, or
severe density variations. When it does, it can usually be assumed that
they are also present below the surface.
If a large number of parts are involved and the condition observed is
borderline, then it may be advisable to supplement the alcohol test with
X-ray or ultrasonic immersion testing or both. Both are directly applica-
ble by standard methods, providing X-ray penetrameters and ultrasonic
test blocks are machined from sound material of equal density and struc-
ture.
Immersion ultrasonic inspection is performed to further check for in-
ternal structural deviations when the alcohol inspection of the surface
suggests their presence. Absorption of water is prevented by the applica-
tion of a thin, strippable rubber coating which can be easily removed.
Several formulations of natural latex materials can be used for this pur-
pose. A compound of Lotol-NC 356 and "Butvar" dispersion (BR) ap-
pears to have the majority of the desired characteristics. This compound
may be appliedby with
Copyright ASTMa Int'l
brush(all or with
rights suitable
reserved); Monspray apparatus.
Dec 26 20:58:32 ESTThe mate-
2011
rial will cure at roombytemperature (73 F) in approximately 20 min.
Downloaded/printed
Filtered
(PDVSAparticle penetrants
Los Teques) pursuant have beenAgreement.
to License used and No found to be effective
further reproductions authorized.
46 NUCLEAR GRAPHITE
as surface-flaw locators. They were discarded as an inspection procedure

for several reasons; cost, lack of simplicity, greater time, and residual
surface contamination.
Common penetrants such as water soluble fluorescent penetrant leave
water and flourescent material in the part, as contrasted to brief expo-
sure to clear methyl alcohol which evaporates quickly and totally. Such
penetrants are not used because fluids retained in a porous matrix have
been known to cause failure of nozzle components.
Conclusion
Inspection of molded and extruded graphite by wetting with alcohol
shows discontinuities clearly and reliably. Time for drying of alcohol
from the surface (measured in seconds) gives a relative measurement of
porosity and density. This versatile and economical inspection is highly
valued for in-process inspection of graphite rocket nozzle components
and can be a valuable tool when applied to other close tolerance graphite
products, where reduction or detection of cracks and maintenance of
fairly uniform density is necessary to meet production specifications.
A cknowledgments
The majority of work done in the development of alcohol inspection of
graphite was conducted by F. X. Schoner. The associated ultrasonic stud-
ies were conducted by A. P. Rogel.
Compilation of the long term investigations was initiated by R. B.
Oliver, now at Haynes-Stellite Division of Union Carbide. Principal in-
vestigators were L. M. Swope of the Materials Advanced Technology
Department of Aerojet-General Corp. and T. J. Delacy, now at Electric
Boat Co.
DISCUSSION ON APPLICATION OF ALCOHOL PENETRANT 47
DISCUSSION
L. R. Bunnell1 (written discussion)—Have you made any attempts to

determine the minimum crack width detectable by your method? Since
capillary action is responsible for the original uptake of the alcohol, the
visibility of an alcohol-defined crack is probably the prime factor in the
detection of that crack.
Author's reply—Due to the difficulty of producing specimen cracks,
no effort has been made to make such a determination. Analysis of ex-
isting cracks indicate that alcohol sensitivity is sufficient to reveal all sur-
face defects which are detrimental to rocket nozzle graphite.
1
Research engineer, Battelle Memorial Institute, Pacific Northwest Laboratory,
Richland, Wash.
L. H. Fanelli1 and R. D. McKown1
Prediction of Strength of Graphitic

Material by Nondestructive Test
Techniques
REFERENCE: Fanelli, L. H. and McKown, R. D., "Prediction of

Strength of Graphitic Material by Nondestructive Test Techniques,"
Nondestructive Testing of Nuclear Graphite, ASTM STP 439, Ameri-
can Society for Testing and Materials, 1968, pp. 48-60.
ABSTRACT: A material consisting of zirconium diboride, zirconium
carbide, and silicon carbide dispersed in a continuous graphite matrix
was examined by nondestructive test techniques. To improve reliability
of the material, a method of predicting strength was desired. Testing
consisted of bulk density, penetrant, X-ray, eddy current, and ultra-
sonic measurements. These were correlated with compressive and flexural
strength measurements. Penetrant, X-ray, and ultrasonic measurements,
as performed, did not provide any useful information for the prediction
of strength. Bulk density and eddy current measurements correlated
with strength. Since density (and strength) were found to vary significantly
over very short distances within the material, density alone did not pro-
vide sufficient information to predict strength. However, by the use of
a combination of density to determine an average strength, and eddy
current readings to measure local variations in strength, it was found
that the strength of a graphite part could be predicted.
KEY WORDS: graphite, nondestructive testing, strength of materials,
eddy currents, density measurement
The purpose of this investigation was to develop a nondestructive test

technique for predicting strength in order to upgrade the quality of a
low-porosity graphitic material which is used as the throat section in small
liquid propellant rocket motors. This material was shown in prior testing
to vary significantly in strength even in a single batch, and the use of
such a method would permit construction of parts from material of known
strength. The reliability of the throat sections would thereby be improved.
In the development stages of the motor, some throats were subject to
thermal shock cracking, and, less frequently, to spalling of material from
the inner surface. In a separate program, not reported here, it was deter-
mined Copyright
analytically that the cracking and spalling tendencies could be re-
by ASTM Int'l (all rights reserved); Mon Dec 26 20:58:32 EST 2011
1 Downloaded/printed by
Members, Technical Staff, North American Rockwell Corp., Los Angeles,
Calif. (PDVSA Los Teques) pursuant to License Agreement. No further reproductions authorized.
48
FANELLI AND McKOWN ON NONDESTRUCTIVE TEST TECHNIQUES 49
duced by decreasing the scatter of the material strength. Laboratory

testing also showed that the absorption and subsequent rapid expulsion
of moisture contributed to the spalling. To minimize the possibility of
failure of production units by these mechanisms, it then appeared de-
sirable to eliminate from use those throats with higher porosity and lower
strength.
A large scatter in strength values is typical of brittle materials such as
graphite, even of those of highest quality, and is a severe limitation to the
use of such materials in designs which require efficiency plus high proba-
bility of success. Many factors contribute to this scatter, including: (1)
intrinsic lack of any significant plastic flow, so that the strength is de-
pendent upon the amount, distribution, and severity of microcracks,
which act as stress concentrators; and (2) variations in fabrication, which
cause corresponding variations in density, grain size, anisotropy, purity,
and particle bonding from part to part and within one part. It is also
recognized that because of the inherent difficulty in the measurement of
strength of brittle materials, some of the scatter indicated by typical
strength tests is unreal [I].2
The material employed for throats consisted of about 43 per cent (by
weight) of zirconium diboride plus zirconium carbide and 13 per cent
silicon carbide dispersed in a continuous graphite matrix [2]. It was avail-
able as cylindrical billets from which the throats were machined. Normal
inspection consisted of lot checks of chemical composition and compres-
sive and flexural strength, plus 100 per cent inspection by visual, radio-
graphic, and dye-penetrant techniques. The billets also met a minimum
bulk density requirement. This testing yielded what was considered high
quality material but was not selective enough to sort out the strength level
desired.
One method used to sort out the lower portion of the strength distri-
bution curve is to proof test finished parts to some fraction of their break-
ing load. However, this technique was not acceptable, for it has been
shown that the quality of the ware may be reduced by the formation of
microcracks when the applied load is sufficient to break the weaker parts
[3]-
The investigation presented in this paper consisted of the fabrication
of test specimens from billets of material, measurement and evaluation
of the specimens by means of nondestructive test techniques, and cor-
relation with compressive and flexural strength results. Nondestructive
testing consisted of bulk density, eddy current, ultrasonic, X-ray, and
penetrant evaluation. It was desired to study the pattern of strength dis-
tribution within the graphite and to develop a practical means to predict
strength so thatbythe
Copyright desired
ASTM strength
Int'l (all level could
rights reserved); Mon be
Decmaintained by sorting
26 20:58:32 EST 2011
2
The(PDVSA
italic numbers in brackets
Los Teques) pursuantrefer to theAgreement.
to License list of references appended
No further to thisauthorized.
reproductions
paper.
50 NUCLEAR GRAPHITE
or possibly by orientation of the higher strength material into the areas

of higher stress.
Experimental Procedure
Specimen Selection
Compression and flexure test specimens were machined from 3-in.-
diameter by 3 Vg-hi.-long graphite billets. The billets are formed by hot-
pressing, and the laminar graphite crystals are preferentially oriented
normal to the pressing direction, that is, normal to the billet axis. The
compression specimens consisted of a total of sixty-three %-in.-diameter
by l-in.-long solid cylinders. All of the specimens were removed so that
their axes were parallel to the billet axis. Compression testing was, there-
fore, in the "across the grain" (transverse) direction. Sixteen cylinders
(designated Group A) were taken from four different billets. Thirty-five
cylinders (Group B) were taken from a single billet and were of known
location relative to the source billet. The remainder were taken from the
billet used for the flexure specimens.
Flexure specimens consisted of thirty-two % by % by 1%-in. bars,
which were machined from a single billet with the long dimension nor-
mal to the billet axis. This restriction still allows two of the three possible
grain orientations, and both were used. About half of the bars were se-
lected so that the % by 1 %-in. faces were parallel to the billet ends, and,
for the remaining half, these faces were normal to the billet end faces.
In testing, the load was applied to this face of the specimen so that the
stresses for either grain orientation were in the "with the grain" direction.
Test Methods
Density, X-ray, and Penetrant—Test specimens were oven dried and
bulk densities were determined by weighing and measuring. All parts
were X-rayed to detect any gross structural defects and to determine if
this technique is useful to detect or predict strength variations. Because
of their small size, the specimens were immersed in a water mask to pre-
vent undercut. The X-ray voltage ranged from 100 to 150 kV and expo-
sure from 10 to 15 mA min, depending upon specimen size. Focal length
was 48 in., using a 0.5-mm focal spot beryllium window tube. Film den-
sities were compared by means of a transmission densitometer. All spec-
imens were also tested by means of a water-base red dye penetrant for
cracks and for porosity indications.
Eddy Current—Measurements were made with a Magnaflux ED-500
eddy current instrument using a %-in.-diameter probe. This instrument
measures the eddy
Copyright current
by ASTM activity
Int'l (all rights induced
reserved); in a Dec
Mon material by theEST
26 20:58:32 small
2011
primary a-c coil probe. byIn materials of little or no magnetic permeability,
Downloaded/printed
these measurements are a pursuant
(PDVSA Los Teques) direct function
to LicenseofAgreement.
conductivity. In thereproductions
No further absence authorize
of any standards of calibration, one specimen from each of Groups A and

B compression cylinders was used as a datum for comparing eddy current
variations within each group. A technique (frequency, sensitivity, etc) was
selected which produced the greatest range of values throughout each
group. Readings were obtained on both ends and the outer diameter of
the cylinders. Different calibrations were used for end and outside di-
ameter readings because of different surface geometry. The reference
cylinder readings were adjusted midrange on the 0 to 500 unit scale, and
each cylinder was measured at this setting. The two end readings of each
cylinder were averaged and termed the "axial eddy current parameter."
FIG. 1—Technique for comparison of ultrasonic attenuation.
The outside diameter readings were taken at four places, 90 deg apart
on the cylinder, and were averaged.
For the flexure bars, the instrument was similarly calibrated using an
arbitrary reference bar. Readings were taken at twelve places on each
bar, three places equally spaced on each of the four faces. The readings
were considered as "bulk readings" and "breaking-area readings." The
former value was an average of the twelve readings, and the latter an
average of the four center readings at the expected cross-sectional area
of fracture (center point loading was used).
Ultrasonics—A number of measuring techniques are possible using
pulsed high-frequency ultrasonic energy. Since both time and amplitude
information areby available
Copyright ASTM Int'lby
(allthis
rightsmethod,
reserved);relative
Mon Decvalues of acoustic
26 20:58:32 EST 2011ve-
locity, Downloaded/printed
attenuation, surface
by impedance, and internal reflections (known
as "hash") may be determined. Relative attenuation was selected as the
52 NUCLEAR GRAPHITE
most likely indicator of variations in strength, and was the property used
for the comparison of strength. Attenuation comparisons were obtained
with the following equipment: (1) Sperry Model 721 reflectoscope with
Type ION pulser/receiver, (2) Sperry Transigate adapter, (3) Sperry
Transigate recorder output, (4) Automation Industries water immersion
tank and automatic X-Y scanning system, and (5) Alden 19-in. Alfax
X-Y facsimile paper recorder. Figure 1 shows a schematic of the equip-
ment arrangement. The signal reflected from the far surface of the speci-
men was selected from the display by the gating circuit and was trans-
mitted to the recorder output circuit, which discriminated the signal and
supplied the recorder with a proportional signal. Since the attenuation in
TABLE 1—Ultrasonic rating of Group A specimens.
Compressive Bulk Ultrasonic Group-
Specimen No.
Strength, ksia Density, g/cm3 ing at S.O MHz6
D-15 46.2 3.080 A

