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Volume 2 in this 14 volume TPRC Data Series covers nonmetallic materials which
are in the solid state st normal temperature and pressure, including five
elements (with over 100 varieties of graphite), 53 simple end complex oxides,
82 systems of oxide mixtures, 83 nonoxide compounds, seven systems of mixtures
of oxides snd nonoxides, 15 organic compounds, 22 kinds of cermets, 10 groups
of systems, eight kinds of refractory materials, ovsr 40 kinds of glssses, 24
minerels, 16 polymers, 26 animal and vegetable natural substances, 30 processed
composites and processed natural and mineral substances, snd 10 aggregate mixes,
slags, scales, and residues. Data for the elements and for a few oxides have
been critically evaluated, analysed, and synthesised, and recommended values
or provisional values are presented in addition to the original experimental
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THERMAL
CONDUCTIVITY
Nonmatailic Solids
__ . -r^ v
P
THERMOPHYSICAL PROPERTIES OF MATTER
The TPRC Data Series
A Comprehensive Compilation of Data by the
Thermophysical Properties Research Center (TPRC), Purdue University
New data on thermophysical properties are being constantly accumulated at TPRC Contact TPRC
and use its interim updating services for the most cunent information
' III
-7-
^_
THERMAL
CONDUCTIVITY
Nonmetallic Solids
Y. S. Touloukian
Director
Thermophysical Properties Research Center
and
Distinguished Atkins Professor of Engineering
School of Mechanical Engineering
Purdue University
and
Visiting Professor of Mechanical Engineering
Auburn University
R. W. Powell
Senior hes)archer
Thermophysical Properties Research Center
Purdue University
Formerly
Senior Principal Scientific Officer
Basic Physics Division
National Physical Laboratory
England
C.Y. Ho
Head of Data Tables Division
and
Associate Senior Researcher
Thermophysical Properties Research Center
Purdue University
P. G. Klemens
Professor and Head
Department of Physics
University of Connecticut
and
Visiting Research Professor
Thermophysical Properties Research Center
Purdue University
'*.
Library of Congress Catalog Card Number 73-129616
r
Copyright 1970, Purdue Research Foundation
. , ...^.w Wv
"In this work, when it shall be found that much is omitted, let it not be forgotten
that much likewise is performed...''
m **
Foreword
In 1957. the Thermophysical Properties Research that about 100 journals are required to yield fifty
Center (TPRC) of Purdue University, under the percent. But that other fifty percent I It is scattered
leadership of its founder. Professor Y. S. Touloukian. through more than 3500 journals and other docu-
began to develop a coordinated experimental, ments, often items not readily identifiable or ob-
theoretical, and literature review program covering ainable. Nearly 50,000 references are now in the
a set of properties of great importance to science and files.
technology. Over the years, this program has grown Thus, the man who wants to use existing data,
steadily, producing bibliographies, data compila- rather than make new measurements himself, faces
tions and recommendations, experimental measure- a long and costly task if he wants to assure himself
ments, and other output. The series of volumes for that he hi.s found all the relevant results. More often
which these remarks constitute a foreword is one of than not, .> earch for data stops after one or two
these many important products. These volumes are a results are found- or after the searcher decides he
monumental accomplishment in themselves, re- has spent enough time looking. Now with the
quiring for their production the combined knowledge appearance of these volumes, the scientist or engineer
and skills of dozens of dedicated specialists. The who needs these kinds of data can consider himself
Thermophysical Properties Research Center de- very fortunate. He has a single source to turn to;
serves the gratitude of every scientist and engineer thousands of hours of search time will be saved,
who uses these compiled data. innumerable repetitions of measurements will be
The individual nontechnical citi/en of the avoided, and several billions of dollars of investment
United States has a stake in this work also, for much in research work will have been preserved.
of the science and technology that contributes to his However, the task is not ended with the genera-
well-being relies on the use of these data Indeed, tion of these volumes. A critical evaluation of much
recognition of this importance is indicated by a of the data is still needed. Why are discrepant results
mere reading of the list of the financial sponsors of obtained by different experimentalists? What un-
the Thermophysical Properties Research Center; detected sources of systematic error may affect some
leaders of the technical industry of the United States or even all measurements? What value can be derived
and agencies of the Federal Government are well as a "recommended" figure from the various con-
represented. flicting values that may be reported ? These questions
Experimental measurements made in a labora- are difficult to answer, requiring the most sophisti-
tory have many potential applications. They might cated judgment of a specialist in the field. While a
be used, for example, to check a theory, or to help number of the volumes in this Series do contain
design a chemical manufacturing plant, or to com- critically evaluated and recommended data, these
pute the characteristics ol a heat exchanger in a are still in the minority. The data are now being
nuclear power plant. The progress of science and more intensively evaluated by the staff of TPRC as an
technology demands that results be published in the integral part of the effort of the National Standard
open literature so that others may use them. For- Reference Data System (NSRDS). The task of the
tunately for progress, the useful data in any single National Standard Reference Data System is to
field are not scattered throughout the tens of thou- organize and operate a comprehensive program to
sands of technical journals published throughout prepare compilations of critically evaluated data on
the world. In most fields, fifty percent of the useful the properties of substances. The NSRDS is ad-
work appears in no more than thirty or forty journals. ministered by the National Bureau of Standards
However, in the case of TPRC, its field is so broad under a directive from the Federal Council for Science
vil
f"
w
viii Foreword
and Technology, augmented by special legislation books. Scientists and engineers the world over are
of the Congress of the United States, TPRC is one indebted to them. The task ahead is still an awesome
ofthe national resources participating in the National one and I urge the nation's private industries and all
Standard Reference Data System in a united effort concerned Federal agencies to participate in fulfilling
to satisfy the needs of the technical community for this national need of assuring the availability of
readily accessible, critically evaluated data.
As a representative of the NBS Office of Stan-
standard numerical reference data for science and
technology.
i
dard Reference Data,l want tocongratulate Professor EDWARD L. BRADY
Touloukian and his colleagues on the accomplish- Associate Director for Information Programs
ments represented by this Series of reference data National Bureau of Standards
i mi tm m -I mt a^i m*
r
Preface
ThcrmophysUat Properlies of Maller, the TPRC numerical data of science and technology without a
Data Series, is the culmination of twelve years of continuing activity on contemporary coverage. The
pioneering effort in the generation of tables of loose-leaf arrangements of many works fully recog-
numerical data for science and technology. It nize this fact and attempt to develop a combination
constitutes the restructuring, accompanied by ex- of bound volumes and loose-leaf supplement arrange-
tensive revision and expansion of coverage, of the ments as the work becomes increasingly large.
original TPRC Data Book, first released in I960 in TPRC's Data Update Plan is indeed unique in this
loose-leaf format, ll'xl?' in size, and issued in sense since it maintains the contents of the TPRC
June and December annually in the form of supple- Data Series current and live on a day-to-day basis
ments. The original loose-leai" Daia Book was or- between editions. In this spirit, I strongly urge all
ganized in three volumes: (I) metallic elements and purchasers of these volumes to complete in detail
alloys, (2) nonmetallic elements, compounds, and and return the Volume Registration Certificate
mixtures which are solid at NT.P.. and (3) non- which accompanies each volume in order to assure
metallic elements, compounds, and mixtures which themselves of the continuous receipt of annual
are liquid or gaseous at N.T.P. W ithin each volume, listing of corrigenda during the life of the edition.
each property constituted a chapter. The TPRC Data Scries consists initially of 13
Because of the vast proportions the Data Book independent volumes. The initial ten volumes will
began to assume over the years of its growth and the be published in 1970, and the remaining three by
greatly increased effort necessary in its maintenance 1972. it is also contemplated that subsequent to the
by the user, it was decided in 1967 to change from the first edition, each volume will be revised, updated,
loose-leaf format to a conventional publication. and reissued in a new edition approximately every
Thus, the December 1966 supplement of the original tillh ye<r. The organization of the TPRC Data Scries
Data Book was the last supplement disseminated by makes each volume a self-contained entity available
TPRC. individually without the need to purchase the entire
While the manifold physical, logistic, and Series.
economic advantages of the bound volume over the The coverage of the specific thermophysical
loose-leaf oversize format are obvious and welcome properties represented by this Series constitutes the
to all who have used the unwieldy original volumes, most comprehensive and authoritative collection of
the assumption that this work will no longer be numerical data of its kind for science and technology.
kept on a current basis because of its bound format Whenever possible, a uniform format has been
would not be correct, fully recognizing the need of used in all volumes, except when variations in
many important research and development programs presentation were necessitated by the nature of the
which require the latest available information. property or the physical stale concerned. In spite of
TPRC has instituted a Data Update Plan enabling the wealth of data reported in these volumes, it
the subscriber to inquire, by telephone if necessary, should be recognized that all volumes are not of the
for specific information and receive, in many in- same degree of completeness. However, as additional
stances, same-day response on any new data pro- data are processed at TPRC on a continuing basis,
cessed or revision of published data since the latest subsequent editions will become increasingly more
edition. In thiscontext. the TPRC Data Series departs compleif and up to date. Each volume in the Series
drastically from the conventional handbook and basically comprises three sections, consisting of a text,
giant multivolume classical works, which are no the body of numerical data with source references,
longer adequate media for the dissemination of and a material index.
IX
**
L _
Preface
The aim of the textual material is to provide a the result of obtaining internally consistent sets of
complementary or supporting role to the body of property values, termed the "recommended reference
numerical data rather than to present a treatise on values." In such work, gaps in the data often occur,
the subject of the properiy. The user will find a basic for ranges of temperature, composition, etc. When-
theoretical treatment, a comprehensive presentation ever feasible, various techniques are used to fill in
of selected works which constitute reviews, or com- such missing information, ranging from empirical
pendia of empirical relations useful in estimation of procedures to detailed theoretical calculations. Such
the property when there exists a paucity of data or studies are resulting in valuable new estimation
when data are completely lacking. Established methods being developed which have made it possible
major experiir.Tital techniques are also briefly to estimate values for substances and/or physical con-
reviewed. ditions presently unmeasured or not amenable to
The body of data is the core of each volume laboratory investigation. Depending on the available
and is presented in both graphical and tabular formats information for a particular property and substance,
for convenience of the user. Every single point of tho end product may vary from simple tabulations of
numerical data is fully referenced as to its original isolated values to detailed tabulations with generating
source and no secondary sources of information are equations, plots showing the concordance of the
used in data extraction. In general, it has not been different values, and, in some cases, over a range of
possible to critically scrutinize all the original data parameters presently unexplored in the laboratory.
presented in these volumes, except to eliminate The TPRCData Series constitutes a permanent
perpetuation of gross errors. However, in a signifi- and valuable contribution to science and technology.
cant number of cases, such as for the properties of These constantly growing volumes are invaluable
liquids and gases and the thermal conductivity of sources of data to engineers and scientists, sources in
all the elements, the task of full evaluation, synthesis, which a wealth of information heretofore unknown
and correlation has been completed. It is hoped that or not readily available has been made accessible.
in subsequent editions of this continuing work, We look forward to continued improvement of both
not only new information will be reported but the format and contents so that TPRC may serve the
critical evaluation will be extended to increasingly scientific and technological community with ever-
broader classes of materials and properties. increasing excellence in the years to come. In this
The third and final major section of each volume connection, the staff of TPRC is most anxious to
is the material index. This is the key to the volume, receive comments, suggestions, and criticisms from
enabling the user to exercise full freedom of access to all users of these volumes. An increasing number of
its contents by any choice of substance name or colleagues are making available at the earliest pos-
detailed alloy and mixture composition, trade name, sible moment reprints of their papers and reports as
synonym, etc. Of particular interest here is the fact wel! as pertinent information on the more obscure
that in the case of those properties which are re- publications. I wish to renew my earnest request that
ported in separate companion volumes, the material this procedure become a universal practice since it
index in each of the volumes also reports the con- will prove to be most helpful in making TPRC's
tents of the other companion volumes* The sets of continuing effort more complete and up to date.
