Proceedings of the International Forum on Structural Ceramics Joining: Ceramic Engineering and Science Proceedings, Volume 10, Issue 11/12

453 Pages·1989·9.64 MB·English

Proceedings of the
International Forum on
Structural Ceramics Joining
Symposium Chairs:
Ronald E. Loehman, Sandia National Laboratories
Sylvia M. Johnson, SRI International
Arthur J. Moorhead. Oak Ridge National Laboratory
A Collection of Papers Presented at the
International Forum on Structural Ceramics Joining
Sponsored by the
Engineering Ceramics Division
The American Ceramic Society, Inc.
April 26-30, 1987
Pittsburgh, PA
ISSN 0196-6219
Published by
The American Ceramic Society, Inc.
757 Brooksedge Plaza Drive
Westerville, OH 43081-6136
Copyright@ 1989, The American Ceramic Society, Inc.
Erectrtive Director & Ptthlislier Editor
W. Paul Holbrook John B. Wachtman
Director of Publications Pmdticlion Mnmger
Linda S. Lakemacher Alan Hirtle
Committee on Ptrhlicntionc David W. Johnson, Jr., chair; Ronald E. Loehman;
Richard E. Tressler; Robert J. Eagan, ex officio;W . Paul Holbrook, ex oficio;
Waltraud M. Kriven, a oficio; John B. Wachtman, ex oficio.
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CESPDK Vol. 10, NO. 11-12, pp. 1503-1950, 1989
The American Ceramic Society assumes no responsibility for the statements
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Each issue of Ceramic Engineering and Science Proceedings includes a collection of
technical articles in a general area of interest, such a~ glass, engineering ceramics, and
refractories. These articles are of practical value for the ceramic industries. The
issues are based on the proceedings of a conference. Both The American Ceramic
Society, Inc., and non-Society conferences provide there technical articles. Each issue
is organized by an editor who selects and edits material from the conference. Some
issues may not be complete representations of the conference proceedings. There is
no other review prior to publication.
I 1
Preface
Although joining methods for structural ceramics have been investigated since
the early development of advanced ceramics, it is only in the last few years
that the importance of joining to the practical success of these materials has
been recognized. Reliable joining methods are not only critical for compo-
nent and system assembly, but they are also required for repair technology.
The heightened awareness of joining as an integral part of the fabrication pro-
cess for advanced ceramics is reflected in its present increased level of research
and development activity.
Against this backdrop, the Engineering Ceramics Division of the American
Ceramic Society sponsored a two day International Forum on Structural Ce-
ramics Joining at its 89th Annual Meeting in Pittsburgh, PA, April 28-29,
1987. The Forum featured forty-two oral presentations by scientists and en-
gineers throughout the world. In fact, more than one third of the speakers
were from outside the United States emphasizing the truly international scope
of ceramic joining work. Bringing together such a distinguished group of
researchers on ceramic joining provided a valuable forum at which the state
of the art and its future directions could be discussed.
This issue comprises the papers that were submitted for publication by the
Forum paticipants and which were then peer-reviewed according to the nor-
mal procedures of the American Ceramic Society. We have arranged the
proceedings into four sections to present a logical progression of topics. Thus,
the papers in the first section deal with fundamental studies of interfaces and
with investigations of model ceramic-metal systems, as exemplified by the pa-
per on Pd/A120, interfaces by Eastman and Ruhle. The second section con-
tains the papers concerned with interfacial reactions between brazing filer metal
alloys and structural ceramics such as Si,N,, SIC, and Zr02. The common
thread that ties together most of those papers is their focus on the high tem-
perature chemistry of interfacial reactions relevant to joining. The third sec-
tion groups the papers that report development of practical joining methods
for structural ceramics. The last section of the book contains the papers deal-
ing primarily with strength, mechanical properties, and durability of struc-
tural ceramic joints. The results of those papers have a common dependence
on studies such as those presented in the first three sections; that is, in order
to make strong, reliable joints with any degree of control, one must under-
stand the structure and chemistry of the interface. Thus, this book forms a
more coherent whole than one ordinarily finds in a volume assembled from
a collection of presentations at a scientific meeting.
We appreciate the efforts of the speakers and their co-authors for their
presentations at the Forum, and, particularly, for providing the manuscripts
that made this volume possible. We also wish to acknowledge the organiza-
tional and editorial support of the staff of the American Ceramic Society in
the production of this volume.
Ronald E. Loehman
Sylvia M. Johnson
Arthur J. Moorhead
Table of Contents
Model Systems
Ultrahigh Vacuum Diffusion Banding of Metals to
.....................................
Ceramics 1503
B. Gibbesch, G. Elssner, W. Mader, and H. Fischmeister
................
TEM Studies of Pd/A1a3 Interfaces 15 15
J. A. Eastman and M. Riihle
........