D-13 45.6 3.092 B
D-14 45.5 3.089 A
D-16 44.5 3.096 A
B-7 39.2 3.087 E
B-6 38.3 3.080 F
A^ 37.6 3.078 E
B-8 34.8 3.052 F
A-l 33.4 3.075 B
C-12 31.9 3.048 F
A-2 31.7 3.078 C
A-3 29.8 3.062 C
C-10 28.9 3.015 E
C-9 28.6 3.015 D
C-ll 27.1 2.994 E
B-5 25.8 3.044 E
a
Arranged in decreasing order of strength.
* "A" ultrasonic designation indicates lowest absorption (highest transmis-
sion).
the water was constant, the changes in signal amplitude from the far side
of the specimen were proportional to the attenuation through two speci-
men thicknesses.
Five ultrasonic readings were obtained for the Group A compression
cylinders in the axial direction (across the grain) at a frequency of 5.0
MHz. The amplication was increased for each recording, starting at a
level which displayed only the cylinders with the lowest attenuation. The
parts were grouped into six categories (A through F) depending on the
recording density. Those with the A rating had the lowest absorption
(highest transmission). Ultrasonic tests of the Group B compression cyl-
indersCopyright
were conducted
by ASTM Int'l in
(allarights
similar manner
reserved); Mon Decexcept thatEST
26 20:58:32 a test
2011 frequency of
2.25 MHz was used.
The (PDVSA
flexureLosbars were
Teques) recorded
pursuant to Licenseusing a frequency
Agreement. of 5.0 MHz.
No further reproductions A suffi-
authorized.
cient number of readings were made to separate the specimens into four
groups based on attenuation. Recordings were examined for both overall
and breaking-area attenuation properties, and the bars were assigned sep-
arate ratings for each.
Compressive and Flexural Strength—Compressive strength was meas-
ured with an Instron testing machine using center loading at a loading
rate of 0.02 in./min. Uniform load distribution was achieved by align-
ment of specimens and by use of cushion pads. All specimens were
ground flat and parallel within 0.001 in. Flexure bars were broken with
center point loading at a rate of 0.02 in./min. All breaks were close to
FIG. 2—Variation of Compressive strength with bulk density.
the center of the bar. To minimize torsional moments, the loaded and
supported surfaces were ground flat and parallel to within 0.0005 in.
Results
Penetrant, X-ray, and Ultrasonics

The specimens were free of cracks as indicated by penetrant testing.
However, the penetrant did not produce any useful information of den-
sity or porosity variations for the graphite tested. Several indications of
a slight amount of porosity did not correlate with low strength and were
probably caused by surface roughness.
TheCopyright
X-ray bydata
ASTMshowed
Int'l (allonly
rights that the Mon
reserved); specimens were EST
Dec 26 20:58:32 free2011
of gross
voids Downloaded/printed
and large cracks. by The densitometer did not produce any useful
data to(PDVSA Los Teques) pursuant to License Agreement. No further reproductions authorized.
distinguish density variations.
54 NUCLEAR GRAPHITE
Table 1 compares the ultrasonic ratings with compressive strength and

density for the Group A cylinders. The A ultrasonic rating indicates
lowest attenuation and was expected to indicate highest strength. With
the exception of the high strength shown by the A rated specimens, there
was virtually no correlation of attenuation with strength or density. The
Group B compression specimens showed even less correlation, and the
flexure bar ultrasonic readings did not suggest the strength level for either
PIG. 3—Bulk density and compressive strength profile of material billet—

Group B specimens.
the bulk or breaking area averages. The ultrasonic data for these speci-
mens are not shown.
Density
Figure 2 shows the variation of compressive strength with bulk den-
sity for all of the cylinders tested. The data are plotted in accord with
most Copyright
investigators, whoInt'l
by ASTM have
(allfound
rights log strength
reserved); Monproportional
Dec 26 20:58:32 to density
EST 2011
for ceramic materials. by
Downloaded/printed A reasonable fit to this relationship is shown. Fig-
ure 3 shows
(PDVSAtheLosbulk density
Teques) and tostrength
pursuant License distribution
Agreement. Nooffurther
the billet from authorize
reproductions
which 35 test specimens (Group B) were extracted. Both density and
FIG. 4—Variation of flexural strength with density.
FIG. 5—Relationship between compressive strength and axial eddy current

parameter—Group A specimens.
strength are seen

Copyright to beInt'l
by ASTM highest around
(all rights theMon
reserved); periphery and to
Dec 26 20:58:32 ESTdecrease
2011 to-
ward the center and toward
Downloaded/printed by the bottom of the billet. Strength varied from
about 27 to 39 ksi as density varied from about 3.04 to 3.13 g/cm3 within
the billet.
56 NUCLEAR GRAPHITE
FIG. 6—Relationship between compressive strength and axial eddy current

parameter—Group B specimens.
FIG. 7—Relationship between bulk density and axial eddy current parameter.
Figure 4 shows the variation of flexural strength with density for the
bars extracted from a single billet. Both grain orientations are identified,
and theCopyright
curve by
appears to generally
ASTM Int'l follow Mon
(all rights reserved); the Dec
log 26
strength-density
20:58:32 EST 2011rela-
tionship. Since the point
Downloaded/printed by of fracture of each bar came from the low den-
sity area(PDVSA
close Los
to the centerline
Teques) ofLicense
pursuant to the billet, a true
Agreement. No strength-density
further reproductions plot
authorized.
would be shifted toward lower density.
Eddy Current
Figures 5 and 6 show the relationship between compressive strength
and the axial eddy current parameter for the A and B groups of cylinders,
respectively. In both cases, the eddy current parameter is seen to increase
with strength. These groups were measured at different times, and the
Group A standard was not available for the Group B measurements, so
that there is no correlation between groups. The outside diameter read-
ings from the cylinders showed a similar variation with compressive
strength with about the same amount of scatter in results. Figure 1 shows
that the axial eddy current values increased with increasing density for
the Group B cylinders.
FIG. 8—Relationship between bulk density and bulk eddy current parameter
for flexure specimens.
The combined effects of sample geometry and grain orientation pro-

duced two distinct sets of eddy current values for the flexure bars. Thus,
plots of eddy current versus strength (or density) produced two distinct
curves displaced from each other but with similar slopes. Based on the
average displacement, one set of data was adjusted so that both sets could
be combined for Figs. 8 and 9. Bulk eddy current parameters were com-
pared with bulk density and are shown in Fig. 8. It is seen that the eddy
current values generally increase with increasing density. The breaking-
area eddy current
Copyright parameters
by ASTM werereserved);
Int'l (all rights comparedMon with
Dec 26flexural
20:58:32strength,
EST 2011 as
both represent measurements
Downloaded/printed by of the same area. These results are shown
in Fig. (PDVSA
9. Except for several
Los Teques) pursuantscattered points, a No
to License Agreement. linear
furtherrelationship is
shown between log strength and the eddy current values.
58 NUCLEAR GRAPHITE
Discussion
Penetrant, X-ray, and Ultrasonics

Penetrant and X-ray measurements, although useful tools for the eval-
uation of macrodefects, did not provide the strength criteria data required
for this study. Penetrant testing is known to be valuable for the detection
of fine cracks in graphite. X-rays, although not sufficiently sensitive to de-
tect fine cracks, are useful to locate gross voids or compositional inho-
mogeneities.
FIG. 9—Relationship between flexural strength and breaking area eddy cur-
rent parameter.
Ultrasonic measurements, as performed in this study, provided vir-

tually no correlation with strength and was not successful in selecting
consistently strong or weak material.
Density
The strength of the graphite material tested has been shown to be sen-
sitive to small variations in density. This is consistent with other investi-
gators, who have found that the strength of porous ceramics is nearly
exponential with porosity, so that for about 10 per cent porosity, the
strength is about
Copyright by half
ASTM ofInt'l
that(allofrights
a pore-free
reserved);body
Mon Dec Although
[4]. 26 20:58:32 the
EST ma-
2011
terial tested contains abyconsiderable amount of additives, the graphite
Downloaded/printed
phase is(PDVSA
continuous, so that
Los Teques) low-porosity
pursuant to Licensegraphites
Agreement.without additives
No further are
reproductions authorized
expected to behave in a similar manner. High strength is desirable for
resistance to fracture, but a high ratio of strength-to-elastic modulus is

even more significant for thermal shock resistance. It has been found for
this material that the ratio of strength-to-modulus appears to be constant
at densities above about 3.0 g/cm3, but that the ratio drops sharply for
lower densities [5]. Thus, in order to maintain high strength and a high
strength-to-modulus ratio, it is desirable to maintain high density (low
porosity).
For certain applications, such as rocket motor throats or leading edges,
failure of some comparatively small portion of the structure can result
in complete failure. Thus, the integrity of the structure may be a func-
tion of some weaker area which is under relatively high stress. Considera-
tion of this factor, in conjunction with the wide variation in strength
which was found along rather short distances within the material, sug-
gests that local strength variations are important. A part several inches
in dimension, if machined from the graphite billets studied in this work,
will include areas of widely varying strength. Although bulk density is
proportional to strength, density measurements will not indicate this
strength variation and thus may not reliably predict strength. As both the
dimensions of the manufactured part and the strength variation within
the source billet increase, the less will bulk density measurements serve
as an indicator of strength.
Eddy Current
Eddy current values have been shown to correlate directly with
strength. Much of the scatter observed is explainable in terms of geom-
etry limitations imposed by the small dimensions of the specimens used.
Also, compression specimens were measured on each end and averaged
for the axial eddy current parameter without knowing if a uniform gra-
dient existed. Examination of broken fragments of the Group B compres-
sion specimens revealed that failure had occurred at the end with the
lowest eddy current reading in about 80 per cent of the cylinders. In
flexure testing the maximum stress occurs at the center of the specimen.
It is seen by comparison of Figs. 6 and 9 that by using only the breaking-
area eddy current readings, correlation with strength in flexure was im-
proved over the compression test results. This suggests the desirability of
obtaining local nondestructive measurements to supplement bulk meas-
urements such as density.
Eddy current readings thus appear useful to study strength variations
in graphite structure, as, for example, to examine critical high stress areas
for low strength. This knowledge can be useful to reject a substandard
part from use or, in some instances, to allow orientation of the part so
that the highest
Copyright by strength
ASTM Int'lareas are reserved);
(all rights used in Monthe high
Dec 26stress regions.
20:58:32 In a
EST 2011
somewhat more sophisticated
Downloaded/printed by approach, it appears feasible to map an in-
formative strength
(PDVSA profilepursuant
Los Teques) of a graphite
to Licensestructure byNomeans
Agreement. further of combining
density and eddy current measurements. Density values would be used to
60 NUCLEAR GRAPHITE
establish an average strength (assuming homogeneity). A predetermined

strength-density relationship for the material, derived from physical test-
ing of small specimens of uniform density, would be required. Eddy cur-
rent readings would be used to either verify homogeneity or indicate the
magnitude of deviations from average strength. Since eddy current read-
ings depend upon grain orientation, a knowledge of the anisotropy of the
material would be required.
It would be informative to learn whether eddy current measures
strength independently of density or by virtue of the density. The eddy
current test of graphite is a means of detecting small changes in electrical
conductivity. In a sintered material such as graphite, conductivity is de-
pendent not only upon the density but also upon the bonding character-
istics between crystals. Although density and bonding characteristics are
interrelated, they are not synonymous. Thus, eddy current measurements
may be more perceptive of strength variations, but the data from this
study are insufficient to establish this factor. One complicating factor is
that the particular material studied contained poorly conducting addi-
tives, so that the material conductivity would vary with the quantity and
arrangement of these additives within the matrix.
Conclusions
1. Strength and density within the material decreased-toward the cen-
ter and bottom of the billet. Compressive strength varied from 27 to 39
ksi within one billet, showing the need for local strength measurements.
2. Strength of the material is sensitive to small variations in bulk den-
sity. Strength increased with increasing density.
3. Strength increased with increasing eddy current values, and a log
strength versus eddy current relationship appears reasonable from the
data.
4. Eddy current measurements provide a method to detect local
strength variations.
5. The strength distribution in a graphite part can be determined by
means of a combination of bulk density and eddy current measurements.
6. X-ray and penetrant testing, and measurements of ultrasonic atten-
uation did not provide any useful information for the prediction of
strength.
References
[/] Sedlacek, R., "Tensile Strength of Brittle Materials," MIL-TDR-64-49, March
1964.
[2] Bortz, S. A., "Physical Properties of Refractory Materials," AFML-TR-66-223,
Air Force Materials Laboratory, Aug. 1966.
[3] Dukes, W., "The Design of Structural Elements with Brittle Materials," Pro-
ceedings of 1964
Copyright Golden
by ASTM Int'lGate
(all Metals MonFeb.
Conference,
rights reserved); Dec 1964, Aug. 1966.
26 20:58:32 EST 2011
[4] Kingery, W. D., Introduction
Downloaded/printed by to Ceramics, Wiley, New York, 1960, p. 621.
[5] "Some Thermophysical
(PDVSA Los Teques)Properties
pursuant toof License
JTA Graphite From
Agreement. No—further
250°F reproductions
to 4000°F," authorized.
Southern Research Institute, Final Report to Rocketdyne, Division of North
American Aviation, Inc., Jan. 1965.
L. R. Bunnell1
Contact Microradiography of Graphite*
REFERENCE: Bunnell, L. R., "Contact Microradiography of Graphite,"

Nondestructive Testing of Nuclear Graphite, ASTMSTP439, American
Society for Testing and Materials, 1968, pp. 61-69.
ABSTRACT: This paper describes the use of contact microradiography
to define and characterize the microstructure of graphite. Contact micro-
radiography uses a thin (20 to 500 /an) specimen in contact with a fine-
grained photographic emulsion. The emulsion has a resolution limit of
1500 to 2000 lines/mm and can be magnified X500 without excessive loss
of detail. Because the source-to-film distance is large (about 10 in.) in
comparison with the maximum specimen-to-film distance, ordinary X-
ray sources can be used. Thus, most of the problems of point projec-
tion X-ray microscopy are avoided. Long wavelength X-rays were used
to examine microcracks and other structural features of graphite speci-
mens 100 yam thick. The microcrack structure and coke particle orienta-
tion were clearly visible. Direct observation of the surface had not fully
defined these microcracks. The technique was also used to locate and
characterize very small amounts of metal carbide in graphite-metal sys-
tems. For example, 10 /urn particles of uranium dicarbide were located in
graphite specimens where photomicrography had shown no carbide.
Vacuum impregnation with liquids opaque to X-rays has proven useful
in defining graphite pore structure. If tetrabromoethane, for example, is
used, short wavelength X-rays provide an image of only the filled pores.
Longer wavelengths then are used to show graphite structure and unfilled
pores. Mixing resins with the tetrabromoethane will immobilize it in the
specimen. Impregnating bulk samples with this mixture before thin sec-
tions are taken permits the investigation of possible access routes for
chemical attack.
KEY WORDS: radiography, X-ray analysis, microradiography, graphite
structure, graphite
Most artificial graphites contain 10 to 30 volume per cent porosity.