companion volumes are as follows: It is indeed a pleasure to acknowledge with
gratitude the multisource financial assistance re-
Thermal conductivity: Volumes I. 2. 3
ceived from over fifty of TPRC's sponsors which
Specific heat: Volumes 4. 5, 6
has made the continued generation of these tables
Radiative properties: Volumes 7, 8, 9
possible. In particular, I wish to single out the sus-
Thermal expan >a: Volumes 12, 13
tained major support being received from the Air
The ultimate aims and functions of TPRC's Force Materials Laboratory-Air Force Systems
Data Tables Division are to extract, evaluate, re- Command, the Office of Standard Reference Data-
concile, correlate, and synthesize all available data National Bureau of Standards, and the Office of
for the thermophysical properties of materials with Advanced Research and Technology- National Aero-
nautics aad Space Administration. TPRC is indeed
*For the first edition of ihe.Scries, this arrangement was not
Ceasihle for Volume 7 due lo the sequence and the schedule
proud to have been designated as a National In-
of its publication. This situation will be resolved in sub- formation Analysis Center for the Department of
sequent editions. Defense as well as a component of the National
-a-
Preface xl
Standard Reference Data System under the cog- thank those members of the staff, research assistants,
nizance of the National Bureau of Standards. graduate research ass-stants, and supporting graphics
While the preparation and continued mainten- and technical typing personnel without whose dili-
ance of this work is the responsibility of TPRC's gent and painstaking ;fforts this work could not have
Data Tables Division, it would not have been possible materialized.
without the direct input of TPRC's Scientific Docu-
Y. S. TOULOUKIAN
mentation Division and, to a lesser degree, the
Theoretical and Experimental Research Divisions. Director
The authors of the various volumes are the senior Thermophysical Properties Research Center
staff members in responsible charge of the work. Distinguished A tkins Professor of Engineering
It should be clearly understood, however, that
many have contributed over the years and their Purdue University
contributions are specifically acknowledged in each Lafayette, Indiana
volume. 1 wish to take this opportunity to personally July 1969
UMta <
Introduction to Volume 2
This volume of Thermophysical Properties of Matter. increasing number of materials which can be
the TPRC Data Series, is among the more compre- reasonably well characterized to enable critical
hensive of all the volumes of the Series. Indeed, it analysis.
is the result of one of TPRC's oldest data tables As stated earlier, all data have been obtained
programs, initiated in 1960. from their original sources and each data set is so
The volume comprises three major sections: referenced. TPRC has in its files all documents cited
namely, the front text material together with its in this volume. Those that cannot be readily obtained
bibliography, the main body of numerical data and elsewhere are available from TPRC in microfiche
its references, and the material index. form.
The text material is intended to assume a role The material index at the end of the volume
complementary to the main body of numerical covers the contents of all three companion volumes
data which is the primary purpose of this volume. (Volumes 1, 2, and 3) on thermal conductivity.
It is felt that a concise discussion of the theoretical It is hoped that the user will find these comprehensive
nature of the property under consideration together indices helpful.
with a review of predictive procedures and recognized This volume has grown out of activities made
experimental techniques will be appropriate in a possible by TPRC's Founder Sponsors and through
major reference work of this kind. The extensive the principal support of the Air Force Materials
reference citations given in the text should lead the LaboratoryAir Force Systems Command, under
interested reader to sufficient literature for I detailed the monitorship of Mr. John H. Charlesworth.
study. It is hoped, however, that enough detail is The limited effort on the critical analysis of the
presented for this volume to be self-contained for data for the elements and some oxides was made
the practical user. possible through the support of the Office of
The main body of the volume consists of the Standard Reference DataNational Bureau of
presentation of numerical data compiled over the Standards, under the monitorship of Dr. Howard J.
years in a most comprehensive and meticulous White, Jr. Over the past nine years, many graduate
manner. The ,cope of coverage includes most students and research assistants have rendered
nonmetallic materials of engineering importance assistance for long or short periods under the
which are in the solid state at normal temperature authors' supervision. We wish to acknowledge in
and pressure. The extraction of all data directly chronological order of their association with TPRC,
from their original sources ensures freedom from the contributions of Messrs. C. V. Wang, K. C. Lin,
errors of transcription. Furthermore, some gross D. Y. Nee, R. L. Feng, J. J. G. Hsia, M. Mangkorn-
errors appearing in the original source documents kanok, M. Nalbantyan, G. K Kirjilian, and Mrs.
have been corrected. The organization and presenta- E. K. C. Lee and Mr. K. Y. Wu. The two last
tion of the data together with other pertinent mentioned are still at TPRC and participated in the
information on the use of the tables and figures are final organization of the tables and figures and the
discussed in detail in the text of the section entitled demanding task of checking details. We also wish to
Numerical Data. acknowledge the benefit of extensive discussions with
While only a very limited number of the Dr. J. Kaspar, Senior Staff Scientist, Materials
materials reported have been critically evaluated, Sciences Laboratory, Aerospace Corporation. He
it is planned that the policy of Volume 1 will be is also a Visiting Research Professor at TPRC.
extended and that future editions of this volume Inherent to the character of this work is the
will include the "recommended values" for an fact that in the preparation of this volume, we have
xiii
xiv Introduction to Volume 2
drawn most heavily upon the scientific literature and The authors and their contributing associates
feel a debt of gratitude to the authors of the are keenly aware of the possibility of many weak-
referenced articles. While their often discordant nesses in a work of this scope. We hope that we
results have caused us much difficulty in reconciling will not be judged too narshly and that we will
their findings, we consider this to be our challenge receive the benefit of your suggestions regarding
and our contribution to negative entropy of infor- references omitted, additional material groups
mation, as an effort is made to create from the needing more detailed treatment, improvements in
randomly distributed data a condensed, more presentation, and, most important, any inadvertent
orderly state. errors. If the Volume Registrali-m Certificate accom-
While this volume is primarily intended as a panying this volume is returned, the reader will
reference work for the designer, researcher, experi- assure himself of receiving annually a list of corre-
mentalist, and theoretician, the teacher at the genda as possible errors come to our attention.
graduate level may also use it as a teaching tool to
point out to his students the topography of the state Lafayette, Indiana Y. S. TOULOUKIAN
of knowledge on the thermal conductivity of non- July 1969 R. W. POWELL
metallic solids. We believe there is also much food C. Y. Ho
for reflection by the specialist and the academician P. G. KLEMENS
concerning the meaning of "original" investigation
and its "information content."
-
Contents
Foreword Ml
Preface l\
x\
*** MM*
xii Contents
Numerical Data
Numerical Data on Thermal Conductivity of Nonmetallic Solids (See pp. xviii to xxix for detailed listing
of entries for each of the following groups of materials) I
1. Elements ........... 1
2. Single Oxides . 93
3. Oxide Compounds ......... 251
4. Binary Mixtures of Single Oxides and/or Oxide Compounds 321
5. Multiple Mixtures of Single Oxides and/or Oxide Compounds 453
6. Mixtures of Oxide and Nonoxide 541
7. Borides 561
8. Bromides 565
9. Carbides 571
10. Chlorides 613
11. Fluorides and Their Mixtures 627
12. Nitrates 647
13. Nitrides 653
14. Phosphates 679
15. Sulfates .... 687
16. Sulfides and Their Mixtures 697
17, Cermets .... 707
- *
ti>iii
1 18. Miscellaneous Inorganic Compounds and Mixtures
Contents x*ii
757
19. Minerals ......... 797
20. Aggregate Mixes 861
21. Miscellaneous Refractory Materials a.)r\Ji (rla>SS*< 889
22. Polymers 943
23. Miscellaneous Organic Compounds 985
24. Systems . 1009
25. Animal and Vegetable Natural Substances and Their Derivatives 1059
26. Fabrics, Yarns, and Hairs ....... 1093
27. Processed Composites 1107
28. Processed Mineral Substances ...... 1135
29. Slags and Scales 1147
30. Residues 1155
References to Data Sources ....... 1159
Material Index
Material Index to Thermal Conductivity Companion Volumes I, 2. and 3 Al
***mmm*m
xvlii Grouping of Materials and List of Figures and Tables
ELEMENTS
1 Boron B I
2 Carbon C 5
:i Carbon (Diamond) C 9
Carbon (Graphite) C
4 AGOT Graphite 13
5 ATJ Graphite 20
AWG Graphite 24
7 Pvrolvtie Graphite M
8 SA-25 Graphite 42
< K75S Graphite 45
hi M9()S Graphite 4
11 Miscellaneous Graphite J 53
11 Iodine I 83
13> Phosphorus P 86
U* Sulfur S 89
2. SINGLE OXIDES
3. OXIDE COMIHJUNDS
Number marked with an asterisk indicates that recommended values are also reported for this material
on separate figure and table of the same Dumber followed by the letter li.
xx Grouping of Materials and List of Figures and Tables
Figure and/or
Namt Page No.
Table No.
II
Grouping of Materials and List of Figures and Tables xxi
Figure and/or
Name Formula Page No,
Table No.
120 Aluminum Oxide + Silicon Dioxide + ..\i AljO, 4 SiO, + EXj 453
121 Aluminum Oxide + Titanium Dioxide + DCj AljO, + TiO, 4 EXj 456
122 Barium Oxide + Silicon Dioxide + ^Xi BaO + S10| 4 EXj 467
12.1 Barium Oxide + Strontium Oxide + EXj BaO + SrO 4- EX, 460
124 Beryllium CJMde + Aluminum Oxide + LXj BeO + A1,0, + EXj 461
125 Beryllium Oxide + Magnesium Oxide + EXj BoO + MgO + EX, 464
12(1 Beryllium Oxide + Thorium Dioxide 4- IXi BeO + ThOi + EX, 467
127 Beryllium Oxide + Zirconium Dioxide + EXj BeO + Zr! 4 EXj 470
128 (di)Chromium Trioxlde + Magnesium Oxide + EXj Cr^ + MgO + EX, 473
1211 Lead Oxide + Silicon Dioxide * :.\1 PbO + SlOj + EXj 474
130 Magnesium Oxide + Calcium OKide + ,.X1 MgO + CaO + ZXj 477
l:u Magnesium Oxide + (di)Chromlum T( (de + IXj MgO + Cr,0, + EXj 480
132 Magnesium Oxide + (dl)Iron Trioxlde < ZXi MgO + FejO, + EXj 483
133 Magnesium Oxide + Silicon Dioxide 4- JXj MgO y SIO, 4 EXj 484
1.14 Silicon Dioxide + Aluminum Oxide + EX SIO, + AljO, + EX, 487
135 Silicon Dioxide 4- Barium Oxide + SX SIO, + BaO + EX, 495
136 Silicon Dioxide + Boron Oxide + EXj SiO + Bf>, 4 EX, 498
137 Silicon Dioxide 4- Calcium Oxide + EXj SiO, 4 CaO + IX, SOJ
138 Silicon Dioxide + Lead Oxide + EXj SlOj 4 PbO 4 EX, 504
131 Silicon Dioxide 4- (dl)Potasium Oxide + EXj SIO, + K|0 + EX, 507
140 Silicon Dioxide 4 (di)Sodium CKide 4- EXj SIO, 4 NajO 4 EXj 5Jo
141 Strontium OKide + Lithium Aluminate + EXj SrO + L1,0 AljO, + EXj . . . 513
142 Strontium OKide + Lithium Zirconium Silicate +
EXj Sr04 U,0-ZrO-SiC),+EXj . . . 514
14:i Strontium Oxide 4 Titanium Dioxide + EXj SrO + TiO, 4 EXj 517
144 Strontium Oxide + zinc Oxide + EXj SrO + ZnO 4 EXj 520
14;. Tin Dioxide + Magnesium Oxide + EXj SnO, 4 MgO 4 EXj 523
14(i Tin Dioxide + Zinc Ofcide + EX, SnO, + ZnO 4 EXj 524
147 Zinc Oxide + Strontium Oxide + EXj ZnO 4 SrO + DC, 527
14^ Zinc CKlde Tin Dioxide 4 EX, ZnO + SnO, + ZX, 528
1411 Zirconium Dioxide + Calcium Oxide + EXj ZrO, + CaO + EXj 531
160 Zirconium Dioxide + Silicon Dioxide 4 J3C1 ZrO, + SiO, 4 EXj 534
151 Zirconium Dioxide 4 Yttrium Oxide + EXj ZrO + YjO, 4 EXj 537
Figure and/or
Name Formula Page No.