Spinel Formation in the Nickel-Alumina System 1531
H.S. Betrabet, S.N.S. Reddy, S. Purushothaman, and I. Reimanis
........
Crystallographic Study of Ceramic-Metal Joints 1541
Shotaro Morozumi and Michio Kikuchi
Material Transport Mechanisms During the
..............
Diffusion Bonding of Niobium to A1203 1549
K. Burger and M. Rahle
............
Intrusion Bonding of Nickel and Zirconia 1567
I. E. Reimanis, S. L. Shinde, and L. C. DeJonghe
................
Alumina-Copper Diffusion Bonding 1575
R. M. Crispin and M. G. Nicholas
Bonding and Fracture of Titanium-Containing Braze
...........................
Alloys to Aluminum 1582
Roger T. Cassidy, Russell E. Pence, William E. Moddeman,
and Anthony D. Buonaquisti
Interfacial Reactions
......
Brazing Ceramics with Alloys Containing Titanium 1602
M. G. Nicholas and R. M. Crispin
........
Brazing Alloy Design for Metal/Ceramic Joints 1613
Rakesh R. Kapoor and Thomas W. Eagar
........................
Joining Nitride Ceramics 1631
A. P. Tomsia, J. A. Pask, and R. E. Loehnian
Wetting of Silicon Nitride with Selected Metals and
.....................................
Alloys 1655
Lennart Ljungberg and Richard Warren
An Investigation of Interfacial Microstructure and
Bonding in Brazed Silicon Nitride-Silicon Nitride
........
and Silicon Nitride-Ne-Cr-Fe Alloy 600 Joints 1667
S. C. Hsu, E. M. Dunn, K. Ostreicher, and T. Emma
..........
Interfacial Reactions in Metal-Sia, Bonding 1685
R. K. Brow and I<, E. Loehman
Interface Mixing Between Metals and Ceramics:
.......
Classification, Thermochemistry, and Processing 1696
S. N. S. Reddy, H. S. Betrabet, S. P. Purushothaman, and
C. Narayan
Morphological Development of Zirconia-Metal
...................................
Interface 1708
B. S. Chiou, Y. C. Wu, and J. G. Duh
Interfacial Reaction Between Zirconia and Carbon
......................................
Steel 1722
Nobuya Iwamoto, Yukio Makino, and I-Iajime Yokoo
Wetting of Silicon Carbide Surfaces by
....................
Mg0-Li@-AI@,-SiO2 Glasses 1735
Dennis N. Coon and Robert M. Neilson, Jr.
Joining Methods
.......
Joining Between Zirconias Using Platinum Metal 1745
Nobuya Iwamoto, Yukio Makino, and Tokio Sera
Joining Silicon Carbide Using Nickel- Active Metal
....................
(or Hydride) Powder Mixtures 1761
Nobuya Iwamoto, Yukio Makino, and Hiroshi Miyata
Silicon Nitride Joining with Glasses in the System
..................................
CaO-SiO, 1768
Yukio Haibara, Norimasa Unicsaki, and Nobuya Iwamoto
Strength and Fracture
........
The Strength of Ceramics Bonded With Metals 1786
B. J. Dalgleish, M. C. Lu, and A. G. Evans
..........
Modeling of Ceramic to Metal Brazed Joints 1801
Pierre 0. Charreyron, Donald 0. Patten, Jr. and Bradley J. Miller
Boundary Effects on the Interfacial Transient
.........
Thermal Fracture of Ceramic-To-Metal Bonds 1825
Klod Kokini
.........
Mechanical Behavior of Brazed Silicon Nitride 1846
Sylvia M. Johnson
Comparison of Strengths of Active Metal
Brazements in Alumina and SIC Whisker-
...........................
Reinforced Alumina 1853
A J. Moorhead and Hyoun-Ee Kim
.....
Mechanical Behavior of Ceramic-Metal Braze Joints 1866
Donald 0. Patten, Maurice L. Torti, and Pierre 0. Charreyron
.........
Ultrasonic Characterization of Ceramic Joints 1879
W. A. Simpson, Jr. and R. W. McClung
Strength of Silicon Nitride-Silicon Nitride Joints
....................
Bonded With Oxynitride Glass 1893
Robert M. Neilson, Jr. and Dennis N. Coon
Effect of Testing Atmosphere on Mechanical
.................
Properties of Ceramic/Metal Joints 1908
K Suganuma, M. Morita, T. Okamoto, and M. Koizumi
Effect of Surface Grinding Conditions on Strength
.......................
of Alumina/Niobium Joint 1919
K. Suganuma, T. Okamoto, M. Koizumi, and S. Gohda
................................
Author Index 1935
...............................
Subject Index 1943
Ceramic Engineering and Science Proceedings
Ronald E. Loehman, Sylvia M. Johnson, Arthur J. Moorhead
copyright 0 1989, The American Ceramic Society, Inc.