The pore structure in graphite is extremely complex and covers a wide
size distribution throughout the binder and filler [I].2 The pores are
classed as closed or open depending on their accessibility. This pore
* This paper is based on work performed under United States Atomic Energy
Commission Contract AT (45-l)-1830.
1
Research engineer,
Copyright by Materials
ASTM Int'l (all Department,
rights reserved); PacificESTNorthwest
Mon Dec 26 20:58:32 2011 Laboratory,
BattelleDownloaded/printed
Memorial Institute,
by
Richland, Wash.
2
The italic numbers in brackets refer to the list of references appended to this
paper. (PDVSA Los Teques) pursuant to License Agreement. No further reproductions authorized.
61
62 NUCLEAR GRAPHITE
structure is somewhat unique in its connected nature; many of these

connected pores probably have their origin in extrusion during manu-
facture. The connected pore system plays a major part in the perme-
ability of the final product. Gas-flow measurements provide necessary
permeability data concerning different graphites but disclose little in-
formation about the flow routes taken by the gas.
In addition to the pore system, graphite contains a complex system
FIG. 1—Experimental setup for contact microradiography.
FIG. 2—Specimen thinning fixture.
of microcracks. Here the term "microcrack" refers to an internal crack

in a coke particle, which may or may not be included in the open pore
system. In view of the profound influence of microcracks on many prop-
erties of brittle materials, more needs to be known concerning the role
of these microcracks in, for instance, the accommodation or arrest of
thermal stress cracking in graphite.
Experimental
Copyrightby ASTM Int'l (all rights reserved); Mon Dec 26 20:58:32 EST 2011
Inmany respects
(PDVSA contactpursuant
Los Teques) microradiography providesNoa superior
to License Agreement. tool
further reproductions autho
for examining such pores and microcracks in graphite. Contact micro-
FIG. 3—TSGBF
Downloaded/printed by graphite: (left) photomicrograph, sensitive tint illumination (X250), (right) microradiograph, 200-»m-
thick Los
(PDVSA specimen, tungsten
Teques) tube,
pursuant to 8License
kV, 15Agreement.
mA, heliumNo
beam path,reproductions
further 10-min exposure (X250).
authorized.
64 NUCLEAR GRAPHITE
radiography is a simple extension of ordinary radiography to the micro

scale. The three main differences making this extension possible are:
1. The film used is a plate type,3 with an extremely fine-grained emul-
sion (resolution limit 2000 lines/mm).
2. The specimen is much thinner, typically 20 to 200 /tin. This
eliminates excessive overlapping of fine details.
3. The thin, flat specimen is an ideal shape for radiography, permitting
a specimen-to-film: source-to-film distance ratio of 10~3 to 10~4. The
smaller the ratio, the smaller the geometrical unsharpness. A simple
FIG. 4—Microradiograph of another area in the TSGBF graphite specimen in

Fig. 3. A small amount of heavy metal is visible. 200-fj.m-thick specimen, tungsten
tube, 8 kV, 15 mA, helium beam path, 10-min exposure (X250).
X-ray source may be used, with only minor provisions for collimation
and no provision for focusing.
The experimental arangement is diagrammed in Fig. 1.
Specimen preparation is correspondingly simple. Specimens may
simply be cut with ganged abrasive cutoff wheels. However, most of our
specimens were prepared by mechanically thinning on abrasive papers,
using the simple fixture of Fig. 2. The brass sleeve is sacrificial, ground
away with the specimen; the specimen is not cemented to the steel plug
but is left free-floating,
Copyright by ASTM resulting in areserved);
Int'l (all rights flat specimen
Mon Decwith sides parallel
26 20:58:32 EST 2011to
0.0005Downloaded/printed
in. or less. by
3
Eastman Kodak High Resolution Plate, Eastman Kodak, Rochester, N. Y.
BUNNELL ON CONTACT MICRORADIOGRAPHY OF GRAPHITE 65
After the specimen is thinned and placed in the fixture shown hi Fig.
1, the film is exposed and processed. The film may then be magnified
and photographed by transmitted light. Magnifications of up to X500
may be used. This magnification limit is imposed by film granularity; cal-
culations of the geometrical unsharpness indicate a slightly higher useful
limit.
FIG. 5—Microradiograph of graphite electrode stock showing open porosity

in white. 200-^m-thick specimen, copper tube, 35 kV, 18 mA, air beam path, 5-
min exposure (X250).
Discussion
A great deal of meaningful information about graphite structure is
available through optical microscopy. Easily seen structural features
include coke particle size, shape, and orientation. The use of sensitive
tint illumination [2] provides an indication of which areas are relatively
graphitic or nongraphitic. The internal alignment of coke particles is also
evident. An example of graphite microscopy is shown in the left side of
Fig. 3, which is a photomicrograph of TSGBF graphite [3]. Sensitive
tint illumination is used in preference to polarized light because the
sensitive tint produces areas of black, white, and gray as an indication
of relative orientation; these are easier to interpret than the black or
white areas seen with polarized light.
Additional information is revealed by microradiography. On the right
side of (PDVSA
Fig. 3 isLosa Teques)
microradiograph of a similar
pursuant to License area
Agreement. No on the reproductions
further same speci-authorized.
men. Microcracks not visible in the micrograph are clearly distinguish-
66 NUCLEAR GRAPHITE
able in the radiograph. Figure 4 is from another area of the same micro-
radiograph, in which a tiny amount of a well-diffused heavy metal is
visible. In view of the high purity of this graphite, the discriminating
power available is well demonstrated.
The pore structure of graphite is also visible by optical microscopy.
Optical microscopy, however, gives only a two-dimensional view of
porosity, and the true shape of a pore is not evident in a section view.
Also, one gains no knowledge of the interconnection among pores.
Staining of pores and cracks by vacuum impregnation of a liquid
FIG. 6—Microradiograph of gas-impregnated SGBF graphite showing open

(white) and closed (black) pores. The black areas in the center are closed pores
inside a coke particle. 100-^m-thick specimen, tungsten tube, 8 kV, 15 mA, he-
lium beam path, 7-min exposure (X250).
containing elements more opaque to X-rays than carbon provides a

specimen which gives a better view of the "open" porosity of graphite
—that is, pores which have surface access. Some investigators [4]"have
used molten sulfur as the liquid. However, tetrabromoethane has a
comparable absorption coefficient and may be conveniently vacuum-
impregnated into the graphite at room temperature, while the sulfur
must be heated. Tetrabromoethane has been used by others inspecting
graphite for relatively large cracks [5].
Proper choice
Copyright of X-ray
by ASTM wavelength
Int'l (all permits
rights reserved); Mon viewing either EST
Dec 26 20:58:32 closed
2011
or open porosity or both.
Downloaded/printed by For Fig. 5 the specimen was radiographed
with a (PDVSA
copper Los
tubeTeques)
excitedpursuant
at 35tokV. Where
License only the
Agreement. open pores
No further are authorize
reproductions
important, this approach, using relatively hard X-rays, eliminates super-

fluous details. Both the open and closed pore structure is visible in Fig.
6, which was obtained by using softer X-rays from a tungsten tube
excited at 8 kV, with a helium beam path.
In cases where a fabricated graphite article is exposed to a corrosive
environment, the porosity directly open to the surface offers the main
route for the attack. For example, if the graphite is covered by a pro-
tective coating, it is important to know how much porosity is available
at a coating defect. If only some of the external surfaces are critical, as
FIG. 7—Microradiograph of CbC-coated graphite showing penetration of ra-

diological stain into porosity beneath coating. 200-p.m-thick specimen, tungsten
tube, 8 kV, 15 mA, helium beam path, 10-min exposure (XlOO).
when surfaces have been created by sampling, these surfaces may be

masked by covering them with resin.4 In such studies of porosity, the
specimen is impregnated with a mixture of resin5 and tetrabromoethane,
which is hardened in place after vacuum-impregnation. A 50-50 (vol-
ume per cent) resin-tetrabromoethane mixture provides high contrast;
the percentage of resin may be increased to produce a harder stain.
The specimen is thinned after the resin cures. Figure 7, made using the
aforementioned method, reveals the porosity beneath defects in a
columbium carbide coating on graphite.
Downloaded/printed
* Fiberlay by
Clear-Cast polyester resin, Fiberlay Inc., Seattle, Wash.
5
Maraglas
(PDVSAType
LosATeques)
thermosetting
pursuantepoxy resin,Agreement.
to License Marblette, No
Long Island,
further N. Y. authorized
reproductions
68 NUCLEAR GRAPHITE
Many of the carbides produced by reaction of metals with graphite

have about the same reflectivity as graphite and thus are difficult to
study by metallography. However, very small amounts of metal in a
graphite matrix can be detected by radiography owing to the very large
difference between the X-ray absorption coefficient of graphite and most
metals. Particles of uranium dicarbide 10 pm or less in diameter are
distinguishable in Fig. 8. These particles were present in a low enough
concentration to escape notice by optical microscopy. Passing the X-ray
FIG. 8—Microradiograph showing uranium carbide migration into graphite

and precipitation there. The dark circular area in the upper right-hand corner origi-
nally contained the uranium. 200-/j.m-thick specimen, copper tube, 35 kV, 18 mA,
air beam path, 10-min exposure (X250).
beam through the entire specimen thickness assists in the detection of

small amounts of metal carbide. The small amounts of heavy metal de-
tectable by contact microradiography are well illustrated in Ref 6.
The extension of the method to three dimensions by the use of a
stereo technique has been described [4]. In cases where a three-dimen-
sional structural view of the graphite is necessary, the stereo technique
is quite successful.
Microradiography, then, is a method for looking at graphite struc-
ture and any metallic inclusions which may be present. The method
servesCopyright
to extend the Int'l
by ASTM information usually
(all rights reserved); Mongained through
Dec 26 20:58:32 ESToptical
2011 micros-
copy. (PDVSA Los Teques) pursuant to License Agreement. No further reproductions authorized.
Acknowledgment
The author wishes to thank E. M. Woodruff for his early recognition
that microradiography could provide certain valuable extensions to the
information learned about graphite through metallography.
References
[7] Nightingale, R. E., Nuclear Graphite, Academic, New York, 1962, Ch. 5.
[2] Pincas, J. and Gendron, N. J., "Microscopy and Structures of Brush Carbons,"
Proceedings of the Fourth Conference on Carbon, Pergamon, New York, 1960,
pp. 687-701.
[3] Nightingale, R. E., Nuclear Graphite, Academic, New York, 1962, p. 185.
\4] Nelson, J. B., "X-Ray Stereomicroradiography of Carbons," Proceedings of
the Fifth Conference on Carbon, Vol. 1, Pergamon, New York, 1962, p. 443.
[5] Kornishin, K. I., "Application of Contrasting Liquids in Roentgenography,"
Zavodskaya Laboratoriya, Vol. 30, No. 4, April 1964, pp. 447-449, (pp. 560-
561 in English translation).
\6\ McClung, R. W., Bomar, E. S., and Gray, R. J., "Use of Microradiography
Combined with Metallography For Evaluation of Coated Particles," ORNL-
3577, Oak Ridge National Laboratory, Oak Ridge, Tenn., June 1964.
A. W. Schultz1
A Novel Infrared Nondestructive Testing