TaWe No.
7. IODIDE
BHOMIDES
9. CAB BIDES
1
-, -^ .
I Grouping of Materials and List of Figures and Tables xxlii
10. CHLOR1DK
12. NITRATES
13. NITRIDES
14. raOSPHATEB
15. SULFATKS
Figure and/or
Name Formula Page No.
Table No.
17. CERMETS
-7~
. --
Figure and/or
Name Formula Page No.
Table No.
1. MINERALS
IM Basalt 797
M Beryl 800
M Clay 803
HI Coal 807
HI Dolomite 810
HI Earth 813
Gabbro 816
J71 Granite 817
m Limestone 820
m Mica 823
.'74 Perllte 827
J7r> Rock 828
IN Salt 832
-77 Sand 833
278 Sandstone 840
J7y Siliimanite 845
UNO Slate 846
M Soil 847
^2 Spinel 848
283 Spodumene 851
M Steatite 852
285 Tourmaline 855
.
'
Figure and/ur
Nanu1 V.
Table No.
2S Tuff BS6
287 Wullastonile M
H Cement w
288 Concrete 862
M Piaster Ml
22. POLYMERS
Number marked with an asterisk indicates 'iiat recommended values are also reported for this material
on separate figure and table of the same nuinber followed by the letter R.
Grouping of Materials and List of Figures and Tables xxvll
Hpfra and/or N
Namt Formula Page No.
TabU- No.
U. SYSTEMS
-_ ^
xxvlli Grouping of Materials and List of Figures and Tables
25. ANIMAL AND VEGETABLE NATURAL SUBSTANCES AND THEIR DERIVATIVES (continued)
__ .-
Grouping of Materials and List of Figures and Tables xxix
I Figure ard/or
Table No.
p^ No.
:IU. RESIDUES
j.
d
Theory, Estimation, and Maaauramant
/ ..".
i.
r
-T--^P ,m
i ^li
kMMMHH^ tm^
-
Notation
A Cross-sectional area r Radial distance
a Cube root of atomic volume; Half the focal S Seebeck coefficient
length of an ellipsoid; Axis of ellipse r Temperature
h Amplitude of lattice wave; Axis of ellipse AT" Temperature difference
h Inverse lattice vector / Time
- Specific heat per unit volume
C 'i/a Time required for the back-face tempera-
ow Spectral specific heat ture of a thin-disk specimen to reach half
c, Lattice specific heat per unit volume its maximum value
c Defect concentration r Coefficient of equation (13)
n Thermal diffusivity u Displacement of an atom
E Voltage drop I Electrical potential
Unit vector in the direction of polarization r Velocity of lattice waves; Sound velocity
G Number of atoms in a crystal w Thermal resistivity
k Planck constant , Lattice thermal resistivity
i Klectric current H. Intrinsic lattice thermal resistivity
i Suffix denoting the type of carrier X Reduced frequency (x = hv/xT)
i Index denoting the possible polarizations \ Equilibrium site of an atom
of a wave A.v Distance difference
K Kelvin 3 Index denoting various scattering processes
k Thermal conductivity * Parameter
A, Lattice thermal conductivity r Anharmonicity coefficient
A, Intrinsic lattice thermal conductivity 1 Amplitude decrement
Ar Thermal conductivity of a reference f Local thermal strain
material 9 Debye temperature
L Phonon mean free path for boundary K Boltzmann constant
scattering A Wavelength
1 Mean free path; Effective length of a K Minimum wavelength of lattice waves
specimen corresponding to the maximum wave
l< Phonon mean free path frequency vm
M Atomic mass Wave frequency
N Number of atoms per unit volume % Upper frequency limit of the spectrum of
n Exponent lattice waves
P Slope v Peltier coefficient; Ratio of the circum-
1 Heat flow per unit time; Wave number ference of a circle to its diameter
q Wave vector f Electrical resistivity
la
I
MMgb Mb mm '
OtfflMfll f
r Theory, Estimation, and Measurement 5a
ductivity; however, this neglect may not always be where C(v) is given by equation (4). The lattice
justified. thermal conductivity is thus governed both by the
Because there is some interaction between the magnitude and the frequency dependence of the
different lattice waves, they will tend to be randomly mean free path.
excited, but with an average energy content given The mean free path is limited by several pro-
by the considerations of statistical mechanics. cesses which cause interchange of energy among
In thermal equilibrium at temperature 7", the the lattice waves, or scatter phonons from one mode
lattice specific heat of solids varies as 7"3 at very low into another. These are broadly grouped into
temperatures, and is independent of T at high processes due to anharmonicities of the interatomic
temperatures. The contribution to the specific heat forces, i.e., departures from Hooke's law, into
per unit volume from waves in the frequency interval scattering due to the various kinds of lattice imper-
v and v + dv is given, to a first approximation, by fections, and, as a special case of the last, into
the Debye theory, and is of the form scattering of phonons by the external boundaries.
/TV vV The effective scattering probabilities or recipro-
C(^^ = 9/VK- -dx (4) cals of the mean free path of each group of lattice
Xef (e' - I)3 waves is composed additively of contributions from
when x = IIVIKT is the reduced frequency and N each process, so that
the number of atoms per unit volume. This holds for
I ^ 1 (6)
v < vm; for v > vm, C(v) = 0.
The Debye approximation disregards the dis- Fr^rn
'(O (o) '
persion of the high-frequency lattice wave, dis- where a denotes the various processes. If two
regards differences in polarization, and smears out interaction processes have the same dependence on
the crystal structure of the solid. It is thus a better frequency (v), then it follows from equations (5)
approximation at low temperature, when ill the and (6) that the corresponding thermal resistivities
important waves are long, than at intermediate and follow an additive resistance rule, i.e..
high temperatures. The only concession it makes to
the discreteness of the lattice is the choice of a 1=^ = 2 w(t (7)
cutoff frequency vm or the corresponding minimum "l (o)
wavelength Am = vlvm, where is an average sound where Wia) is the lattice thermal resistivity if only
velocity. The cutoff is chosen so that the total one process (a) were to act. However, if two or more
number of waves corresponds to the correct number processes have different frequency dependences of
of normal modes (3/V per unit volume) which this /(a,(v), then in general
assembly of atoms ought to have.
The lower limit Am of the wavelength is related w, > 2 w'<o (7a)
to a3, the volume per atom, by 4jra3 = 3Am3.
In spite of the obvious inadequacy of the The bigger the difference in frequency dependence,
Debye approximation, it is frequently chosen as a the more pronounced will be the deviation from the
basis for discussing thermal conductivity because additive resistance rule.
the theoretical uncertainties in the phonon mean The interactions due to anh?rmonicities, which
free path usually overshadow errors introduced into may also be viewed as the sea '.ering by thermal
the specific heat by the Debye approximation. vibrations, lead to a mean free path which depends
both on T and v. The other interactions lead to a
mean free path which depends on v only, since the
3. LATTICE THERMAL CONDUCTIVITY
imperfection structure is practically independent of
Since the phonon mean free path is usually a 7". except possibly at very high temperatures.
function of frequency v (it may, of course, also At high temperatures, kg(T) is mainly a reflection
depend on polarization and in extreme cases even of the temperature dependence of /, but at low
on the direction of the wave vector q), the expression temperatures it depends also on the i-dependence of
(3) for the lattice thermal conductivity has to be l(v). This follows because in equation (5)
generalized to
Qv) az T3x*ex{e'~ \)'2 (8)
W)-r OHMM* (5) and if l(v) ac -
K " OC
n n
T~ x' , it follows from equa-
3J n
L -
mm
vT '
I
Theory, Estimation, and Measurement
The conservation condition (I la) corresponds lower magnitude by a factor of order <a>, which
roughly to momentum conservation among the in most solids is about 1 percent at room temperature.
phonons. Umklapp processes must be regarded as a A similar effect, also leading to a T2 term, results
combination of three-phonon processes and Bragg from thermal expansion. This would lower the
reflection. In an elastic continuum only normal effective value of 8 with increasing T, and since Wl
processes would occur. varies as I/o3, it would lead to an increase in thermal
The Peierls' theory is the basis of all subsequent resistivity roughly proportional to T2. This effect
theoretical work. The theory is quite complicated, should also be small.
and has been put into a form suitable for detailed Besides the general review articles, other
work only by subsequent authors. At low tempera- pertinent references to the theory of intrinsic
tures there is a rigid distinction between the roles thermal resistivity at high temperatures are [20, 21,
of normal and I'mklapp processesonly the latter 23, 45, 54 58].
produce thermal resistance, though the former can
indirectly influence the effectiveness of other pro-
5. INTRINSIC RESISTIVITY AT LOW
cesses. At higher temperatures the distinction between
TEMPERATURES
the two types of processes becomes blurred. The
theory, since it involves the inverse lattice vector, At low temperatures the vibrations of the
and thus the details of the crystal structure, becomes lattice cannot be represented as independent vibra-
quite complicated: however, some rough estimates tions of individual atoms, but the representation of
have been made [3, 27]. these vibrations in terms of a superposition of
The intrinsic phonon mean free path, with some lattice waves becomes essential. At this point, the
approximations, takes the following form at high Peierls' theory must be used. The thermal resistance
temperatures arises from Umklapp processes of type (lib).
!//,(.-) oc'r (12) Since the important thermal waves at low tempera-
tures have low frequencies, these processes occur
so that the diveigence difficulties are avoided [3], only as a result of the occasional encounter with a
The intrinsic thermal resistivity is of the form [3, 27] high-frequency wave, of wave vector q comparable
^ = U
$
'1
Ma (*'
(13)
to b/2, where b is an inverse lattice vector. Such a
wave has a frequency vj, when is some parameter,
usually of the order of 2, which depends on the
where M is the atomic mass and a3 the atomic details of the zone structure and on the dispersion
volume. The numerical coefficient V, typically of of the ligh-frequency phonons. The probability
the order 1/3, is somewhat uncertain, and depends of findi ig such a phonon decreases exponentially
on nc details of the crystal structure. with deceasing temperature, so thai
The major factor controlling the intrinsic
M^x -'" (i4)
lattice conductivity is the Debye temperature 0:
solids of high 9 will in general have higher values and the intrinsic thermal conductivity increases
of k,. Another factor is the crystal structuresolids sharply with decreasing temperature, i.e.,
of complex crystal structure have more inverse
MDxf'7" for T<0/6 (14a)
lattice vectors and zone boundaries and a greater
variety of Umklapp processes; such solids will Although there are theoretical expressions for the
have a lower thermal conductivity. However, the precxponential factor [1, 3, 17], these are somewhat
effect of crystal structure on the intrinsic thermal uncertain, and in practice this factor is unimportant
conductivity is still not well understood from a in comparison with the theoretical uncertainty
theoretical point of view. relating to the exponent BI.