Technique For Determining the
Thermal Conductivity
of Graphite*
REFERENCE: Schultz, A. W., "A Novel Infrared Nondestructive Test-

ing Technique for Determining the Thermal Conductivity of Graphite,"
Nondestructive Testing of Nuclear Graphite, ASTM STP 439, Ameri-
can Society for Testing and Materials, 1968, pp. 70-86.
ABSTRACT: A unique method has been developed for rapidly deter-
mining, nondestructively, the localized thermal conductivity, and ther-
mal diffusivity of graphites near room temperature. The method em-
ploys transient heating and requires access to only one surface of a
solid. It involves heating a small area on the surface of an apparent
"semi-infinite" solid with radiant energy and simultaneously observing
the parabolic-shaped temperature history of this area's center using an
infrared radiometer as the sensor. This history is related to the thermal
inertia of the solid, so that a comparison of it with a history for a "stand-
ard" material will yield the conductivity and diffusivity if the density
and specific heat of the solid-of-interest are known. Typically, the period
of time to generate a measurement is 10 s, and the temperature rise is
less than 10 C. Application of this technique to coated ATI graphite in-
dicates that it is capable of discerning inertia differences equal to 15 per
cent, conductivity differences of 15 per cent, and diffusivity differences
of 10 per cent. Approximately 70 per cent of the error contributing to
these precision values is caused by variability in the applied coating
thickness. Precision could ultimately be expected to increase to about 3
per cent. The probable accuracy of the technique is limited to that of
the standard and is about 9 per cent for an inertia measurement when
calibrated against Armco iron. Three noteworthy features of this method
include: (1) point-to-point conductivity /diffusivity /inertia determinations,
which afford an additional tool for nondestructively evaluating material
variability; (2) extension of its application to poor thermal conductors,
which will increase the method's precision; and (3) probable application
to materials in elevated temperature environments.
KEY WORDS: graphite, infrared testing, nondestructive testing, transient

measurements, thermal conductivity, thermal diffusivity, thermal inertia,
thermal measurements, thermal properties
* Work presented
Copyright in Int'l
by ASTM this (all
paper
rightswas performed
reserved); for26Air
Mon Dec ForceEST
20:58:32 Materials
2011 Lab-
oratoryDownloaded/printed
under Contract No.by
AF 33(615)-3942.
1
Senior staff scientist, Research and Technology Laboratories, Avco Space
Systems(PDVSA Los Teques)
Div., Avco Corp.,pursuant
Lowell,to License Agreement.member
Mass. Personal No furtherASTM.
70
SCHULTZ ON NOVEL INFRARED NONDESTRUCTIVE TESTING TECHNIQUE 71
The high degree of reliability that must be achieved in designs for

today's critical applications has given rise to a need for the nearly total
determination of property variability within materials. Nondestructive
methods for measuring properties and their variabilities have become
essential for providing the necessary degree of confidence to be placed
in the integrity of finished hardware. A material exhibiting a high degree
of variability and which is widely used both in thermal and nuclear
applications is graphite. Because of the current interest in graphite, a
nondestructive method for measuring certain thermal properties of this
material has been a development goal undertaken by this author. The
result of this effort is a new technique for rapid, nondestructive measuring
of thermal inertia (kp Cp}, within a localized area, from which the
thermal conductivity and diffusivity of graphite can be derived, the
determination of variability in these properties being limited principally
by the measurement precision of the technique. A desirable consequence
of this study is that the technique can be extended to include essentially
all solids, in a variety of geometrical shapes, and, with modification,
may also prove useful for high-temperature measurements.
The technique consists of heating, for a few seconds with radiant
energy, a small area on the surface of a semi-infinite solid and simul-
taneously observing, with an infrared radiometer, the characteristically-
shaped temperature history at this surface. Since the temperature rise
is limited to the order of 10 C above room temperature, the technique is,
indeed, nondestructive. Analysis of the resulting history record and
companson of it with the record for a standard material yields the
inertia value for the material of interest. Conductivity and diffusivity are
derived from the inertia value by determining density, with the use of
other nondestructive tests, and by applying a characteristic specific heat
for the material. For graphite, only density need be known. Because
of the comparative nature of the method, measurement accuracy is
essentially limited to that of the reference standard.
We believe that before this study direct nondestructive measurements
of the so-called thermal inertia (kp Cp) and determinations of the con-
ductivity (k} and the diffusivity (k/p Cp) have not been performed.
Also, since we believe the technique proposed for performing these
measurements is itself unique, I will proceed by outlining the funda-
mentals of the method in such a way as to incorporate certain experi-
mental aspects involved in the development. The results reported here
are for ATJ graphite, the testing of which is but a part of a larger effort
being conducted to validate and evaluate the technique for a wide
range of materials.
Fundamentals
The (PDVSA
following
Los four relationships
Teques) formAgreement.
pursuant to License the basisNooffurther
the method intro-
duced in this paper:
72 NUCLEAR GRAPHITE
The first relationship describes the temperature behavior of a surface

while the solid absorbs a constant heat flux Q.2 The quantity T is the
temperature of this surface above an initial ambient temperature T0 ;
k represents the thermal conductivity of the solid, a its thermal diffusiv-
ity, and t the time during heating. The surface temperature rise generated
by Q is seen to be proportional to the square root of time, so that a
parabolically-shaped history will be a characteristic to be realized.
The second equation is a definition and relates a solid's diffusivity to
conductivity, its density (p), and its specific heat (Cp). The third rela-
tion expresses a boundary criterion to be adhered to for all measure-
ments. The relation implies that a solid appear dimensionally semi-
infinite to heat flow during the period of simultaneous heating and
observation, L« being the distance into the solid at which semi-infinite-
ness still exists after a heating time t.3 Moreover, so that negligible
lateral heat-flow loss occurs, theory requires that the heat-flow front
be unidirectional and spatially uniform in intensity. The fourth equation
is a modified form of the well-known Stephan-Boltzmann law and
describes the rate of heat loss, or radiance W, emitted from a warm
surface, at temperature T, to a cooler surface or environment at T0.
The quantity eT is the total radiant emissivity of the surface, and the
quantity a is the Stephan-Boltzmann constant. Also included in Eq 4 is
the approximate form of the radiation law. This is the form most con-
venient to use when the surface temperature rise is small, as is the
case in this study. For a rise of 10 C above room temperature, the dif-
ference between the exact fourth power and the approximate forms is
4 per cent. Within this error, the radiance emitted from a surface heated
a few degrees above ambient is proportional to its temperature rise and,
thus, is also proportional to the square root of the time during heating.
Since an infrared radiometer was selected as the most practical sensor
of radiation near room temperature, modification of these basic equa-
2
Carslaw, H. S. and Jaeger, J. C., Conduction of Heat in Solids, 2nd edition,
Oxford,Copyright
London,by1959,
ASTMp. 75.
Int'l (all rights reserved); Mon Dec 26 20:58:32 EST 2011
3
Beck, J. V. and Hurwicz,
Downloaded/printed by H., "Study of Thermal Discontinuities and Asso-
ciated Temperature
(PDVSA Los Disturbances
Teques) pursuant in ato Solid Subject
License to a Surface
Agreement. Heat
No further Flux, Partauthorized.
reproductions
II," Avco Technical Report, TR-9-59-14; 28 April 1959, p. 9.
tions is necessary in order to incorporate typical characteristics of such a

detection system. The formulations sought are those that relate radiome-
ter-produced signal voltage to the period of heating, the resulting history
being correctable with the thermal inertia of a solid, from which value
conductivity and diflusivity are determined. The following four expres-
sions transform the fundamentals into a practical relationship for
measuring the inertia.
where:
and
Equation 5 serves to transform the radiant energy (W'}, emitted

from a surface and entering the optics of the radiometer, into an elec-
trical voltage (V) by means of the conversion constant (K). W is analo-
gous to W in Eq 4, except that W includes the mechanism within the
radiometer for producing a signal. This mechanism involves alternate
sampling of (1) the specimen and (2) a radiation reference source; the
output signal being proportional to the difference between the two
radiation levels.
Equation 6 relates the radiant flux (Q) absorbed at the surface to the
flux (F) incident to the surface. The proportionality constant aT is the
total radiant absorptance of the surface. An important assumption is
made in order to account for emissivity differences between surfaces.
Surface heating is assumed to be caused principally by the infrared
wavelength region of the incident radiation spectrum. This infrared
region and the infrared spectrum emitted by a surface as its temperature
increases from ambient are considered to be contained within a detect-
able spectral region for which emissivities are equivalent. Consequently,
the flux absorbed by the surface can be expressed in terms of the incident
Copyright
flux and the by ASTM Int'l
spectral (all rights reserved);
emittance Mon Dec 26 20:58:32
(e\) corresponding to theEST detectable
2011
infrared(PDVSA
region. Moreover, if the solid were assumed to be opaque to
Los Teques) pursuant to License Agreement. No further reproductions authorized.
the incident radiation, then the fraction of the incident flux reflected
74 NUCLEAR GRAPHITE
from the surface into the radiometer would be simply r\F, where the
reflectance r\ is defined in Eq 6. The self-emitted radiation W is super-
posed on this constant reflected radiation, and the signal voltage gen-
erated is the sum of these two components. Unless filter techniques are
used to minimize the reflected component, this superposition will
normally create the undesirable situation of low signal-to-background.
As will be shown, however, this superposed signal is separated elec-
tronically into its components and is used advantageously to permit
both the emissivity and the thermal inertia to be measured during the
same test run.
Combining these several equations and solving for the self-emitted
signal yields Eq 7, which is a voltage history of parabolic form analogous
to the surface temperature history and which incorporates the several
practical aspects of the technique into the theory. The quantity VA
represents the signal that corresponds to the difference between ambient
temperature T0 and the radiometer reference-source temperature T0'.
Two interesting facets to be noted from Eq 7 are: (1) that the constants
C and VA are independent of any characteristics of the solid and (2)
that the shape of the history curve is dependent essentially on the radia-
tion flux, the emissivity, and the thermal inertia. A higher flux, a higher
emissivity, or a lower conductivity tends to increase the width of the
parabola and, consequently, the signal voltage. At the same time, the
VA term causes the vertex of the parabolic history to be suppressed
below an observable signal level, which is to say that V must be positive
for observability to be realized. The resultant observable history shape
is thus distorted, although the characteristics of a parabola are main-
tained. Since vertex suppression arises out of using a radiometer that
has a reference source temperature greater than ambient, a reference
source temperature equal to, or less than, ambient will eliminate this
effect. Vertex suppression is a most important consideration when
either the thermal inertia of a material is large or the incident flux and
surface emissivity are small, as compared with the period of heating,
the net effect being to produce a weak signal.
Equation 8 follows directly from Eq 7 and yields the voltage difference
along a solid's history curve within the time interval t\ to tz. This ex-
pression provides the basis for experimentation and analysis. Since Eq
8, by itself, requires knowledge of the flux in order to obtain the inertia,
a comparison is made between the histories for a material of interest,
labelled a, and that for a standard material, labelled b, in order that
knowledge of the flux becomes unnecessary if identical experimental
conditions are used in each case. The comparative expression for the
corresponding
Copyright byvoltage differences
ASTM Int'l (all rightswithin theMonsame
reserved); time
Dec 26 interval
20:58:32 EST is
2011
shown in Eq 9. It is seen that measurements of surface reflectances and
voltage differences, within a time interval during which the criterion
FIG. 1—History representations to illustrate aspects of the theory.
of semi-infiniteness can be realized, are all that are necessary for de-
termining the localized thermal inertia of a solid,
To obtain the thermal conductivity and diffusivity of a solid, Eq 9 is
restated in Eqs 10 and 11 in the appropriate forms. It is seen that for
determinations of either k or a, the volumetric heat capacity (pCp) of the
material of interest must be known:
Other nondestructive test methods can be used to determine localized
76 NUCLEAR GRAPHITE
density values, and Cp is an atomic or molecular quantity that can be

predetermined for the particular chemistry of the material. Fortunately,
for manufactured graphites, Cp can be considered constant when com-
paring two sections either of the same or different grade;4 thus, only
density measurements need be performed. Furthermore, it follows that
if conductivity can be uniquely correlated with density, then only a
density measurement need be made in order to determine conductivity.
FIG. 2—Recorder deflection (signal voltage) for time difference of 0.1 s,

at a time base = 1.0 s for a parabolic function.
History Curve Analysis

Before describing some of the experimentation performed and the
results, I will present idealized illustrations of the types of histories
generated, as well as the graphical procedure used to analyze these
histories. Figure 1 shows three histories presented in a way that empha-
sizes important aspects of the theory. The histories are depicted by
parabolically shaped curves exhibiting signals that contain system
* The Industrial Graphite Engineering Handbook, Union Carbide Corp., 1964,
p. 5B.05.01.
noise, as within the time interval h to t2, as the curves would appear
on a recorder chart. Of interest is the fact that the steeper the slope of
the curve, the smaller the value of thermal inertia. The three curves,
labelled A, B, and C, originate at a common vertex, corresponding to
the initiation of the heat pulse at ambient temperature, and then rise to
a voltage level corresponding to the radiometer reference source temper-
ature, only above which can their values be observed. Curves A
and B are unaffected by the suppression of their vertexes within the time
interval noted; therefore, the ratio of the voltage differences for A and,
say, for the standard B, can be read directly as the ratio of thermal
inertias. Curve C, on the other hand, lies partially within the zero level
of the system noise. Because of this, the curve will appear to be more
linearly than parabolically shaped and cannot be compared directly
with the voltage difference of the standard. The required correction
consists of adding to the measured voltage (F2c) a voltage equal to
V\c . From geometrical characteristics of a parabola, V\c can be ex-
pressed by the relationship shown in the figure. The sum of V\c and
Vic can then be compared with the voltage difference for the standard
material.
A convenient scheme for determining whether a history is indeed
parabolically shaped is to display the history logarithmically. The ad-
vantage of this type of display over a rectilinear display is that the former
facilitates both the determining of the latus rectum of a curve, as well
as the comparing of experimental and theoretical curve shapes, in order
to ensure that the curve segment measured conforms with theory. The
logarithmic equivalent of a parabolic curve is a straight line having a
slope equal to one half (see Fig. 2). Since only a segment of a curve is
measured to obtain voltage difference, this segment translated to loga-
rithmic scales will appear not as a straight line, but as a curve whose
shape depends upon the time selected after pulse initiation for beginning
the analysis interval. The figure includes characteristic curves for any
parabolic segment beginning at 0.9, 1.0, and 1.1 after pulse initiation
and ending at 4.5 s. These curves, when overlayed on data points ob-
tained from within corresponding segments of any history, will match
exactly if the experimental segment exhibits characteristics of a parab-
ola. Should, for example, the solid not behave semi-infinitely within a
selected time interval, or should the history curve be partially obscured
by vertex suppression, then the plotted data would exhibit, in either
case, a curve shape having a slope greater than that for semi-infiniteness.
The shaded area between time bases of 0.9 and l.ls indicates the region
of possible curve
Copyright shapesInt'l
by ASTM that
(allcould result from
rights reserved); Mon an
Decerror of 0.1EST
26 20:58:32 s in2011
deter-
miningDownloaded/printed
when pulse initiation
by occurs. Accordingly, anomalies in test
technique can Los
(PDVSA be easily
Teques) assessed.
78 NUCLEAR GRAPHITE
FIG. 3—Schematic diagram of the experimental arrangement used to measure

the thermal parameter k/o C P .
Experimentation
Because of the uniqueness of the technique, considerable experimen-
tation was performed on several materials in order to provide sufficient
evidence of technique validity and to determine its limitations. Since
graphite is of principal interest, a description of work performed will be
limited to this material.
Apparatus
A schematic diagram
Copyright by of the
ASTM Int'l (all experimental
rights reserved); arrangement used toEST
Mon Dec 26 20:58:32 meas-
2011
ure thermal inertia is by
Downloaded/printed shown in Fig. 3. The radiant source consists of
(PDVSA Los
two type-CYS, 1200Teques) pursuant to License
W, projection lamps, Agreement.
each lampNobeing
furtherfocused
reproductions
by authorize
means of an ellipsoidal mirror. The lamps are focused into a radiation

collector-homogenizer-intensifier unit, consisting of a large aluminum
block, into which has been machined a funnel shape having dimensions
comparable to that of a 125-ml erlenmyer-type flask. (This unit is not
shown in the figure.) The surface of this funnel shape is highly polished.
Radiation from the lamps is reflected many times from this surface and
is thus intensified such that a nearly homogeneous radiant flux is avail-
able at the exit port. This flux has a diameter of % in. and an intensity
FIG. 4—(top) Self-emitted radiation history and (bottom) total infrared radi-
ant signal received by radiometer.
of about 6 cal/cm2/s (120 W/in2). Between this intensifier unit and the
radiant source is a shutter system that permits the radiation from the
lamps to be brought to a constant output level before specimen heating
is initiated. Approximately 4.5 s are required for both the filaments and
the glass envelope of a lamp operated at 120 V to reach a constant out-
put. An electronic interval timer and a time delay relay are used to
energize the lamps and actuate the shutter system. Specimens are heated
for about 5 s; thus, the total elapsed time for a run is about 10 s.
Surface temperature
Copyright rise(all
by ASTM Int'l is rights
monitored using
reserved); a Barnes
Mon Dec Engineering
26 20:58:32 EST 2011 Co.,
Industrial Infrared Radiometer, Model R4D1. The radiometer field-of-
view is adjusted to about % 6 in. diameter at the center of the area under-
80 NUCLEAR GRAPHITE
going heating. The ratio of this diameter to that for the heated area is
small enough for plane parallel heat flow into the solid to be nearly
realized, from the viewpoint of the radiometer, during the heating pe-
riod. The radiometer reference source temperature is about 5 C above
ambient in this application; thus, the specimen surface temperature
must exceed this amount to be observable.
The signal generated by the radiometer is recorded using a Brush
Instrument Co., dual-channel recorder. One channel features a cali-
brated zero-suppression, or voltage offset, control, making the elimina-
tion of the reflected radiation component possible by simple voltage
subtraction. This offset channel permits the self-emitted, information-
hearing component to be observed with optimum sensitivity. The sec-
ond channel is used to observe the superposed, two-component signal
FIG. 5—Superposition of self-emitted radiation histories of copper, aluminum,

graphite, steel, and lead.
from which emissivity is determined. This recorder also features variable

chart speeds up to 200 mm/s thereby affording flexibility in readout
analysis. Timing is accomplished by a time-mark trace included in the
chart readout.
Specimens
The graphite selected for study was Type ATI, obtained in billet form.
Since only laboratory tests have been performed to date, specimen
geometries have been controlled to the extent of evaluating technique
capabilities. For example, to determine the semi-infinite dimensions for
graphite, for the time interval selected for analysis, specimens having
various thicknesses and diameters were systematically tested. To deter-
mine the extent to which conductivity is affected by density, a series of
finite, Copyright
1-in. cube-shaped specimens
by ASTM Int'l were
(all rights tested Mon
reserved); in order that20:58:32
Dec 26 their densi-
EST 2011
ties could be uniquelybycorrelated with conductivity. Moreover, the de-
Downloaded/printed
gree of(PDVSA Los Teques) pursuant to License Agreement. No further reproductions authoriz
grain orientation was also determined using these specimens.
PARAMETERS: NOTE:
1. LAMP VOLTAGE = 120V 1. SOLID LINES INDICATE

2. COATING: 3M VELVET BLACK THEORETICAL CURVE
3. NO. COATS = 1 SHAPES FOR PARABOLA
4. SPEC. DIAM. = 2 INCHES FOR TIME BASE = 1.0 SEC.
5. TIME BASE AFTER PULSE 2. DASHED LINES INDICATE
INITIATION = 1.0 SECOND THEORETICAL CURVE SHAPES
FOR STRAIGHT LINE FOR
TIME BASE =1.0 SEC.
FIG. 6—Effect of specimen thickness on recorder deflection for AT] graphite

(against grain).
But regardless of the specimen geometry, in this work each surface

undergoing heating had to be coated with a high-emissivity paint in
order to increase radiation absorption. The coating selected was 3M
Brand, Black Velvet, No. 101-C10, which is purchased in a spray con-
tainer. The coating emissivity as applied here, was estimated to be 0.96.
I should point by
Copyright out thatInt'l
ASTM inherently low-A: coatings,
(all rights reserved); Mon Dec 26 when
20:58:32applied
EST 2011to high-£
materials, tend to inhibit
Downloaded/printed by heat flow; the observed effect of this retarda-
tion is (PDVSA
initiallyLostoTeques) pursuant to License Agreement. No further reproductions authorized.
distort the shape of the temperature history. This dis-
82 NUCLEAR GRAPHITE
tortion, however, can be neglected after a suitable time, the principal

advantage of increased heating thus outweighing several of the disad-
vantages. One obvious disadvantage of using any coating is the control
problem for applying it to a surface. For the results described here, only
reasonable care in applying the coatings was taken; thus, variability in
coating thicknesses is a significant aspect of measurement precision. The
average coating thickness applied was estimated to be approximately
y20 mil.
History Characteristics
Figure 4 illustrates typical histories generated by the system, including
(I) recordings of just the self-emitted component for a semi-infinite,
coated-graphite specimen, and (2) recordings of the superposed reflected
and self-emitted radiation components. Pertinent characteristics are
noted in the figure. The superposed history in the lower channel is used
to determine the emissivity correction for the specimen, the correction
being a relative one, serving only to normalize the flux absorbed at the
surface to some convenient constant value. The value of using a re-
corder that features a voltage-offset control is seen in the upper channel.
The reflected component has been subtracted from the total signal, and
the remaining self-emitted component has been amplified by a factor
of 10. This particular specimen was heated to approximately 15 C above
ambient.
An additional illustration of self-emitted histories for several materials
is shown in Fig. 5. This superposition was drawn from actual histories
to indicate the relative signals obtained for different values of thermal
inertia. Copper is seen to have the greatest inertia value, and lead the
smallest.
Results
Some results for graphite are shown in order to demonstrate capa-
bilities of the technique. In Fig. 6, histories for several thicknesses of
graphite have been generated in order to determine that thickness which
can be regarded as exhibiting semi-infiniteness in the time interval be-
tween 1 and 4.5 s after pulse initiation. Notice that the signal voltage
differences (recorder deflection differences) decrease as thickness in-
creases, up to about \1A to l J /2 in. where the rate of increase tends to
level off. When a further increase in thickness no longer changes the
signal voltage differences, the condition of semi-infiniteness has been
realized. An additional important observation should be made: the ex-
perimental data are seen to exhibit a steeper slope as thickness de-
creases, that is,byasASTM
Copyright the specimens appear
Int'l (all rights more Mon
reserved); finite.
DecThe dashed curves
26 20:58:32 EST 2011
drawnDownloaded/printed
through the data by correspond to a theoretical segment for a time
base equal to 1 s for a straight-line function rather than a parabolic
PARAMETERS: NOTE:
1. LAMP VOLTAGE = 120 V 1. BOTH THE SOLID AND DASHED 3. THE DASHED LINES INDICATE
LINES ARE CURVE SHAPES WITH-THE-GRAIN ORIENTATION
2. COATING: 3M VELVET BLACK DERIVED FROM A STRAIGHT OF THE CUBES.
LINE FUNCTION FOR A TIME
3. NO. COATS = 1 BASE= 1.0 SEC. 4. CORRECTION FOR REFLECTANCE
LESS THAN 0.5 PERCENT FOR
4. SPEC. DIMENSIONS: 1-INCH CUBES 2. THE SOLID LINES INDICATE EACH CUBE
AGAINST-THE-GRAIN ORIENTATION
5. TIME BASE AFTER PULSE OF THE CUBES.
INITIATION = 1.0 SECOND
FIG. 7—Illustration of the ability of the system to distinguish between ori-

entations and normal density variability of ATJ graphite (for finite geometry).
function. The solid curves drawn through the more semi-infinite data
correspond to a theoretical segment for a time base equal to 1 s for a
parabolic function. Thus, a finite condition can be detected by carefully
noting the shift in history shape from the parabolic form toward the
linear form.
Results of measurements performed on two cube-shaped ATJ speci-
mens are shown in Fig 7. These specimens are grain oriented, have dif-
ferent densities, and appear finite to heat flow. Note that the specimens
are easily distinguishable, both in density and orientation, the solid
curvesCopyright
representing
by ASTM against-the-grain
Int'l (all rights reserved);directions for theEST
Mon Dec 26 20:58:32 two
2011specimens,
and the dashed curves representing with-the-grain directions. The curve
shapes are derived from a straight-line function. To be especially noted
84 NUCLEAR GRAPHITE
RESULTS: NOTES:
1. THE AVERAGE RATIO FOR 1. THE EOUIV. THERM. COND.