While the theory predicts the intrinsic thermal In anisotropic crystals both the preexpcnential
resistivity to vary as T at high temperatures, small factor and exponent BI can depend on the direction
deviations could arise from several causes. Quartic of heat flow. Since B/ depends on the zone structure,
anharmonicities, i.e., terms in the potential energy it can also be changed by phase transition , with
qjiartic in the strain, would lead to foui-phonon important consequences to the thermal conductivity.
processes and a contribution to the resistivity pro- In spite of the theoretical uncertainties, wc
portional to T2. Onewould expect the T2 term tobe of can clearly expect, as Peierls had originally predicted
-
, ~- ^ _
8a Theory, Estimation, and Measurement
[17], that the thermal conductivity of perfect oiC.tx of tens of microns, would resi in a corres-
crystals, which varies roughly as 1/7" at intermediate ponding depression of k(T), and the extension of the
and high temperatures, should increase much more region where k(T) oc C(7") to higher temperatures
rapidly with decreasing temperature at low tempera- than in the case of single crystals. !n that case, the
tures, until the phonon mean free path attains temperature nnge where boundary scattering domi-
macroscopic dimensions. At this point k attains a nates would include a temperature range where
maximum, and at lower temperatures k decreases C(T) varies more slowly than T3. Such casr, have
as T is fuither decreased, since / is kept fixed and been reviewed by Berman [5].
k(T) is now controlled by the specific heat. The effective value of L has been cal.ulated by
However, this presupposes a structurally perfect Casimir [61] for the case of heat flow along the
crystal. Near the conductivity maximum the thermal axis of a narrow cylinder with perfectly rough
conductivity is particularly sensitive to all kinds of surfaces. He assumed that phonons are diffusively
crystal imperfections. In some cases, even the mass scattered at the surface and that there is no effect
variation due to the naturally occurring isotopic from the end surfaces. In this case, L depends
distribution is enough to appreciably depress the entirely on the geometry. In many cases, however,
thermal conductivity around its maximum. phonons arriving at the surfaces may be scattered
In the exponential region also, crystals of with a forward biasthis would lengthen the
higher Debye temperature 6 generally have higher effective values of L correspondingly. This forward
thermal conductivities. bias (often crudely expressed as a fraction specularly
The role of normal processes in the low-tempera- reflected) may be a function of phonon frequency.
ture thermal resistivity has been discussed in [11. The This would make l(v) dependent on frequency, and
phonon mean free path for the normal processes lead to corresponding deviations from the T3
has been given in [22, 59. 60]. dependence of the therinal conductivity. Casimir's
theory has been extended to apply to short cylinders
with smooth surfaces [1,62.63]. The factors con-
6. BOUNDARY RESISTANCE
trolling the degree of specularity of real surfaces
At sufficcntly low tempcratuies, the phonon for phonons of the relevant wavelength (typically
mean free path is limited by the external boundaries. several hundred angstroms) are at present not
Under those conditions understood.
The long cylinder is not the only important
Arm = JC(7>Z. (15)
geometry. Another extreme case is the thin slab,
where L is of the order of the shortest linear dimen- with conduction across the slab. In this case, L is
sion of the specimen. The temperature dependence of the order of the slab thickness, and is governed
of thermal conductivity would then parallel the by the acoustic emissivity and reflectivity, res-
temperature dependence of the specific heat due to pectively, of the surfaces.
lattice waves, and k{T) would vary as T"3 at lowest Since boundary resistance is a resistive process
temperatures. which is not uniformly distributed throughout the
In many cases C(T) is not only due to lattice volume of the specimen, one should not really use the
waves, but there arc additional thermal excitations additivity relation (6) to obtain the combined effect
which contribute to the specific heat, and cause ofboundary scattering and other scattering processes.
substantial deviations from the T"3 dependence Deviations from (6) are likely to be significant, but
expected for lattice waves. Those excitations would will not change the order of magnitude of the
have to be treated as separate carriers according to corresponding resistances.
equation (I). In many cases they have either a lew An interesting case, first discussed in reference
group velocity, or :i short mean free path, or both. [3], is the case when the important processes are
It is thus possible that crystals having substantial boundary scattering and "normal" three-phonon
deviations from a 7"3 dependence of C(7") may still processes (Ila). The normal processes actually
have a 7"3 variation of)!:(/") at low temperatures. decrease the resistivity by slowing down the rate at
In a polycrystalline aggregate the phonon which phonon "momentum" is brought to the
mean path L would he given not by the external surface and obliterated. One can define an effective
dimensions, but by the size of the individual crystal- viscosity of the phonon gas in terms of the normal-
lites or grains. Such grain sizes, typica'ly of the process mean free path. The heat transport or
; r
Theory, Estimation, and Measurement 9
phonon flow is then analogous to Poiseuille flow in role of the "normal" three-phonon processes.
a pipe, while the more usual boundary resistance, These do not reduce the momentum or heat flow
as discussed by Casimir [61], corresponds to of the phonon gas, but they can move momentum
Knudsen flow. This phenomenon occurs only in from one group of lattice waves to another, and by
very perfect crystals near the conductivity maximum. moving momentum to a group of modes for which
the defect scattering is highly effective (such as
modes of higher frequency), these processes can
7. THERMAL RESISTANCES DIE TO
contribute indirectly to the thermal resistivity.
LATTICE IMPERFECTIONS
The exact description of this interplay of processes
Nearly all imperfections scatter lattice waves is mathematically complicated; approximations have
and reduce the lattice thermal conductivity, particu- been given by Klemens [25] and Callaway [32]; for
larly at low and intermediate temperatures, where a recent review see reference [1].
the intrinsic phonon mean free path is long. In all Point defects will depress k, near the thermal
cases, one can regard the imperfection as a local conductivity maximum and. less spectacularly, at
change in the velocity of the lattice wave, either higher temperatures. They will tend to obliterate the
because of a change in mass or density, or because exponential dependence expected for the intrinsic
of a change in the elastic properties. These local thermal conductivity (I4a). and lead to a thermal
changes in wave velocity act as a perturbation, and conductivity roughly proportional to 1/7".
scattering is usually calculated by perturbation At high temperatures, however, point delects
theory [3, 71], though in the simpler defects it has will lead to a slower temperature dependence of the
been possible to arrive at a more self-consistent thermal conductivity; furthermore, the resistivity
solution of the wave equation in the presence of a due to point defects will not increase linearly with
defect through Green's function techniques [87, 88]. concentration. This is a consequence of the properties
According to the simplest perturbation tech- of the integral of equation (5). with C(v) given by
nique, the Born approximation, the perturbation, the high-temperature limit of equation (8). i.e..
which is a function of position, can be Fourier C(i') a v2. and \ll(v) being additively composed of
analyzed, and the scattering of a wave or phonon point-defect scattering, proportional to A and
from mode q into q' involves the (q - q')th Fourier intrinsic scatterint given by equation (12). In the
component of the perturbation. The amplitude of the limit of hijjh le iperatures and high defect con-
scattered wave q' is proportional to that Fourier centration c, one can show [65]
component, the intensity oi'scattering to the square
Af ac[f(l -c)] -i/2T-i;a (16)
of the perturbation, so that total scattering cross
section i are generally proportional to the square of Quantitative estimates of the strength of point
the perturbation. This has been reviewed by several defect scattering can be made in terms of the
authors [1,3,4,7]. The theory bears close resem- difference between the mass of a normal site and a
blance to other theories describing scattering of defect site [25] and in terms of the volume misfit [1, 7],
waves by obstacles. The magnitude and frequency dependence of
It follows that, for waves of a particular the scattering by point defects is also sensitive to
wavelength, the most important obstacles are those short-range order or other types of correlation. The
having dimensions comparable to the wavelength. formal theory [122] is analogous to the theory of
At intermediate and high temperatures, the important x-ray scattering, however, there is little information
defects are thus mainly point defects, while extended about such correlations in nonmetals and no detailed
defects are more important at lower temperatures. calculations have been made.
Another factor to be considered, particularly Extended defects which have been treated
when the defect scattering cross section varies theoretically include dislocations and stacking faults.
rapidly with frequency (e.g., point defects and In the simple theory the dislocations are treated as
concentrated line defects, where 1// varies as t4 and fixed "l position, scattering because of their long-
v3, respectively), is the interplay with other interaction range strain fields. In nonmetals, where dislocation
processes. Not only is it essential to consider other densities are usually lower, this may not be an
interaction processes such as boundary or Enhar- adequate model. Whether one must seek a solution
monic scattering to remove the low-frequency in terms of the flutter of dislocations under the
divergence, but one must consider in detail the applied stress of a low-frequency lattice wave, or in
10a Theory, Estimation, and Measurement
terms of electrostatic interactions between a charged be scattered much more strongly than one would
core and other charges in the solid is not clear at expect from passive defects of comparable size. This
present. leads to changes in the temperature dependence of
Pertinent references to the theory of thermal the thermal conductivity, in extreme cases to dips
resistance due to lattice imperfections at high tem- in the conductivity. The theory of mechanical
peratures are [64 69] and at low temperatures include resonances is not well understood. In the case of
(70 120], of which the references [92 120] deal with some paramagnetic impurities whose electronic level
point defects of the general type and explain the structure is strongly strain dependent, the resonant
thermal resistance in terms of phonon-defect scattering of lattice waves can be calculated from the
resonant scattering processes. spin-lattice relaxation. Effects of this type are clearly
important in many crystals at low temperatures,
particularly in the case of semiconductors with
8. AMORPHOUS SOLIDS
donor or acceptor impurities or radiation damage.
In amorphous solids, the mean free path of
lattice waves is short; in fact, it is questionable
10. OTHER CASES
whether one may describe the thermal vibrations in
terms of lattice waves. Kittel [121] suggested that We have so far discussed the contribution of
the thermal conductivity can be described by lattice waves (or phonons) to the thermal con-
equation (3) with a mean free path which is quite ductivity of ordinary nonmetallic solids and the
short (typically of the order of 10 angstroms) and various scattering mechanisms which reduce the
independent of temperature. This seems to hold at phonon mean free path and cause thermal resistances.
high and intermediate temperatures. At low tem- For other special kinds gf solids such as magnetic
peratures, however, when the wavelength of the insulators, solids partially transparent to infrared
lattice waves becomes longti, the amorphous solid radiation, and semiconductors which are practically
resemblo more and more an elastic continuum, and insulators for purposes of thermal conductivity, we
the randomness of the underlying atomic structure have to consider other mechanisms of heat transfer
becomes less important. This means that, at low and other mechanisms of resistivity.
temperatures. /, should increase with decreasing In a magnetic insulator at low temperatures,
temperature, as is indeed found. A formal theory of cooperative effects between the magnetic moments
the scattering of elastic waves in such random arranged in a regular lattice, leading to the concept
structures has been given [122]. One interesting of spin waves or magnons, can act both as a new
consequence is that the role of order is reversed mechanism of heat transport and at the same time
from what one would expect intuiti\ely. The role of as a resistive mechanism of phonon transport
order or structural coherence is now to reinforce [137 164]. The exchange energy between neighboring
the scattering process. However, our knowledge of spins of atoms is probably a rough criterion of the
the structure of amorphous material is so rudimentary upper limit of temperature at which these effects need
that we have at the moment no predictive theory. to be considered. At very low temperatures the spin-
Other references to the theory of the thermal wave thermal conductivity of a ferromagnetic
conductivity of amorphous solids include [123 126]. insulator is roughly proportional to T2. Consequently,
at sufficiently low temperatures where the mean free
paths of both magnons and phonons become
9. RESONANT SCATTERING
boundary limited, frequency independent, and of
So far we have considered defects which scatter equal magnitude, the magnon conductivity, varying
passive!) that is. scattering is due to local variations as r2, should exceed the phonon conductivity, which
in the wave velocity. There are geometrical inter- varies as T"3 under these conditions. The total
ferences, leading to reinforcement or destructive thermal conductivity is the sum of the magnon and
interference of the scattered wave. However, it is phonon conductivities.