k /k
w ag ~ 1 . 3 A T P = 1 . 7 G M / C M 3
2. A 1-PERCENT INCREASE IN
DENSITY GIVES RISE TO APPROXIMATELY
A 3-PERCENT INCREASE IN THERMAL
CONDUCTIVITY WHERE M IS A PROPORT.
CONST. WHICH INCLUDES
THE CONST. Cp FOR GRAPH.
AND AD IS DEFLECTION.
FIG. 8—Effect of density on thermal conductivity of ATJ graphite.
is that signal voltage differences increase as density decreases, implying

that thermal inertia decreases as density decreases.
Assuming that density variability within the cube-shaped specimens
is negligible, we can normalize the finite inertia values to a correspond-
ing set of thermal conductivity values. The conductivities can then be
compared to their corresponding densities. Figure 8 shows the results
of such a comparison
Copyright for
by ASTM Int'l (allarights
setreserved);
of grain-oriented ATJ EST
Mon Dec 26 20:58:32 specimens
2011 having
a selected range of density
Downloaded/printed by values. From straight-line fits to the data, we
observe(PDVSA
that Los
a 1Teques)
per pursuant
cent increase in density
to License Agreement. givesreproductions
No further rise to authorized.
about a 3
per cent increase in conductivity. Scatter in the data is directly attribu-

table to differences in the thicknesses of the coatings applied. We would
expect to find that, for a fixed change in density, increased controls
would result in a somewhat greater increase in conductivity in the with-
the-grain as opposed to the against-the-grain direction. A measure of the
degree of grain orientation is seen in the ratio of with-the-grain and
against-the-grain conductivities. From the figure, an average ratio of
about 1.3 is obtained. This is in remarkable agreement with the gen-
erally accepted, published ratio of 1.33 for highly-oriented, Type ATJ
graphite. Also notable from these results is that the degree of orientation
is apparently not related to density.
Discussion
The discussion here considers the fact that (1) measurement precision
is principally affected by coating thickness variability, and (2) the selec-
tion of a suitable time interval for analysis is influenced by the very
use of a coating. From the original work, we determined that should
the coating thickness variability be controlled to within 15 per cent, the
measurement precision of the inertia for graphite would be comparable to
that normally achieved using standard test techniques to obtain the k, p,
and Cp values. A higher conductivity coating material than that used here,
but still exhibiting a high emissivity, would also increase precision.
A further improvement in precision can be achieved by increasing the
radiant flux incident to a surface. Most improvement, of course, would
result were it possible to eliminate the need for a coating. A flux in-
crease would tend to reduce the need for correcting the effect of vertex
suppression and would provide a more favorable signal-to-noise level
for analyzing histories of high-inertia materials, the correction for vertex
suppression being essentially negligible when a radiometer reference
source is at a temperature that is equal to, or less than, ambient tempera-
ture. Tradeoffs between these interacting variables are necessary in order
to arrive at an optimized technique for a particular situation.
It is also important to point out that when a coating is used a time
interval must be selected that is suitably delayed after pulse initiation
in order to eliminate the effect of heat-flow retardation. This delay,
in turn, makes it necessary to work with larger specimens, because of the
criterion of semi-infiniteness. Thus, improvement in the coating material,
or its elimination, will permit either the testing of smaller, ideal, speci-
mens or of smaller regions within a solid section.
Extension of this method to include other materials is, of course,
entirely feasible. Since measurement precision increases rapidly as inertia
decreases, an obvious
Copyright by ASTMextension of this
Int'l (all rights work would
reserved); Mon Decbe26its20:58:32
application
EST 2011
either Downloaded/printed
to materials having
by low thermal inertias or, almost in general,
to materials
(PDVSAhaving low conductivities.
Los Teques) For dielectric
pursuant to License Agreement.materials,
No further emissivi-
reproductions author
86 NUCLEAR GRAPHITE
ties are uniformly high, and the need for coatings may well be eliminated.
A further extension of the method to include high-temperature measure-
ments is possible, although the present technique would probably re-
quire considerable modification.
The probable accuracy of the present technique is essentially limited
to that of the reference material and is estimated to be approximately 9
per cent when calibrated against an Arnco iron reference standard.
On the other hand, the probable precision error will decrease as thermal
inertia decreases; the present range for inertia being about 9 per cent
for copper to 7 per cent for lead. While derived diffusivity values will
have a comparable error range, derived thermal conductivity values
will have a precision error range approximately twice as great as that
for inertia. As coatings are now applied, thickness variability is esti-
mated to contiibute about 70 per cent of the error to these precision
values. These errors are to be compared to a calculated accuracy of
about 6 per cent for (kp C P ) J / 2 values derived from typical measurement
errors associated with k, p, and Cp values obtained using standard
destructive test techniques. Measurement precision can ultimately be
expected to approach about 3 per cent for low inertia materials.
Application of this technique to semi-infinite, coated, ATI graphite
has indicated that it is capable of discerning (kp Cp)1/2 differences equal
to 10 per cent, conductivity differences of 15 per cent, and diffusivity
differences of 10 per cent. Standard, steady-state conductivity measure-
ments near room temperature are accurate to about 10 per cent. For
finite graphite specimens, conductivity differences of about 7 per cent
are minimally observable, this increased precision resulting from the
stronger signal generated.
During the coming year, we intend to continue to develop this tech-
nique, as a part of a major effort at Avco Space Systems Division in
the nondestructive evaluation of materials. The immediate plans are to
adapt the technique to field testing.
C. H. Hastings1
Strength Predictions for Graphite;

A Review of Prior Work at
AVCO SSD
REFERENCE: Hastings, C. H., "Strength Predictions for Graphite: A

Review of Prior Work at AVCO SSD," Nondestructive Testing of Nu-
clear Graphite, ASTM STP 439, American Society for Testing and Ma-
terials, 1968, pp. 87-96.
ABSTRACT: A number of investigators in the author's laboratory have
successfully studied the correlation of nondestructive measurements and
destructively determined mechanical properties. General work in this
area has been going on since 1958 and specifically on graphite since
early 1964. Accomplishments include nondestructive testing capability
for predicting density in small discrete volumes of bulk graphite to
better than ±1 per cent, Young's modulus to better than ±3 per cent,
and ultimate tensile strength (all at room temperature) to better than
±10 per cent. Predictions can be made in five or six different aerospace
(fine-grained) grades of graphite, for both with- and against-the-grain
orientation, employing a single set of calibration curves. Experiments
indicate the strong possibility of extension to other fine-grained graphites,
including graphite composites containing additives such as silicon and
zirconium diboride.
KEY WORDS: graphite, strength of materials, modulus, density, me-
chanical properties, ultrasonics, radiometry, nondestructive testing
The attractive potential of graphite as a high-temperature material

for missile reentry vehicle tips and rocket nozzles has interested design-
ers for many years. The use of graphite guide vanes in the V-2 missile of
World War II frustrated German rocketeers. Early research led to non-
destructive (NDT) crack detection techniques to avoidance of brittle
failures but did not succeed in preventing failure incidence. Unpre-
dictable failures still plague the designer who attempts to use graphite
under high heat flux and errosive environments.
Literature [1-3]2 attests to significant variability in the mechanical
* Work presented in this paper was performed for the Air Force Materials
Laboratory, Dayton, Ohio, under Contract AF 33(615)-1601 and 3942.
1
Chief, NDT
Copyright by Evaluation Section,
ASTM Int'l (all Avco Corp.,
rights reserved); Mon DecSpace Systems
26 20:58:32 EST Div.,
2011 Lowell,
Mass. Downloaded/printed by
2
The italic numbers in brackets refer to the list of references appended to this
paper. (PDVSA Los Teques) pursuant to License Agreement. No further reproductions authorized.
87
88 NUCLEAR GRAPHITE
properties of bulk graphites, both within small volumes and from one
billet to another of the "same" grade. Coefficients of variability for
modulus and tensile strength in excess of 20 per cent are not uncommon.
When products such as rocket nozzles, containing property gradients of
this magnitude, are exposed to severe thermal-gradient-producing en-
vironments, brittle failures are easy to imagine, even if no cracks or
other macrodefects are present. Hence, NDT defect detection as con-
ventionally practiced is not expected to be adequate by itself to ensure
reliable performance.
When graphite products fail under severe environments, the designer
tends to point to the material and its wide variability as the likely cause.
The materials producer responds by suggesting that designers do not
understand how to design with graphite as it exists and are therefore
responsible for the failure.
If one examines the outstanding successes which have been experi-
enced in the use of graphite for aerospace applications, including the de-
tailed design aspects, it is apparent that successful graphite hardware
is overdesigned. Design models which consider graphite properties vari-
ability do not exist or at least are not in common use. Variability in
properties must be covered by large safety factors.
Since there has been no way of determining properties and property
gradients in graphite fabrications prior to service (handbook averages
are useless), the designer and material producer remain deadlocked in
their argument with no way to prove either correct. It can be surmised
that both are correct and both liable for failures to some uncertain de-
gree.
It would appear that three technologies must improve their capa-
bilities if this dilemma is to be resolved:
1. Nondestructive properties prediction capability applicable to de-
liverable hardware.
2. Improved uniformity of available graphite.
3. More sophisticated design models which consider allowable mate-
rial variability.
This paper reviews work during the past three years [2,4-6] to develop
useful NDT techniques, including their meaningful interpretation.
Property Controlling Variables
At the outset of the Air Force Materials Laboratory sponsored pro-
gram, discussion with graphite producers disclosed general agreement
that density variability exerts the predominant influence on strength
variability. There are many material-energy interactions available for
use in Copyright
NDT that by can
ASTMrespond
Int'l (all quantitatively
rights reserved); to density
Mon Dec 26variations.
20:58:32 ESTSome2011
of these include the following:
1. Ultrasonic
(PDVSA Los pulse velocity
Teques) pursuantand attenuation.
to License Agreement. No further reproductions authorized.
HASTINGS ON STRENGTH PREDICTIONS FOR GRAPHITE 89
2. Ultrasonic resonance (thickness resonance).

3. Sonic vibration (mass resonance).
4. X- or gamma-ray attenuation (mass per unit area).
5. Electrical resistivity dc or ac, that is, eddy current.
6. Infrared transient and steady-state thermal techniques.
The goal in evaluating available material-energy interactions is to
select the technique yielding a unique response to property controlling
material variability, uncluttered by side responses to irrelevant vari-
FIG. 1—Poisson ratio (a) plotted versus the function f (a) = [(1 — a)]/[(l +«r)(l — 2<r)].
ables. Since most NDT respond to both relevant and irrelevant variables,
this aspect of the problem represents the real challenge.
The result of initial studies of NDT-destructive correlations [2] con-
cluded that the cleanest relationships would be obtained with combined
use of gamma ray radiometry (density times thickness gaging) and ultra-
sonic pulse velocity measurements. Ultrasonic attenuation is sensitive to
a host of irrelevant variables, as is electrical resistivity. Sonic mass
resonance is not applicable to local determinations within a product,
and infrared NDT technique studies were felt to be more applicable to
thermal property correlations, discussed in another paper at this sym-
3
posium.
3
See(PDVSA
p. 70. Los Teques) pursuant to License Agreement. No further reproductions authorized.
90 NUCLEAR GRAPHITE
While an excellent measure of local density variability in graphite

can be obtained by radiation gaging alone, one does not obtain infor-
mation relative to size and distribution of micropores responsible for
both density variability and strength in graphite. Hence the need for
ultrasonic velocity measurements which sense elastic variability. Actu-
ally, bulk density measurements commonly made gravimetrically for
a graphite billet or product are of little value in characterizing strength
variability, since they ignore pore size/distribution, the controlling mate-
rial variable. Of course it is recognized that grain size, binder-filler ra-
tios, and microcracks also influence strength. However, the graphite pro-
ducers are in agreement that density/porosity exerts a major influence.
FIG. 2—Block diagram of ultrasonic velocity measuring apparatus.
Material Energy Interactions

For homogeneous material, the velocity of a longitudinal-mode ultra-
sonic pulse is described by
where:
K = constant to adjust units,
VL = longitudinal wave velocity,
ED = Young's modulus (sonic),
p = density, and
a = Poisson's ratio.
Although graphite is far from homogeneous, structurally, and is best
described as a composite of filler, binder, and porosity, it has been useful
to attempt application of Eq 1.
Figure 1 shows the influence of Poisson ratio on the function of the
Poisson ratio in
Copyright by Eq
ASTM1. Int'l
For(allgraphites of interest,
rights reserved); Mon Decsigma is usually
26 20:58:32 0.2 or
EST 2011
less, soDownloaded/printed
that the functionby of sigma approaches unity. This permits practi-
cal simplification of the equation:
FIG. 3—Block diagram of radiation density gage for graphite.
FIG. 4—Composite plot of five grades of graphite showing relationship o/KpVj,2 and ED .
and suggests a nondestructive test for modulus of graphite at room tem-

perature. Ultrasonic velocity can be measured conveniently through a
thickness of atbyleast
Copyright ASTM18Int'l
in. (all
in fine-grained
rights reserved);graphite.
Mon DecFigure 2 shows
26 20:58:32 EST a2011
block Downloaded/printed
diagram of typicalby test equipment.
Density
(PDVSAcanLos
be Teques)
conveniently andLicense
pursuant to nondestructively
Agreement. No determined by authoriz
further reproductions
92 NUCLEAR GRAPHITE
radiometry in the same volumes as those measured ultrasonically by

observing the relation :
where:
/ = intensity of transmitted X- or gamma rays,
I0 = intensity of incident radiation,
e = 2.72, the Naperian constant,
Mm = the mass absorption coefficient,
p = density, and
x = graphite thickness at point of measurement,
so, that,
The need for determining the mass absorption coefficient can be elimi-
nated by calibrating the equipment of Fig. 3 against small specimens of
graphite of known uniform density, determined gravimetrically.
Figure 4 shows a cross plot of Eq 2 for which p was measured radio-
metrically, VL ultrasonically, and ED is dynamic modulus measured by
sonic resonance, for the same volumes of graphite. Note that specimens
were taken from several billets involving five different grades of fine
grained graphite in both grain orientations. A total of 132 specimens
was taken. Graphite grades studied included CFZ, ZTA, CFW, RVA,
and ATI.
The regression line through the data points was obtained using a
Benson-Lehner Plotter and led to the equation and other data as follows:
Equation:
rms value: 0.045

Correlation coefficient: R = 0.991
The rms value, derived from the computer program, is the root mean
2
square of the differences between the experimental KpV L values and
that calculated from the best linear fit. A correlation coefficient (R)
value of 1.0 indicates a "perfect" fit while a value of 0 indicates no fit.
The value R has been calculated from the coefficient of the modulus
term of the equation \ ED = 1.0<r2, and the standard deviations of the
2
two variables ED and KpVL according to the equation:
If one considers
(PDVSA individual
Los Teques) grades
pursuant to License of graphite
Agreement. No the
furthercorrelation coeffi-
cients vary between 0.961 and 1.000, suggesting even better prediction
accuracy for some grades than for others. This might be attributable to
the degree to which density/porosity is the controlling variable.
Consider now, Fig. 5. An idealized stress-strain curve for graphite
at room temperature is shown with three modulus lines indicated. The
FIG. 5—Typical stress-strain plot showing relative positions of pV\?, tensile modulus
(Ex) and secant modulus (Fs) for a typical graphite tension specimen at room temperature.
dynamic modulus (ED), measured usually by sonic resonance, is con-

sidered equivalent to KpVi? as measured nondestructively. It is tangent
to the stress-strain curve at its origin. The tensile modulus (ET) is shown
as an "eyeball" tangent somewhere near the origin. The secant modulus
(Es} isCopyright
drawnbybetween the origin and the point of rupture. As shown,
ASTM Int'l (all rights reserved); Mon Dec 26 20:58:32 EST 2011
94 NUCLEAR GRAPHITE
where:
UTS = ultimate tensile stress, and
(T — total strain to failure.
Analysis of tensile test data has shown that the ratio of KpVj} to
Es is essentially constant for a given direction in a given grade of graphite.
Figure 6 is a composite plot of KpVLzand E s for five grades of graphite.
The term Es was calculated from actual ultimate tensile stress and total
strain-to-failure values from tension tests. The KpV values were cal-
FIG. 6—Composite plot of five grades of graphite showing relationship o/KpVi* and Eg
culated from NDT measurement on the same tensile bars before de-
structive testing. With- and against-grain orientations were identified
during data collection and calculation. However, both directions are
included in Fig. 6. For the grades included in the plot, strain to failure
was found to be nearly constant for a given grade and direction, al-
though this is not always the case.
Having obtained the KpVJ versus E s relationship for specific grades of
graphite, tensile strength can be calculated for additional specimens of
those Copyright
grades. by
The slopeInt'lof(all
ASTM therights
Fig.reserved);
6 line becomes
Mon Dec 26a 20:58:32
constantEST(A)
2011used
with NDT data and the
Downloaded/printed by appropriate e r (for specific grade and direction)
to compute
(PDVSAthe ultimate
Los tensile to
Teques) pursuant stress:
License Agreement. No further reproductions authorized.
The regression line plot of Fig. 6, when analyzed, yields the following
data:
Equation:
rms value: 0.087

Correlation coefficient: R = 0.988
Based on 2.33 a; ED and Ea for a single grade of graphite, say CFW, is
predictable from NDT data to within 6 and 11 per cent, respectively,
at the 98 per cent confidence level. For usual tension tests the one-
sigma limit is on the order of 15 per cent.
Conclusion
Although these correlations are not regarded as highly precise, they are
considered extremely useful and provide a new capability for character-
izing graphite variability. This capability represents one important leg
of the design, materials, and test-capability triangle required to un-
scramble the existing dilemma of reliable application in both the aero-
space and nuclear engineering fields.
The next urgent needs are as follows:
1. To use these new NDT capabilities to verify progress in graphite
production processing towards more uniform strength properties.
2. To determine design allowables for strength gradients as related
to specific service requirements for hardware.
The first of these needs should be a joint response on the part of
graphite producers and users (materials engineers). The second require-
ment is for a response from design engineers leading to realistic design
models.
A cknowledgment
Being a review, the work discussed was largely accomplished by other
individuals at Avco Space Systems Division. Particular thanks are given
to the following named and to those who provided essential support:
G. E. Lockyer, project engineer; E. A. Proudfoot, leader, NDT Develop-
ment Group; E. Wagner, mechanical measurements; C. L. Theberge,
mechanical measurements; C. A. Lermond, statistical analysis; A. Chet-
son, NDT measurements; and T. Ludwig, NDT measurements.
Work was by
Copyright performed under
ASTM Int'l (all rights Air Force
reserved); MonMaterials Laboratory
Dec 26 20:58:32 EST 2011 Con-
tracts Downloaded/printed
AF33(615)-1601 by and 3942, with W. L. Shelton serving as project
monitor.
96 NUCLEAR GRAPHITE
References
\1] Lockyer, G. E., "Evaluation of a Resin Ceramic Heat Shield Material by
Ultrasonic Techniques," Nondestructive Testing, Vol. XXIII, No. 3, 1965.
[2] Lockyer, G. E., "Investigation of Nondestructive Methods for the Evaluation
of Graphite Materials," Technical Report AFML-TR-65-113, Air Force Ma-
terials Laboratory, Dayton, Ohio, May 1965.
[3] Glasser, J. and Few, W. E., "Directory of Graphite Availability," Technical
Documentary Report No. ASD-TDR-63-853, Air Force Materials Labora-
tory, Dayton, Ohio, Sept. 1963.
[4] Lockyer, G. E. et al, "Investigation of Nondestructive Methods for the
Evaluation of Graphite Materials," Technical Report AFML-TR-66-101, Air
Force Materials Laboratory, Dayton, Ohio, May 1966.
[5] Lockyer, G. E. et al, "Investigation of Nondestructive Methods for the
Evaluation of Graphite Materials," Technical Report AFML-TR-67-128, Air
Force Materials Laboratory, Dayton, Ohio, June 1967.
f6],'Lockyer, G. E. and Proudfoot, E. A., "Nondestructive Determination of Me-
chanical Properties of Refractory Materials," American Ceramic Society
Bulletin, Vol. 46, No. 5, 1967, p. 521.
R. W. McClung1
Low Voltage Radiographic and

Micoradiographic Techniques
for Graphite*
REFERENCE: McClung, R. W., "Low Voltage Radiographic and Mi-

croradiographic Techniques for Graphite," Nondestructive Testing of Nu-
clear Graphite, ASTM STP 439, American Society for Testing and Mate-
rials, 1968, pp. 97-108.
ABSTRACT: Low-voltage radiography was studied to provide optimum
techniques for graphite thickness less than 2 in. Significant improvements
were made in image quality and sensitivity by use of an intermediate
atmosphere of helium, bare film, and a thin beryllium-window X-ray
tube. Use of a high resolution photographic emulsion allows contact
microradiography to be performed on miniature specimens with a reso-
lution of one micron.
KEY WORDS: X-ray analysis, radiography, microradiography, graphite,
coatings
In recent years in the nuclear and other industries, there have been in-
creasing requirements for improved properties in graphite which, in
turn, created a greater need for better nondestructive testing techniques
to evaluate the material. At the Oak Ridge National Laboratory we have
found radiography to be a valuable tool and developed techniques for
both low-voltage and microradiographic methods to solve many of the
graphite evaluation problems with which we were faced. This work in-
cluded parametric studies of specimen thickness, X-ray energy and ex-
posure, and attainable sensitivity, as well as many special detailed tech-
niques for unusual problems.
Parametric Studies
General Consideration
Graphite is a form of carbon, the sixth element in the periodic table.
In general, the lower the atomic number of an element, the smaller
* Research
Copyrightsponsored by (all
by ASTM Int'l the rights
U.S. reserved);
Atomic Energy
Mon DecCommission under
26 20:58:32 EST 2011contract
with the Union Carbide Corp.
Group leader, Metals and Ceramics Div., Oak Ridge National Laboratory,
(PDVSA
Oak Ridge, Los Teques) pursuant to License Agreement. No further reproductions authorized.
Tenn.
97
98 NUCLEAR GRAPHITE
will be the value of the mass attenuation coefficient, n, for any given
radiation energy. The effect of the attenuation coefficient on the inten-
sity of the radiation beam as it passes through a specimen is given by
the relationship,
where :
/ = radiation transmitted through the specimen, r/h,
I0 = radiation incident upon the entry surface of the specimen, r/h,
/x = attenuation coefficient, cm2/g,
p = density, g/cm3, and
*• = specimen thickness, cm.
For useful radiography there must be sufficient change in the radiation
transmitted through the specimen, /, to achieve an interpretable contrast
of density on the processed radiograph. As evident from the equation,
this is governed by the exponential terms, //, p, and jc. For most practical
cases, p and jc are variables but are restricted within. fairly narrow limits.
For instance, graphite is a very low-density solid as compared with most
structural materials normally considered for radiography. Specimen
thickness is normally determined by design requirements, and for most
of the requirements discussed in this paper was less than 2 in. thick.
This leaves only /x as a true variable with which the radiation transmission
can be controlled. As with density, graphite has a low value of ju when
compared with many other materials. However, the attenuation coeffi-
cient is energy dependent and is generally larger at lower energy levels.
Thus, for examination of thin sections of low-density graphite, it has
been necessary to use low-energy (low-kilovoltage) radiation. This
provided a large enough change in transmission to permit the detection
of the minute changes associated with the discontinuities of interest.
Equipment
We conducted similar studies earlier for the development of tech-
niques for the radiographic evaluation of beryllium, aluminum, and
stainless steel.2 Much of the equipment for the radiography of graphite
is identical to that described in the report on metals. For that reason only
a summary is incorporated here.
The equipment was capable of generating continuously variable X-ray
energies from 0 to 50 kVp. With the lower X-ray energies which are
readily absorbed in the thin graphite sections, it was necessary to
2
McClung,
CopyrightR.byW.,ASTM
"Techniques
Int'l (all for Low-
rights Voltage Mon
reserved); Radiography," Nondestruc-
Dec 26 20:58:32 EST 2011
tive Testing, Vol. 20, No.by4, July-Aug. 1962, pp. 248-253. Many more figures,
Downloaded/printed
technique(PDVSA
charts, Los
and Teques)
other plotted
pursuantdatato for the Agreement.
License three metals
No are found
further in a
reproductions autho
report with the same title, ORNL-3252, 14 Feb. 1962.
McCLUNG ON RADIOGRAPHIC AND MICRORADIOGRAPHIC TECHNIQUES 99
FIG. 1—Low-voltage X-ray equipment.
eliminate all extraneous material between the target of the X-ray tube
and the specimen. These materials not only reduce the intensity of the
X-ray beam, but also preferentially absorb the softer components of the
spectrum which are so important in producing high-contrast radio-
graphs. The first step in minimizing excess absorbers was the use of an
X-rayCopyright
tube with a low-filtration
by ASTM Int'l (all rightsberyllium window
reserved); Mon Dec 26 only 0.010
20:58:32 in. thick.
EST 2011
Air isDownloaded/printed
an effective absorber
by for the soft X-rays, so helium was substi-
tuted as the atmosphere
(PDVSA between
Los Teques) pursuant the X-ray
to License tube No
Agreement. andfurther
the reproductions
specimen. authorized.
This
100 NUCLEAR GRAPHITE
was accomplished with a simple 34-in.-long, 8-in.-diameter cylindrical

chamber with 0.0005-in.-thick polyethylene diaphragms placed over
each end to retain the helium within the drum-like chamber. The very
thin plastic membranes were almost transparent to the X-rays being
used. This system is shown in Fig. 1. The helium chamber extended
from the X-ray tube to within approximately 2 in. of the working surface.
Thus, both the specimen and film were in the normal room atmosphere
and were completely accessible for change without violating the helium
atmosphere.
FIG. 2—X-ray exposure versus density chart for radiography of graphite at

45 kVp.
Another important step in reducing unnecessary absorption was the

elimination of the cassette or film holder and the placement of the
specimen directly on the bare film. This, of course, required us to use
dark-room exposure techniques.
Experimental Procedure
An extensive program was followed to study the effects of variation
in X-ray energy and specimen thickness and in the use of intermediate
atmospheres
Copyright of
by both
ASTMhelium andrights
Int'l (all air. reserved);
We prepared
Mon Dec a step wedge of
26 20:58:32 EST 2011
graphite with thicknesses
Downloaded/printed by varying from 0.100 to 1.650 in. The graphite
wedge was thenLosradiographed
(PDVSA usingto both
Teques) pursuant helium
License and air
Agreement. atmospheres
No further reproductions auth
FIG. 3—Exposure chart for various thicknesses of graphite with air and
helium.Copyright by ASTM Int'l (all rights reserved); Mon Dec 26 20:58:32 EST 201
(PDVSA Los Teques) pursuant to License Agreement. No further reproductio
at discrete energy levels from approximately 5 to 45 kVp. At each