also possible to have dynamic or time-like inter- It is well known that the apparent thermal
ferences. The defect may have internal mechanical conductivity of glasses increases very rapidly at high
resonance frequencies [92 120], or it may have an temperatures and that the thermal conductivity
electronic level structure [127 136]. Lattice waves at versus temperature curves for many translucent
or near the corresponding resonance frequencies will crystals turn up at high temperatures after steady
,1..^.^"
Theory, Estimation, and Measurement 11a
decrease and thus exhibit minima in the curve. This duction. At sufficiently high temperatures, it becomes
is due to the enhanced radiative (photon) heat intrinsic and both the conduction and valence bands
transfer through the material at high temperatures make comparable contributions. This leads to the
in addition to the lattice (phonon) thermal con- ambipolar diffusion of electrons and holes [179-181]
duction. If the material is completely transparent to and gives rise to the transport of ionization energy
infrared radiation, there is no interaction between in addition to the normal direct transport of energy
radiation and material. If the material is opaque, by the carriers. In the ambipolar diffusion process,
heat transfer is entirely by conduction processes. electron hole pairs are created at the hot end of the
Only for the intermediate case where the material is specimen and absorb energy from the heat source.
partially transparent to infrared radiation one can They move down to the cold end of the specimen
speak of a radiative component of thermal con- under the influence of the temperature gradient and
ductivity, which has been the subject of numerous recombine there at the cold end, giving up the
investigations (165 178]. ionization energy to the surroundings. The enhance-
In a material which is partially transparent to ment of the Lorenz function of an intrinsic semi-
infrared radiation, each volume element absorbs a conductor associated with the ambipolar diffusion
part of the incident radiation and also reradiates process can be very significant.
radiant energy. A certain amount of energy is In certain semiconductors the additional heat
therefore transmitted through the material by these transport at high temperatures, which cannot be
radiation and reradiation processes in addition to explained in terms of the conduction processes so
that conducted by lattice waves. The apparent total far mentioned, has been attributed to the exciton
thermal conductivity is the sum of the lattice and contribution to thermal conductivity [182 184].
radiative conductivities. In the limiting case, where Excitons arc bound electron hole pairs which remain
the sample is optically thick, i.e.. the thickness of the associated so that they are electrically neutral and
sample is much larger than the mean free path of the can transport excitation energy but no electrical
photons, the apparent radiative thermal conductivity charge. However, the exciton contribution to heat
is proportional to Tl and inversely proportional to transport is only a rather remote possibility and the
the Rosseland mean extinction coeftkient of the experimental evidence is conflicting. The exciton
material. In the opposite limiting case where the contribution could be significant only if the excitons
sample is optically thin, the apparent radiative have sufficiently low excitation energy.
thermal conductivity is proportional to the thickness In semiconductors the lattice thermal resistances
of the sample as well as to T3, and is therefore not are caused by the same factors as those for dielectric
an intrinsic property of the material. crystals except for scattering of phonons by electrons
Finally we must consider the thermal conduct- [185 194]. However, this phonon electron scattering
ivity of semiconductors. In many semiconductors is important only at very low temperatures. In the
the lattice thermal conductivity is predominant and case of semiconductors having high carrier con-
the electronic component is small enough to be centrations, the phonons are scattered by electrons
neglected. There are. however, a few cases where the (or holes) free to move in some sort of band which is
electronic component of thermal conductivity is not not full [185,186]. For low carrier concentrations, the
negligible at higher temperatures. At sufticiently phonons are scattered by bound electrons [189 191].
low temperatures, a typical semiconductor is The thermal conductivity of semiconductors
extrinsic, with only one band, either the conduction has been comprehensively reviewed in [I I]. Some less
or valence band, making a contribution to con- extensive reviews are also available [195 201].
I -r-
~
u
14a Theory, Estimation, and Measurement
'
^~
be wound directl> onto the specimen to eliminate the rod method except for the specimen length-to-
contact resistance between heater and specimen) or width ratio being greatly reduced to a small fraction.
by a carbon resistor attached to the end. The tem- This specimen geometry is favorable for measuring
peratures may be measured by gas thermometers, poor conductors because the smaller the length to
vapor-pressure thermometers, thermocouples, re- width ratio, the smaller is the ratio of lateral heat
sistance thermometers, or magnetic-susceptibility losses to the heat flow through the specimen, and the
thermometers. General reviews of the low-tempera- shorter is the equilibrium time. The size of specimen
ture measurements and experimental techniques have used in various apparatus designed for different
been presented by White (230, 231]. For details of kinds of materials varies greatly. For apparatus
some of the useful low-temperature apparatus the designed to measure semiconductors, the specimen
reader may consult references [232-243]. used may be about I cm wide [259], while the
For measurements at high temperatures, heat apparatus for measuring less homogeneous insulating
loss becomes a serious problem because radiant heat or refractory materials may require a specimen of
transfer increases rapidly with temperature. To pre- over one foot in width [260].
vent radial heat losses, a guard tube surrounding the In this method, the thermal conductivity is also
specimen with controlled guard heaters may be given by equation (17). The rate of heat flow may be
utilized. Insulating powder is usually used to fill the determined by the electrical power input to a guarded
space between the rod specimen and the guard tube, heater [260 262], by a guarded water-flow calori-
which should have the same temperature distribution meter [263], by a boil-off calorimeter [264 267], or
along it as does the rod specimen. In fact, as early as by a heat flow meter [268]. Temperature measure-
1887, Berget [244, 245] started the use of a guard ring ments are made generally with thermocouples in-
surrounding and with the same temperature distri- serted in the specimen or embedded in grooves on the
bution as the specimen to prevent heat losses. specimen surfaces depending on the materials tested.
The rate of heat flow into the specimen may be Lateral heat losses may be prevented either by utiliz-
determined by measuring the power input to a ing guard heaters or by using a large specimen, of
guarded electrical heater at the free end of the rod which only a relatively small central area is used for
specimen [246 248] or by measuring the heat flow measurement. In the first detailed mathematical
out of the specimen with a water-flow calorimeter at analysis of the plate method reported in 1898, Peirce
the low-temperature end [249], or by both [250 252]. and Willson [269] found already that, if the radius of
Temperature measurements are made usually with the specimen is five times larger than that of the
thermocouples. In order to get correct temperature central test section whose thickness equals its radius,
measurements and to minimize heat conduction the temperature at any point within the central test
along thermocouple leads, the thermocouples should section would not sensibly differ from the tempera-
be made of fine wires of low-conductivity alloys and ture at the corresponding point in an infinite disk of
the leads from the junction should be along iso- the same thickness and same face temperatures.
thermal lines. Further mathematical analyses of the errors due to
This method, as used for measurements at high lateral heat loss in guarded hot plate apparatus have
temperatures, has been comprehensively reviewed been given in [270-272].
and discussed by l.aubitz [253] and Flynn [254]. Detailed descriptions of recent apparatus for
Systematic errors in measurements caused by the measurements at cryogenic temperatures can be
effects of heat losses, thermal contact resistance, poor found in the articles collected in [273], and for
thermocouple contacts, and temperature drift have measurements at high temperatures in [274]. A com-
been analyzed by Bauerle [255]. prehensive review of the plate method has been given
A variation of this method has been used [256- in [275]. A description of the NBS steam calorimeter
258) in which the specimen heater is located in a apparatus and some useful discussions on this
cavity at the center of the rod specimen and a heat method have also been given in [254].
sink is at each end. A mean value of the temperature Therearetwomain kinds of experimental arrange-
gradient established toward the two ends is used for ments for the absolute plate (or disk) method: the
the thermal conductivity calculation. single-plate system and the twin-plate system. The
single-plate system [259, 262-269] requires only one
(/(') Plate {or Disk) Method. This method is suitable specimen, which is placed between a hot plate and a
for poor conductors and insulators. It is similar to cold plate, while the twin-plate-system [260-261]
iin Ti i
16a Theory, Estimation, and Measurement
requires two similar specimens to be sandwiched for measuring the thermal conductivity of good
between a hot plate in the middle and two cold plates conductors, and the "short-specimen" type [279,
on the outside. The plate method employing the 281, 284-287] for measuring poor conductors.
single-plate system was probably first used by Comparative methods have the advantages of
Clement, whose experiment on copper was quoted by simpler apparatus, easier specimen fabrication, and
Pdclet [276] in 1841. Peclet also used this method to easier operation. Their disadvantages include addi-
measure the thermal conductivity of copper, and tional measurement errors due to the required
both of them obtained erroneous results. Later im- additional measurementsof temperatures and thermo-
provements on this method have been made by couple separations, difficulty in matched guarding,
Peirce and Willson (269] and Lees [277] among and lower accuracy due to the additional uncertainty
others. The idea of a twin-plate system was devel- in the conductivity of the reference sample, due to
oped by Lees [277] in 1898, but he did not actually the conductivity mismatch between specimen and
adopt the twin-plate system for his plate method reference sample, and due to the interfacial thermal
in the series of measurements reported in [277]. contact resistance. These have been carefully
However, he used the twin-plate system in his analyzed by Laubitz [253] and Flynn [254]. Flynn
experiments on the effect of pressure on thermal [254] has pointed out that the ASTM standard cut-
conductivity reported in 1899 [278]. Great improve- bar method C408-58 [286] is not well designed and
ment on the plate method employing the twin-plate the data obtained by using this method can be sub-
system was made by Poensgen [261] in 1912, who ject to large errors.
introduced the guard-ring heater to the system as the
(;;) Plate (or Disk) Method. This comparative
prototype of the modern guarded hot-plate appara-
method is suitable for poor conductors and insulators
tus.
and is similar to the divided rod method in principle
b. Comparatire Methods except that the specimen and the reference samples
are now flat plates (or disks) sandwiched between a
In the earliest steady-state comparative method
hot and a cold plate. Christiansen [288] was the first to
suggested by Franklin and carried out by Ingcn-
report in 1881 the use of this type of comparative
Hausz [204] as reported in 1789, rods of various
method in which he compared the thermal conducti-
metals were coated with wax and heated at one end
vity of liquids with that of air. Peirce and Willson
to a common temperature in a bath of hot water or
[269] used this method to measure the thermal con-
oil. The wax melted over a greater distance on a rod
ductivity of marble slabs with glass plates as refer-
of better conducting material, and under steady-
ence material for comparison. Sieg [289] employed
state conditions the ratio of the conductivities of the
the guard ring in his apparatus to prevent lateral heat
rods is roughly proportional to the squares of these
loss.
distances. The modern comparative methods are the
divided-rod (or cut-bar) method and the comparative c. Combined Method
plate method as discussed below. In using a "combined" method, the apparatus
(/) Divided-Rod (or Cut-Bar) Method. The combines the features of both absolute and compara-
divided-rod method was originated by Lodge [279] tive methods. The rate of heat flow is determined
in 1878 and later used by Berget [280], Lees [281], both through a reference sample placed in series with
and many others. In this method a reference sample the specimen and simultaneously by a water-flow
(or samples) of known thermal conductivity is placed calorimeter [290-292] or by measuring the electrical
in series with the unknown specimen with hopefully power input to a heater [293]. In the measurements
the same rate of heat flow through both the reference reported in [293], a "dual combined" method was
and the specimen. Under such ideal conditions, the employed in which a heater is located at the center
thermal conductivity of the specimen is given by of the divided rod between two short specimens with
two longer reference samples at the two ends which
/MA77Ax)r are cooled by flowing water.
it =Ar (18)
A{AT/x) B. Forbes1 Bar Method
where the subscript r designates the reference sample. Forbes' original method [207 210] consists of
This method may be divided into two distinct two separate experiments. The first was termed by
groups: the "long-specimen" type [280, 282, 283] Forbes the statical, and the second the dynamical, or
in -lifi V\i
Theory, Estimation, and Measurement 17
cooling, experiment. In the statical experiment a to the references given for individual methods for
square wrought iron bar with 1.25-inch side and finer details. A comprehensive review of radial heat
8 feet long was heated at one end by molten lead or flow methods has been made by McElroy and
solder at a fixed high temperature, and the steady- Moore [299].
state temperature distribution along the bar was
determined with the surface of the bar losing heat by a. Absolute Methods
convection and radiation to a constant-temperature (0 Cylindrical Method. The cylindrical method
environment. In the thnamical or cooling experi- uses a specimen in the form of a right circular cylin-
ment a sir '.ilar bar, but only about 20 inches long, was der with a coaxial central hole, which contains either
cooled in the same environment from a high uni- a heater or a heat sink, depending on whether the
form temperature and the rate of heat loss was desired heat flow direction is to be radially outward
determined. From these two experiments, the thermal or inward. The use of this method was first reported
conductivity may be computed as follows. by Callendar and Nicolson [300] in \?,-)l for measur-
Replacing Ax/AT" in equation (17) by dxjdT, ing the thermal conductivity of cast iron and mild
diflerentiating the resulting equation with respect to steel. The cylindrical specimens used were 5 inches
x and rearranging gives in diameter and 2 feet long with I-inch coaxial holes
heated by steam under pressure. The outside of the
1 dq 1
*=--!2 (19) cylinder was cooled by water circulating rapidly in a
Adxd Tldx2 spiral tube. Niven [301] in 1905 also used the radial
The statical experiment provides values for d2Tjdx2, heat flow method for measurements on wood, sand,
and the heat loss per unit time per unit length of the and sawdust. His method is close to the so-called
bar in the cooling experiment is hot-wire method developed by Andrews [302] in
1840 and Schleiermacher [303] in 1888 for measure-
dq dT ments on gases. Kannuluik and Martin [304] used
= AC (20)
dx dt the hot-wire method for measurements on powders
as well as on gases.
where dTjdt is the measured cooling rate and C the In the early experiments and also in many later
specific heat per unit volume. designs [305 308], end guards are not employed. The
Hogan and Sawyer [294] have improved this effect of heat losses from the ends of the specimen is
method so that it is not necessary to know the specific minimized by using a long specimen and monitoring
heat of the material. They used a thin long rod en- the electric power within only a small section of the
closed in an isothermal furnace. Radial heat loss specimen away from the ends.
from the specimen was determined by passing an The guarded cylindrical method employing end
electric current through the specimen and measuring guards at both ends of the specimen to prevent axial
the electric power required to maintain it at a tem- heat losses was developed by Powell [309] and first
perature slightly above that of the furnace. This re- reported in 1939 for measurements on Armco iron at
places Forbes' cooling experiment, and it is not high temperatures. In the guarded cylindrical method
necessary to know the specific heat since a steady- the specimen is generally composed of stacked disks
state condition is prevailing. with a coaxial central hole containing either a heater
Hogan and Sawyer's method was further im- or a heat sink. Temperatures within the specimen
proved by Laubitz [295]. In his comprehensive are measured either by thermocouples or by an
review Laubitz [253] has discussed in detail the optical pyrometer. For details of some of the useful
generalized Forbes' bar method, including the other apparatus employing the guarded cylindrical method,
major variants currently in use [296 298]. the reader may consult references [299, 309 314].
The thermal conductivity is calculated from the
C. Radial Heat Flow Methods expression
There are several different types of apparatus all q ta(Vi)
employing radial heat flow. The classification is k m (21)
2W(r1 - T2)
mainly based upon specimen geometry. In the fol-
lowing we will briefly describe the cylindrical, where / is the length of the central heater and Tj and
spherical, ellipsoidal, concentric sphere, concentric T2 are temperatures measured at radii r, and
cylinder, and plate methods. The reader is referred respectively.
--' ~
18a Theory, Estimation, and Measurement
which indicated the variation of thermal conductivity from a heater at the circular edge of a disk of suitable
in the different directions. conductive reference material sandwiched between
It the substance is Isotropie, the bounding two like specimens, which are in turn sandwiched
curve of the melted wax is a circle, whereas for between two circular cold plates at a constant lower
anisotropic substances, this curve is elliptical, temperature. However, the heat flow in this case is
in such a case, the ratio of the two thermal con- not strictly radial, since, P.S the heat flows radially
ductivities jta and kh along the two axes o and h in the conductive disk toward the center, it flows
of the ellipse is given by the expression also from the disk through the specimens to the
cold plates. As a result, the steady-state temperature
(24) of the disk decreases toward its center, and the rate
Ar.
A,, W of decrease depends on the thermal conductivity
of the specimens. Robinson obtained an expression
Powell [333] has modified the method in his for calculating the thermal conductivity of the
simple test for anisotropic materials. In testing specimens from the known thermal conductivity and
gallium, he cooled a slice of crystal locally by means thickness of the disk and from the temperatures of
of a piece of solid carbon dioxide and observed the the cold plates and of the disk at its center and at a
contours of the dew and frost areas which formed suitable radius.
around the cooled zone. For testing graphite, he
followed de Senarmont's original method, but the D. Direct Electrical Heating Methods
surface of the plate used was covered with frost by In direct electrical heating methods, the speci-
precooling instead of being coated with wax. men is heated directly by passing an electric current
through it. These methods are therefore limited to
b. Comparative Methods
measurements on reasonably good electrical con-
(I) Concentric Cylinder Method. This method has ductors. Furthermore, they usually yield thermal
been used for measurements on some special materials conductivity in terms of electrical conductivity
such as those that are radioactive or reactive [334 rather than directly. However, direct electrical heat-
336] and not for ordinary materials, because it does ing methods also have certain advantages over other
not have any major advantage over the absolute methods, and at high temperatures an increasing
method. A typical apparatus of this kind consists number of materials become sufficiently good
of a cylindrical specimen which is surrounded by a electrical conductors. Direct electrical heating offers
concentric cylindrical reference sample of known a means of easily attaining very high temperatures,
thermal conductivity. A coaxial central hole in the uses simpler apparatus and experimental techniques
specimen contains a heat source, which produces than other methods at high temperatures, uses
heat flowing radially through both the specimen and relatively small specimens, requires relatively short
the reference sample. The advantage of using this time to reach equilibrium, and also offers the
method for measuring ladioactive or reactive possibility of con. nrrent determinations of a number
materials is that the reference sample which encloses of physical properties on the same specimen.
the specimen serves also as a means of containment. According to specimen geometry, these methods
The thermal conductivity is determined from the fall into two major categories: cylindrical rod and
expression rectangular bar. They will be briefly discussed below.
(T3- r) InQ-a//-!) Comprehensive reviews [338-340] on direct elec-
k =kr (25) trical heating methods are available.
(r, - ra)In(r4/r3) The thermoelectrical method to be discussed
where T^ and T2 are two temperatures measured in later involves also the direct passage of an electric
the specimen at two radii r, and r-^, respectively, and current through the specimen. However, in that
Tj and TA in the reference sample respectively at method the specimen is heated (and cooled) by the
r3 and r4. Peltier effect which is totally different from the
Joulean heating responsible for maintaining the
(/';') Disk Method. Robinson [337] developed a specimen temperature in the direct electrical heating
method, which he termed the "conductive-disk methods discussed here. It is therefore preferable
method,'" for comparative measurements on insu- to discuss the thermoelectrical method separately
lators. This method employs inward radial heat flow in another section.
1
-T : r-Tj
20 Theory, Estimation, and Measurement
.
Theory, Estimoiion, and Measurement 21a
Earlier reports [339. 362] had contained examples of electrical resistivity also been made, the unusually
similar discrepancies for other high-melting-point low resultant Lorenz function should have provided
metals, such as molybdenum, stainless steel, and warning that abnormal data were being obtained.
platinum. The main reasons for these differences It might well be added that the inclusion of electrical
include failure to measure accurately small tempera- resistivity measurements on all possible occasions
ture gradients at high temperature, failure to match is a simple extra measurement which also serves to
boundary conditions, errors resulting from simplify- provide very useful information about the properties
ing mathematical approximations, and the use of of the material under test and its behavior on temp-
temperature regions in which the thermal conduction erature cycling.
term is s..iall compared with the Joulean heating and The foregoing example also indicates that users
radiation loss terms. of the data tables of these volumes should, in the
These have been quoted as examples of current absence of any analysis that has produced a curve
experimental work at the TPRC, which became of recommended values, tend to be critical of the
necessary because of the need to resolve some values presented, until these are seen to be well
seriously discordant data and to gain further insight supported by independent experiments, correlations,
into their muses. The impression must not be given, or by additional checks such as that of a reasonable
however, that such discrepancies are confined to Lorenz function.
metals or to direct electrical heating methods. An additional outcome of the current TPRC
This is by no means the case, and the literatui- of investigation has been the development of a method
heat conduction contains many examples of dis- and of equipment capable of determining a large
cordant results for all types of methods used. number of high-temperature physical properties [373].
Titanium carbide, one of the materials dealt with Their multiple-purpose apparatus is the first opera-
in this volume may be mentioned. The first deter- tional model that can accurately measure the thermal
minations reported on titanium carbide by Vasilos conductivity, electrical resistivity, total and spectral
and Kingery [366] to high temperatures showed hemispherical emittance. Thomson coefficient, and
the thermal conductivity to decrease from about Loienz function on one and the same specimen.
0.2Wcm C1 at 200 C to O.IWcm'C1 at This apparatus can also measure the specific heat,
500C and 0.04 W cm1 C1 at I000C. Two enthalpy, thermal diffusivity, thermal expansion.
methods had been used : the divided-rod comparative Seebeck coefficient, Peltier coefficient, and Richard-
method for a cube sample up to about 800 C and an son coefficient. The merit of obtaining many different
ellipsoidal radial-flow ncthod from about 500 to physical properties from one and the same specimei
1100 C. The former method gave results which were so as to permit meaningful quantitative cross-
greater by 20 percent to 30 percent over their correlations between properties need not be em-
common temperature range. In 1961 Taylor [367] phasized here.
used a better-substantiated radial heat flow method
for cylindrical samples of titanium carbide, and b. Rectangular Bar Method
found the thermal conductivity to increase linearly This method was developed by Longmire [374]
from0.38 Wem ' C ' at 600 C to 0.47 W cm1 C1 and is a geometrically-deformed variant of the radial
at 1600 C. heat flow method. The specimen used is in the form
These two sets of values, differing at about of a long rectangular bar. This special specimen
1000 C by about one order of magnitude and geometry enables all temperature measurements to
having temperature coefficients of opposite sign be made on the surface of the specimen. As the
naturally aroused interest, and subsequent con- specimen is heated electrically in vacuum, the heat
tributions by Laubitz [368], Hoch and Vardi [369]. loss by radiation establishes a radial temperature
Powell [370. 371], and the nonsteady-state measure- gradient, and the temperature at the center line of
ments of Taylor and Morreale [372] all supported the wider surface of the rectangular bar will be
the higher values of Taylor [367]. It would seem that higher than that at the center line of the narrower
the higher thermal conductivity of titanium carbide surface. From measurements of these two tem-
led to serious enors being associated with the method peratures, the electrical conductivity, and total
of Vasilos and Kingery, which were not apparent hemispherical emittance of the bar, the thermal
for substances of lower thermal conductivity. conductivity can be calculated using the equation
Incidently, had the much simpler measurement of derived by Longmire.
7% ^-7
22a Theory, Estimation, and Measurement
Longmire's method was improved by Pike and The thermal conductivity can be derived from the
Doar [375-377] both in mathematical analysis and in shape and asymptote of this potential drop versus
experimental techniques. They further extended his time curve provided that the Seebeck coefficient is
method to the determination of anisotropy in thermal known.
conductivity.