energy level, enough radiographs were made with different exposure
times to provide a complete range of readable densities for each thick-
ness. Thus, for each thickness, curves of film density versus exposure
time could be plotted as a function of energy level and atmosphere.
Maximum exposure times were approximately 10 min, but most of the
exposures were less than 5 min. For exposures in excess of 1 min, the
milliamperage was the maximum allowed for the kilovoltage and varied
from 10 to 30 mA. For shorter exposures, lower mA values were used
to improve precision. Eastman Type M film was used throughout the
project.
Film Processing
Control of the film and film-processing variables was mandatory to
attain reproducible results and to allow cross referencing and correla-
tion between the different radiographic conditions. All exposures were
made from the same box of film. All films exposed, under a given atmos-
phere (helium or air) were processed as a batch. With these precautions,
good reproducibility was achieved, and very smooth curves with little
data scatter were possible.
All film densities were measured on dry processed film with a Macbeth-
Ansco Model 12A densitometer3 which is capable of making measure-
ments over a density range from 0 to 2.0 with an accuracy of ±0.02.
Results
All of the data were transferred to basic graphs to display the milli-
ampere-second exposures versus the film density for each specimen
thickness. For each chart the X-ray energy and intermediate atmos-
phere were held constant. Figure 2 is a typical chart showing the data
for an air atmosphere at an energy level of 45 kVp. These curves then
served as the basis for subsequent data evaluation. Useful exposure
charts for radiography of graphite were generated as a function of
energy, intermediate atmosphere, and specimen thickness.
Figure 3 is a typical exposure chart for an air atmosphere. Super-
imposed on this chart is the exposure curve for 0.100 in. of graphite if
a helium atmosphere were substituted between the X-ray tube and
specimen.
As described earlier, several precautionary steps were taken to elimi-
nate extraneous absorbing material between the tube and specimen. This
was most beneficial at lower specimen thicknesses and X-ray energies.
Experimental
Copyright exposures to determine
by ASTM Int'l equivalent
(all rights reserved); Mon thicknesses and EST
Dec 26 20:58:32 com-
2011
parisonDownloaded/printed
with exposure by charts determined the conditions at which there
(PDVSA Los Teques) pursuant to License Agreement. No further reproductions authori
3
Macbeth Instrument Corp., Newburgh, N. Y.
is little advantage in the special precautions. We arbitrarily decided that

any decrease in exposure time of 10 per cent or less was insignificant
The film holder which was selected for comparison was a flexible plastic
cassette which interposed a single layer of plastic between the specimen
and film. Typical results are shown in Fig. 4 to define threshold condi-
FIG. 4—Conditions under which absorber removal will effect 10 per cent
change in exposure requirement for radiography of graphite.
tions at which a 10 per cent decrease in exposure is realized by removing

or replacing the absorber. For X-ray energies and thicknesses below
the curves, greater than 10 per cent benefits are obtained. Removal of
the cassette produced at least 10 per cent improvement throughout the
thickness rangeby studied.
Copyright ASTM Int'l (all rights reserved); Mon Dec 26 20:58:32 EST 2011
TheDownloaded/printed
graphite used in by this study had a specific gravity of 1.7. There-
fore, for(PDVSA
graphites havingpursuant
Los Teques) a different density,
to License a proportional
Agreement. correction
No further reproductions authorized.
would be necessary for all data involving thickness.
Applications
The low-voltage radiographic techniques have been successfully ap-
plied to a variety of graphite inspection problems. One such application
was for the evaluation of 2.46-in.-(6-cm-)diameter graphite spheres
which were subsequently to be machined into shells for nuclear fuel
elements. Because of the spherical configuration, the specimens provided
a large range of thickness for the X-rays. This range coupled with the
inherent radiation scatter allowed only a small cylindrical section which
was coaxial with the X-ray beam to be evaluated in a single exposure.
The radiographic quality was inferior. However, introduction of the
FIG. 5—Masking tray for radiography of graphite spheres.
unique masking tray shown in Fig. 5 allowed a great improvement to

radiographic sensitivity. One-inch Lucite was machined to provide
hemispherical cavities matching the curvature of the spheres. The
Lucite mask allowed a selective absorption of scattered X-rays as well
as providing a more nearly constant total X-ray absorption over the
entire projected sphere diameter. With this technique the entire spheri-
cal volume could be evaluated with a single exposure for three-dimen-
sional discontinuities such as porosity. The sensitivity and resolution
were shown to be capable of detecting flaws about 0.040 in. in diameter.
This is equivalent to approximately 2-IT radiography as defined by
ASTMCopyright
MethodbyforASTMControlling
Int'l (all Quality of Radiographic
rights reserved); Testing
Mon Dec 26 20:58:32(E-142).
EST 2011
We feltDownloaded/printed
that smaller flaws
by could have been detectable, but no such stand-
ards were made. Three-view radiography (in X, Y, and Z directions)
was performed to provide added assurance for the detection of internal

cracks or laminations.
An interesting application was in support of liquid-salt (a complex
form of fluorides of lithium, beryllium, zirconium, and uranium) im-
pregnation studies in various types of graphite. Low-voltage radio-
FIG. 6—Radiograph of graphite specimen with complex salt impregnating

cracks.
graphs were taken prior to impregnation to detect flaws, after initial

impregnation to determine the nature of the salt flow, and again after
heat treatment to observe changes in the graphite in the impregnated
condition. Figure 6 is a reproduction of a radiograph showing the salt
which has filled existing cracks in the graphite specimen (density =
3
1.87 g/cm ) but
Copyright by has
ASTM notInt'l
penetrated
(all rights into the body
reserved); in any
Mon Dec other region.
26 20:58:32 EST 2011
Tension and compression
Downloaded/printed by specimens for destructive tests on graphite
are radiographed
(PDVSA Los to detect
Teques) internal
pursuant flaws.Agreement.
to License Good correlation has been authorized.
No further reproductions
shown between presence of flaws, site of fracture, and reduced breaking

strength. This has allowed a reduced scatter band of data on graphite
strength.
Microradiography
Equipment
Substitution of extremely fine-grained emulsions for the X-ray film
has allowed the performance of contact microradiography with good
resolution.4 A number of photographic detectors were tested, but the
optimum for our purposes was shown to be Eastman Kodak High Reso-
lution Plates. Although several fine-grain developing solutions were
tested, none were found to be superior to the standard X-ray film de-
veloper which was being used for conventional radiography. All other
aspects of the low-voltage radiographic system remained the same for
our microradiography.
Specimens
A major application of our microradiography has been on nuclear
fuel particles coated with a thin layer of pyrolytic carbon.5 The X-ray
energy levels used for the particle evaluation vary from 10 kVp down
to about 4 kVp, depending upon the character and density of the coat-
ing and the information desired. Because of the very thin emulsion and
fine-grain size of the high-resolution plates, the response to X-rays is
rather slow and exposure times as long as 1 h at the lower energies are
not unusual. These exposures are at the maximum current of about
15 mA.
Typical coated fuel particles include a core or kernel 0.008 in. in
diameter with a 0.004-in.-thick coating which may be composed of
several thinner layers with different densities. The microradiography is
performed to allow measurement of core and coating dimensions and
evaluation of integrity. The resolution and accuracy have been shown to
be about 1 ^.m. The principal limitations on observation of detail or
resolution are the resolving power of the optical systems (about 1 /mi)
and the electron diffusion in the emulsion which is rated at about 1 /mi
at the energy level being used. For this reason, the helium chamber was
shortened to about 19 in. for coated particle microradiography, since
this increased the geometric unsharpness to only approximately ^3 /mi,
but decreased the required exposure times by a factor of approximately 4.
4
McClung, R. by
Copyright W.,ASTM
"Studies
Int'lin(all
Contact
rights Microradiography,"
reserved); Mon DecMaterials Research
26 20:58:32 EST 2011
& Standards, Vol. 4, No. 2, Feb. 1964, pp. 66-69.
McClung, R. W., Bomar, E. S., and Gray, R. J., "Evaluating Coated Particles
(PDVSA
of Nuclear Fuel,"Los Teques)
Metals pursuant
Progress, Vol.to86,License
No. 1,Agreement. No 90-93.
July 1964, pp. further reproductions auth
FIG. 7—Microradiograph of selected coated particles to show multilayer,

variable density coating (X75).
Viewing
Several thousand coated particles can easily be radiographed in a
single Copyright
exposurebyon the Int'l
ASTM 2-in.-square plates. Mon
(all rights reserved); The Dec
contact microradiograph
26 20:58:32 EST 2011
which is(PDVSA
produced may then be viewed on a microscope or metallograph
Los Teques) pursuant to License Agreement. No further reproductions authorized.
equipped for transmitted light. Examinations are made at magnifications
up to X500 with little difficulty being caused by the grain size. For
recordings of the magnified image, a photomicrograph can be made of a
representative area of the contact microradiograph. The film used for
this is Eastman Royal Orthofilm exposed with a green (Wratten No.
54) filter and developed in DK-50 according to recommended proce-
dures. Contact prints can now be made from this photomicrograph
restoring the same relationship of light and dark areas present on the
original microradiograph.
Results
Figure 7 is a print of a group of coated particles selected to demon-
strate the detail that may be detected in a multilayer variable density
coating by microradiography. The technique is being used as an evalua-
tion tool for process control of the coating process, for routine evaluation
of the coated product, and for post-service examination after heat treat-
ment or reactor testing. The latter has required a degree of technique
modification, but good quality microradiography is possible despite a
high level of radiation from the specimen.
Summary
Low-voltage radiographic and microradiographic techniques were
demonstrated to be very useful for the evaluation of graphite and carbon.
As a result of parametric studies, detailed exposure charts for graphite
radiography have been prepared. We determined conditions under
which significant improvements could be made by removal of such ab-
sorbers as the air atmosphere and film holder. Use of a high-resolution
photographic emulsion allows performance of microradiography with
1-ju.m resolution on miniature specimens.
A cknowledgments
The author is pleased to acknowledge the significant contributions of
W. J. Mason toward both the technique development and the data ac-
cumulation.
IfflS PUBLICATION is one of many
issued by the American Society for Testing and Materials
in connection with its work of promoting knowledge
of the properties of materials and developing standard
specifications and tests for materials. Much of the data
result from the voluntary contributions of many of the
country's leading technical authorities from industry,
scientific agencies, and government.
Over the years the Society has published many tech-
nical symposiums, reports, and special books. These may
consist of a series of technical papers, reports by the
ASTM technical committees, or compilations of data
developed in special Society groups with many organiza-
tions cooperating. A list of ASTM publications and
information on the work of the Society will be furnished
on request.
(PDVSA Los Teques) pursuant to License Agreement. No further reproductions au

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ASTM SPECIAL TECHNICAL PUBLICATION NO. 439

List price $8.00; 20 percent discount to members

The Society is not responsible, as a body,

Copyright by ASTM Int'l (all Printed

The papers in the Symposium on Nondestructive Testing of Nuclear

Effects of High-Energy Radiation on Inorganic Sub-

The Effects of Radiation on Structural Metals, STP

It is indeed a gratifying assignment to write these introductory remarks

within the rapidly growing field of graphite technology. The graphite

publication to their own efforts in the interest of a large technical com-

Infrared Testing of Bonds Between

REFERENCE: Green, D. R. and Day, C. K., "Infrared Testing of

Nuclear graphite components are often required to conduct a large

the specimen surface emittance (often called emissivity). Emittance in-

Theory and Selection of Temperature Ranges

FIG. 1—Radiometer output, E, versus temperature, T, of specimens having

FIG. 3—E» versus T» for specimens at T» = 39 C,

FIG. 4—Emittance independent infrared bond test.

pendence is shown by approximate coincidence of the three curves.

General Procedure and Arrangement of Equipment

printer, and a heat source. A functional diagram of the system is shown

FIG. 5—Test piece scanner and associated equipment.

Radiometer and Digital Recording System

tubing maintained at 765 C. Heat was supplied to the tubing by passing

Bench Standard Test Piece

steel sheet bonded to a massive piece of graphite with W. T. Bean type

ences in the bond at other locations were detected during subsequent

FIG. 9—Emittance independent plot of data resulting from bond tests on

veloped the scanner; W. H. Gray, L. H. Fischer, R. D. Breneman, and

Nondestructive Testing of Graphite at the

REFERENCE: Blanks, B. L., Edenborough, N. B., Elliott, D. E., and

When the Los Alamos Scientific Laboratory started to use graphite

* Work done under the auspices of the Atomic Energy Commission.

for these inspections is a continuing process based on the performance

Ultrasonics and Sonics

FIG. 1—Model 721 Reflectoscope setup for determining longitudinal sound

FIG. 3—Bar charts sound velocity versus cracking of modules.

The through-transmission, elapsed-time method of determining sound

FIG. 4—Block diagram of high power wave generation experiment.

graph showing cracking as a function of sound velocity in a group of

FIG. 5—Block diagram of the Universal eddy current tester.

FIG. 6—Small diameter eddy current probe.

bridge circuit. The imbalance in the bridge, caused by changes in the

FIG. 7—Calibration curve for conductivity measurements, Universal eddy

ties equivalent to a 0.035-in.-diameter hole extending 0.025 in. radially

TABLE 2—Typical conductivity measurements with a rectangular eddy current

E24 1 0.047 0.045 0.051

Magnates! FM-102. The range of conductivities which can be measured

A typical calibration curve is shown in Fig. 7. Conductivities as low

FIG. 8—Radiation gage for measuring graphite density.

conductivity as the coil orientation is changed has been found to be a

FIG. 9—Close-up of radiation gage showing detector collimator.

FIG. 10—Typical scanning trace from radiation gaging of a graphite cylinder.

Since a two-dimensional scanner is normally used to position speci-

FIG. 11—Schematic beta-backscatter probe for accessible surfaces.

specimens in the research program of the Laboratory. The total error

FIG. 12—Schematic beta-backscatter probe for small diameter bores.

FIG. 13—Calibration chart for beta-backscatter coating thickness measure-

to particular configurations are worthy of recording along with the im-

FIG. 14—Electron micrograph of extruded graphite (X6000).

on the existence of an appreciable difference in the atomic numbers of

FIG. 15—Electron micrograph of pyrocarbon deposit (X6000).