F. Thermal Comparator Method
E. Thermoelectrical Method
The thermal comparator method was developed
The thermoelectrical method was developed by Powell [386 389] and is a simple comparative
by Borelius [378] and reported in 1917 for the method for the rapid, easy measurement of thermal
combined measurement of the Peltier heat and thermal conductivity.
conductivity of he same material, and is particularly The essential part of the thermal comparator is
applicable to the measurements on thermoelectric an insulated probe with a projecting tip. The probe
materials. is integral with a thermal reservoir held at a tempera-
In this method, the specimen is held between ture about 15 to 20 degrees above room tem-
metallic contacts through which a small direct electric perature. A surface thermocouple is mounted at the
current is passed. Peltier heating thus occurs at one tip of the probe and is differentially connected to the
end of the specimen and Peltier cooling at the other thermal reservoir for the measurement of the tem-
end, which establishes a temperature gradient along perature difference between the reservoir and the tip.
the specimen. Under steady-state conditions, the In operation, the probe is gently placed on the
rate of Peltier heat generation at the hot end is just surface of the test material. Upon contact of the
balanced by the rate of heat conduction from the probe tip of known thermal conductivity A^ and
hot to the cold end. Thus the thermal conductivity originally at temperature 7"i with the surface of the
can be calculated from the rate of Peltier heat test material of thermal conductivity ^ and al
production W {n being the Peltier coefficient), the room temperature. 7"2, the temperature of the probe
temperature dilference between the ends AT, the tip drops quickly to an intermediate temperature,
cross-sectional area A, and the length / by the T. giving the expression
expression
k =
nil
(28)
r.-r-^-r.)^ (29)
I
Theory, Estimation, and Measurement 23a
measurement of the rate of heat flow is required. Consequently, methods using specimens in the form
These methods normally determine the thermal of a small plateordisk havebeendeveloperf[398 400].
diffusivity, from which the thermal conductivity
b. Radial Heal Flow Method
can be calculated with an additional knowledge of
the density and specific heat of the test material. In this method, the specimen in the form of a
Nonsteady-state methods fall into two major cate- cylinder is heated by a heat source capable of
gories, the periodic and the transient heat flow producing a periodical temperature variation either
methods, as briefly discussed below. These methods at the axis or at the circumference, and the radial
have been comprehensively reviewed by Danielson temperature variations with time are measured.
and Sidles [392], and will be dealt with in Volume 10 The thermal diffusivity may be calculated from
of the present TPRC Data Series. iJ*e phase change of the temperature oscillations,
or T'om the amplitude variation of the oscillations
A. Periodic Heat Flow Methods with Kequency.
Tinasawa [401] used this method in 1935 for
In periodic heat flow methods, the heat supplied the measurements on humid materials. In his method,
to the specimen is modulated to have a fixed period. a sinusoidal temperature was produced on the
The resulting temperature wave which propagates surface of a cylindrical specimen, and the tempera-
through the specimen with the same period is tures at different radial distances were measured for
attenuated as it moves along. Consequently, the the calculation of thermal diffusivity.
thermal diffusivity can be determined fiom measure- Filippov and his co-workers have further
ments of the amplitude decrement a.id/or phase developed a method of this type [402] and used it
difference of the temperature waves between certain for the measurements on metals [403] and molten
positions in the specimen, in most of the periodic metals [404, 405] at high temperatures.
heat flow methods, heat flow is in the longitudinal The nonsteady-state radial heat flow method
(axial) direction. However, methods with heat flow has also been employed for measurements on
in the radial direction have also been used. insulators [406, 407],
a. Longitudinal Heat Flow Method B. Transient Heat Flow Methods
The periodic heat flow method was first develop- Transient heat flow methods, both longitudinal
ed by Angstrom [211, 393] and reported in 1861. and radial, were first used by Neumann [408, 409]
In his method a variable heat source capable of and reported in 1862. In his method, one end of a
producing a sinusoidal temperature variation was bar was heated by a flame until the temperature
attached to the center of a long thin rod specimen, attained the equilibrium state. The flame was then
and the temperatures as a function of time at two suddenly removed and the temperatures at two
positions / apart towards the ends of the rod, were positions along the bar were measured as a function
measured. From these temperature time measure- of time. Thermal diffusivity can then be calculated
ments, the velocity, i, and the amplitude from these measurements. For the measurements on
decrement, 8, of the temperature wave can be poor conductors he used another method in which
determined for the calculation of thermal diffusivity. a cube or sphere was heated uniformly to a high
This method has been modified and improved by temperature and then was allowed to cool in the air.
King [394] and others [395-397]. The thermal The temperatures at the surface and at the center
iffusivity may be calculated from the expression were measured as a function of time.
[396] Tht modern transient heat flow methods have
vl a wide variety. In the following a number of the
D = (30) major variants are briefly discussed
2ln8
The Angstrm method, which uses a long rod. a. Longitudinal Heat Flow Method
has its limitations. In some cases, specimens in the Similar to the longitudinal periodic heat flow
korm of long rods may not be available, and in other method, the longitudinal transient heat flow method
cases, sulh as in the measurements on poor conduc- can also be subdivided into two major categories:
tors at high temperatures, heat guarding to prevent those ising a long rod and those using a small plate
lateral heat losses from a long rod may be difficult. (or disk)
||
1
.-/-.i" - '^1
24a Theory, Estimation, and Measurement
Methods in which one end of a long rod, which at different radial distances are measured. In the
is initially atAunilor.n temperature, is subjected to a methods developed by Ginnmgs [422] and by Cape,
short heating pulse have been developed [410, 411 ]. Lehman, and Nakata [423], cylindrical specimens
There are also methods in which steady heating is were continuously heated at the outer surface.
provided at one end of a rod and the temperatures Specimens in the form of hollow disks stacked
as a function of time at two or more positions along on an axial heater with outer disks as end guards
the rod are observed [412 414). have been used by Carter, Maycock, Klein, and
Transient heat flow methods in which the Danielson [424].
specimen used is in the form of a small plate or disk Although the line heat source and probe methods
have been developed by a number of workers are also radial transient heat flow methods, they are
[415-418]. quite different from other methods and will be
discussed in a separate section below.
b. Flash Method
Although the flash method is a variant of the </. Line Heal Source and Probe Methods
longitudinal transient heat flow method using a The line heat source method was originally
small thin disk specimen geometry, it has a very developed by Stalhane and Pyk [425] in 1931 and
special feature which makes it a class of its own. used for measurements on ceramic materials
In the "flash" method, a flash of thermal energy [426]. This method is suitable for the measure-
is supplied to cne of the surfaces of a disk specimen ments on loose-tilled materials such as powders.
within a time ii "rval that is short compared with In this method, a long thin heater wire which
the time required for the resulting transient flow of seives as a line heat source was embedded in a large
heat to propagate through the specimen. This specimen initially at uniform temperature. The
method was developed by Parker, Jenkins, Butler, heater is then turned on, which produces constant
and Abbott [419] and reported in 1961. heat, q. per unit length and time, and the temperature
In use, a heat source such as flash tube or laser at a point in the specimen is recorded as a function
supplies a flash of energy to the front face of a of time. The thermal conductivity is given by the
thin disk specimen and the temperature as a function expression
of time at the rear face is automatically recorded.
The thermal ditfusivity is given from the thickness of
the specimen, /, and a specific time, ri,2, at which the
In- (32)
4AT2 - T,)
back face temperature reaches half its maximum
value by the expression where {T.2 - 7",) is the temperature difference at
two times /, and t2. Subsequently, this method was
D = 1.37 //'tiii (31) also de\clopcd by van der Held and his co-workers
[427, 428] and others.
Other expressions for the calculation of thermal The probe method is a more practical line heat
diffusivity have also been used. source method in which the heat source is enclosed
Subsequent improvements on this method have inside a probe for protection and for easy insertion
been made [420,421] by the application of corrections into a sample. This method was developed by Hooper
for the finite pulse-time effect and the radiation-loss and his co-workers [429, 430] md others. Blackwell
effect, [431, 432] has derived theoretical treatments for
practical departures from a true line source, and in
c. Radial Heat Flow Method the discussion of a paper [433] dealing with the use
As mentioned before, a radial heat flow method of a probe method in connection with the routing
was used by Neumann [408, 409] for measurements of electric power cables, he advocated the use of
on poor conductors. His specimens were of spherical very small thermistors as an alternative to thermo-
shape. couples.
In modern apparatus, specimens in the form of
cylinders are used. A long cylindrical ;pecimen, e. Mating Heat Source Method
hollow or solid, which is initially at uniform tem- The moving heat source method was developed
perature, is heated either at the axis or at the outer by Rosenthal and his co-workers [434 436] and
surface and the temperatures as a function of time involves the establishment of a quasi-steady-state
-*- "T^
-:
r
Theory, Estimation, and Measurement 25
temperature distribution in a long tubular-shaped sample whose properties are known. Initially the
specimen heated by a moving localized heat source two sets are heated separately to uniform but
of constant intensity. As the heat source approaches different temperatures, and then they are suddenly
and moves away, each point in the specimen is brought into contact, with the two test specimens
subjected to a temperature rise and fall. When the touching each other. The transient temperature at
heat source passes over the specimen, the tempera- the contact plane between the test specimen and
ture at a point remote from the ends is recorded as reference sample corresponding to a certain time is
a function of time. From this record, a curve of the measured, and from this the thermal diffusivity
logarithm of the temperature variation with time is of the specimen can be calculated.
made. The thermal diffusivity is given from the Another transient-heat-flow comparative method
velocity of the heat source, v, and the slopes Pr and has been used by Deem el al. [439] for the measure-
P, on the rising and falling portions of the curve at ments on irradiated materials. The method of
the same temperature by the expression measurement is to place the lower ends of a specimen
and a reference sample, which are of the same size
D = (33) and initially at room temperature, in molten tin
Pr + P, maintained at a constant elevated temperature and
then measure ihe times required for the tops of them
/. Comparatite Mvtlwd to reach a predetermined intermediate temperature.
A comparative method employing transient heat The ratio ol the thermal diffusivities is assumed
flow was developed by Hsu [437,438]. In this method. directly proportional to the ratio of the two times
two identical sets of composite blocks are used. measured for the specimen and the reference
Each set consists of a test specimen and a reference material.
I
k, _
References to Text
Review Papers and Books 17. Peierls, R. E.. "The Kinetic Theory of Heat Conduction
in Crystals." Ann. Physik, 5. 3. 1055-1101, 1929; English
1. Klemens, P. G., "Theory of the Thermal Conductivity
translation: OTS, AEC-TR-1849. 1-67. [TPRC No.
of Solids," in Thermal Conduclhily (Tye, R. P., ed.).
28 528].
Vol. 1, Chap. I, Academic Press, London, 1-68, 1969.
18. Peierls. R E.. "Some Typical Properties of Solid Bodies,"
2. Klemens. P. G., "Thermal Conductivity of Solids at
Ann. Inst. Henri Poincart, 5, 177-222, 1935.
Low Temperatures," in Handbuch der Physik (Flgge,
19. Frhlich, H. and Heitler, W., "Time Effects in the
S., ed.). Vol. 14, Springer-Verlag, Berlin, 198-281. 1956.
Magnetic Cooling Method. IIThe Conductivity of
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ASMEJ. of Heat Transfer, Part C, 83(4). 403-8, 1961. Iron and an Armco Iron to 1000 C," /. Appl. Phys..
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Can. J. Phys., 41(10). 1663-78, 1963. burn. P. E., "New Method for the Determination of
298. Laubitz, M. J.. "The Unmatched Guard Method of Thermal Conductivities between 1000 C and 3000 C,"
Measuring Thermal Conductivity. II. The Guardless in Progress in International Research on Thermodynamic
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299. McElroy, D. L. and Moore, 1. P., "Radial Heat Flow eds.), ASME Second Symposium on Thermophysical
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304. Kannuluik, W. G. and Martin. L. H., "Conduction of II. Development of a Thermal Conductivity Expression
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305. Kingery, W. D., "Thermal Conductivity. VI. Determina- 320. Adams. M.. "Thermal Conductivity: III. Prolate
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307. Glassbrenner, C. J. and Slack, G. A.. "Thermal Con- Soc, 37(2), p. 84. 1954.
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308. Banaev. A. M. and Chekhovskoi, V. Ya., "Experimental Insulators." VDIZeitschrift, $1(21),'m-Xl, 1908.
Determination of the Coefficient of Thermal Con- 324. "Design Aspects of Plant for Production of Heavy
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309. PoweM, R. W., "Further Measurements of the Thermal Kl. IIA. 65. 45-69. 1872.
Electrical Conductivity of Iron at High Temperatures," 326. Kropschol, R. H.. Schrodt. J. E.. Fulk. M. M.. and
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310. Powell, R. W. and Hickman. M. J.. "The Physical in Cryogenic Engineering, Vol. 5. Plenum Press, 189-97,
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913 39, 1969. Electrical Conductivity, Heat Capacity, and Thermal
328. de Senarmont. H., "Memoir on the Conductivity of Power of Some Metals," IViss. Ahhandl. Physik-tech.
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21,457-70, 1847. 346. Holm, R. and Strmer. R., "Measurement of the
329. de Senarmont, H., "Memoir on the Conductivity of Thermal Conductivity of a Platinum Probe in the
Crystalline Substances for Heal," Compt. Rend., 2, Temperature Kange 19-1020 C," Wiss. Verdff. Siemens-
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330. dc Senarmont, H., "Memoir on the Conductivity of 347. Angell, M. F., "Thermal Conductivity at High Tem-
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331. de Senarmont, H., "Experiments on the Effects of Electrical Conductivities of Carbon and Graphite to
Mechanical Agents on the Thermal Conductivity of High Temperatures," Proc. Phys. Soc. (London), 51(1),
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332. de Senarmont, H., "Thermal Conductivity in Crystallized Tungsten. Tantalum and Carbon at Incandescent
Substances," Ann. Physik, 73, 191-2, 1848. Temperatures by an Optical Pyrometer Method."
333. Powell, R. W., "A Simple Test for Anisotropie Materials," Phys. Rev., 4(6). 535-43, 1914.
J. Sei. Instr.,30. 210, 1953. 350. Osborn. R. H., "Thermal Conductivities of Tungsten
334. Cohen, I., Lustman, B.and Eichenberg, J. D., "Measure- and Molybdenum at Incandescent Temperatures,"
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Monocarbidc Shaping and Irradiation Study. Final 352. Lebedev, V. V., "Determination of the Coefficient of
Report No. 2, March 1, 1962December 31, 1963," Thermal Conductivity for Metals in the High Temperature
United States-Euratom Joint Research and Development Range,"/"A.IJ. Metals Metallog.(USSR), \m\3\-A, I960.
Program. Rept. EURAEC-I179, 1-110, 1964. [English 353. Bode, K. H., "A New Method to Measure the Thermal
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336. Clough, D. J. and Sayers, J B , "The Measurement of Wrmetech. 10(6), 110-20, and 10(7). 125-42. 1961.
the Thermal Conductivity of UOj under Irradiation in 354. Gumenyuk. V. S. and Lebedev. V. V., "Investigation of
the Temperature Range 150-I6O0C," UKAEA Rept. the Thermal and Electrical Conductivity of Tungsten
AERE-R-4690, 1-55, 1964. and Graphite at High Temperalures," Phys. Metals
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Measuring the Thermal Conductivity of Insulations," 355. Bode, K. H., "Measurements of the Thermal Con-
Bull. Intl. Inst. Refrig. Annexe 1962-1, 43-50, 1962. ductivity of Metals at High Temperatures," in Progress
338. Mikryukov, V. E., "The Thermal Conductivity and in International Research on Thermodynamic and Trans-
Electrical Conductivity of Metals and Alloys. Melal- port Properties. (Masi, J. F. and Tsai, D. H., eds.,
lurgizdat, Moskow, 260 pp., 1959. ASME Second Symposium on Thermophysical Proper-
339. Powell, R. W., DeWitt, D. P., and Nalbantyan. M., ties, Academic Press, New York, 481-99, 1962.
"The Precise Determination of Thermal Conductivity 356. Gumenyuk, V. S., Ivanov, V. E., and Lebedev, V. V.,
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by Direct Electrical Healing Methods," Air Force of Metals at Temperatures in Excess of 1000 C,"
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373. Powell, R. W. and Taylor, R. E., "Multi-Property 390. Powell, R. W., "Thermal Conductivity Determinations
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~ -TP! r,
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Theory, Estimation, and Measurement 39
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Apparatus for the Determination of Thermal Con- 435. Rosenthal, D. and Friedmann. N. E., "Thermal Dif-
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431. Blackwell, J. H.. 'Radial-Axial Hsa' Flow in Regions 437. Hsu, S. T.. "Theory of a New Apparatus for Determining
Bounded Internally by Circular Cylinders." Can. J. the Thermal Conductiv-lies of Metals." Rev. Sei. Instr.,
Phys., 31(4), 472-9, 1953. 28(5). 333-6, 1957.
432. Blackwell, J. ".. "A Transient-Flow Method for 438. Hsu. S. T., "Determination of Thermal Conductivities
Determination of Thermal Constants of insulating of Metals by Measuring Transient Temperatures in
Materials in Bulk. I. Theory." 7. Appl. Phys.. 25. 137-44. Semi-Infinite Solids," Trans. ASME, 79, 1197-1203.
1954 1957.
433. Makowski, M. W. and Mochlinski, K., "An Evaluation 439. Deem, H. W., Pobereskin. M., Lusk, E. C, Lucks.
of Two Rapid Methods of Assessing the Thermal C. F , and Calkins, G. D.. "Effect of Radiation on the
Resistivity of Soil." Proc. Insln. Elect. Engrs.. I03A(11). Thermal Conductivity of Uranium1.6 Wt.0 Zir-
453 70, 1956. conium," USAEC Rept. BMI-986, 1-19, 1955.
- - -
Data Presentation and Related General
Information
1. SCOPE OF COVERAGE results derived from semi-:heoretical relationships,
or from generalized empirical correlations. Besides
Presented in this volume are the thermal con- critical evaluation and analysis of the existing data,
ductivity data for 5 elements, over 100 different thermodynamic principles and semi-empirical tech-
grades of graphites, 53 oxides and oxide compounds, niques are employed to fill in gaps and to extrapolate
82 systems of oxide mixtures, 83 nonoxide com- existing data so that the resulting recommended
pounds, 7 systems of mixtures of oxides and non- values are internally consistent and cover as wide a
oxides. 15 organic compounds, 22 kinds of cermets, range of the controlling parameters as possible.
10 groups of systems, 8 kinds of refractory materials, Future editions of this volume will contain recom-
over 40 different kinds of glasses, 24 minerals, 16 mended values for an increasing number of materials.
polymers, 26 animal and vegetable natural sub-
stances. 30 processed composites and processed
2. PRESENTATION OF DATA
natural and mineral substances, and 10 aggregate
mixes, slags, scales, and residues. These data are The thermal conductivity data and information
obtained by processing over 1260 research docu- on test specimens for each material are generally
ments on the thermal conductivity of nonmctallic presented in three sections arranged in the following
solids dated from around 1800 to 1967. of which order; Original Data Plot, Specification Table, and
about 590 contain usable data. Materials within Data Table. For the elements and a number of
each group are arranged in alphabetical order by oxides. Graph and Table of Recommended Values
name, as listed in the Grouping of Materials and is added as a fourth section. Furthermore, for a
Us> of Figures and Tables in the front of the volume. number of materials for which there exists only a
Totally, this volume reports 4627 sets of data on 812 small amount of data, the original data plot may be
materials, which are listed in the Material Index at omitted.
the end of the volume. The Material Index lists also The Original Data Plot is a full-page log-log-
the materials contained in the companion volumes scale graphical presentation of the original thermal
(Volumes I and 3) on thermal conductivity. conductivity data as a function of temperature.
The ranges of temperatures covered by the When several sets of data are coincident, some of the
thermal conductivity data for some materials are data sets may be omitted from the plot for the sake
from near absolute zero to past the melting point, of clarity. They are, however, invariably reported in
though, for most high-temperature materials, the the Data Tabk and Specification Table.
available data are limited to the solid range. The Specification Table provides in a concise
The data for the elements and a number of form the comprehensive information on the test
oxides have been critically evaluated, analyzed, and specimens for which the data are reported. The
synthesized, and recommended reference values arc curve numbers in the Specification Table correspond
presented. This procedure involves critical evaluation exactly to the numbers which also appear in the
of the validity of available data and related informa- Original Data Plot and in the Data Table. The
tion, resolution and reconciliation of disagreements Specification Table gives for each set of data the
of conflicting data, correlation of data in terms of reference number which corresponds to the number
various affectinj; parameters, and comparison of the in the list of References to Data Sources, the year of
resulting values with theoretical predictions, or with publication of the original data, the method of
i
42a Numerical Data
measurement, the temperature range, the reported identify the materials for which their data are re-
estimate of error of the data, the specimen designa- ported. This is particularly true for the authors of
tion, and the specimen characterization and test earlier investigations. Consequently, the amount of
conditions. The information of the last category, information on specimen characterization reported
which is reported to the extent provided in the in the Specification Tables varies greatly from
original source document, includes the following: specimen to specimen.
In the Data Table, tabular presentation is given
(1) Purity, chemical composition;
for all the data described in the Specification Table
(2) Type of crystal, crystal axis orientation,
and shown or not shown in the Original Data Plot.
typo and concentration of crystal defects;
Many tabular data which are not presented in the
(3) Microstructure. grain size, pore size and
original source documents are obtained directly
shape, inhomogeneity. additional phases;
from the authors through private communications.
(4) Specimen shape and dimensions, method
Attempts have often been made to contact the authors
and procedure of fabrication;
of recent publications for tabular data whenever the
(5) Thermal history, heat treatment, mechan-
original data are given in the research paper only in
ical, inadiative. and other treatments;
a figure too small to warrant accurate data extraction
(6) Manufacturer and supplier, stock number,
compatible with the reported accuracy of the
and catalog number;
measurement. The thermal conductivity data are
(7) Test environment, degree of vacuum or
given in watts per centimeter per degree Kelvin, and
pressure, heat flow direction, strength and
the temperatures in degrees Kelvin. For data con-
orientation of the applied magnetic tield;
version, the reader is referred to the Conversion
(8) Pertinent physical properties, such as _ , T-I , ^ J , ,
. . hi tnn*^i*ntkmrrAMtstFactors for Thermal Conductivity Units given later.
,a
* lt'fiwi'ty w ** The recommended thermal conductivity values
(9) Reference materiallAToryv tor a 'comparative . . , L . . . ,
for a material are reported in a separate graph and
method of measurement;
table following the Data Table. The estimated
(10) Form in which the extracted data arc
accuracy of the recommended values and special
presented in the original source document
remarks on material characterization and identifi-
other than raw data points;
cation are also noted in the table.
(11) Additional information obtained directly
from the author.
3. CLASSIFICATION OF MATERIALS
Unfortunately, in the majority of cases the authors
do not report in their research papers all the necessary The classification scheme as shown in the table
pertinent information to fully characterize and for nonmetallic elements, compounds, and mixtures
( lassitication of Materials
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103. *rM,-4-^, vtK xRrfitut. Ttw r\e Uw.V., po^t 0v SAEC
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