Ceram. Eng. Sci. Proc. 10[11-121 pp. 1503-1514 (1989)
Ultrahigh Vacuum Diffusion Bonding of Metals to
Ceramics
B. GIBBESCHG,. ELSSNERW, . MMER, AND H. FISCE~MEISTER
Max-Planck-Institut fur Metallforschung
Institut fur Werkstoffwissenschaften
Seestrasse 92
7000 Stuttgart 1
Federal Republic of Germany
A UHV apparatusf or solid-state bonding of ceramic and metal single crystal and
polycrystaUine materials is described. The apparatus is especiauy designed for the
production of clean integaces in bicrystal joints between crystabgraphically
preoriented fit crystal plutelets. Sandwich-like pieces of 35 mm maximum height
and a welded surface area of 10 mm x 15 mm can be manufactured in the
apparatus which is subdivided into a cleaning chamber, a parking station, and a
welding unit. The maximum welding temperature is 1800°C. Information is given
on the preparation of single crystals for diflusion bonding. First experiments in
the UHV bonding of polycrystalline Nb to polycrystalline alumina are described.
Introduction
The development of high performance structural ceramics together
with considerable advances in the application of bonded ceramic-metal
components in the areas of high temperature technology, energy
conversion, automotive engines, microelectronics, and biomedical
implants have intensified fundamental and applied research on the
nature of metal-ceramic interface and their influence on the properties
of the composite system.
Among the various techniques available for fabricating joints,' high
vacuum diffusion bonding is especially suited for studies of the
structure and chemistry of metal ceramic interfaces and their interrela-
tion to the properties of the interface region and the joint. Sandwich-
like specimens of the configuration ceramic-metal-ceramic offer the
possibility to investigate in a rather simple manner transport pheno-
mena at and across interfaces, interfacial and bulk chemical reactions,
dimensional changes and the development of defects in the interface
regions of single crystals or polycrystalline materials and their depen-
dence on parameters such as bonding temperature, time, mechanical
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pressure, vacuum pressure, surface roughness, and specimen dimen-
sions. Moreover, specimens cut from diffusion bonded pieces can be
thinned to TEM foils for examination by conventional, STEM, and
HREM technique^.^-^ Likewise, bend test specimens can be manufac-
tured to determine mechanical properties of the joint such as bond
strength, fracture resistance, and interface fracture energy.’-’
A considerable drawback of conventional diffusion bonding is the
restriction to a high vacuum of the order of 10” mbar. Bonding
behavior and interface chemistry depend critically on the cleanliness of
the surfaces to be bonded and hence both on the surface cleaning
procedures and the vacuum pressure prior to and during the bonding
process as shown, e.g., by experiments of Pepper on the strength of
metal-sapphire interfaces.’
In the last decade, ultrahigh vacuum techniques have been
developed to produce clean interfaces in artificially bonded bicrystals
manufactured from two separate crystals and to study the bonding
behavior of metal and metal-ceramic single crystal and polycrystalline
combinations. These experimental studies took advantage of ion sputter
techniques to clean the surfaces of ultrahigh vacuum conditions to
maintain their cleanliness. Ruge and co- constructed a UHV
apparatus to investigate solid-state bonding between polycrystalline
metals and of metal-to-ceramic combinations at room temperature.
The UHV chamber is equipped with a tension and compression device
of 1000 N maximum load in order to rupture and to reweld notched
specimens by solid-state bonding of their cleaved or fractured surfaces.
A residual gas analyzer was employed to determine the gaseous species
that are present. The attainable vacuum was 2 x mbar.” Milkove
and Sass” used a UHV apparatus for the preparation of thin metal
bicrystals containing clean grain boundaries. A specimen preparation
jig within the UHV chamber served to manufacture [OOI] metal twist
boundaries by epitaxial metal deposition onto two cleaved and
preoriented NaCI crystals and subsequent pressing of the coated crystals
films. A residual gas analyzer was employed to monitor the composi-
tion of the gaseous species during the different preparation stages.
Akaike and Funakubo” studied the cold pressure welding behavior of
A1/A1203a nd metallmetal combinations under UHV conditions. They
used spherical test specimens which were indented into a single crystal
metal plane. Prior to indentation, the specimens were cleaned by argon
ion bombardment. The apparatus was later designed to allow solid-
state welding of flat plate/plate configuration^.'^ UHV techniques and
ion beam cleaning procedures are also used in studies of the shear
strength’ and the adhesion, friction, and wear properties of sin le
crystal and polycrystalline ceramic/metal and metal/metal pairs.
1F-17
Prior to the friction experiments and after argon-ion bombardment, the
cleanliness of the surfaces of the flat ceramic specimen and of the pin-
like metal specimens is controlled by means of Auger electron spectro-
metry.
1504
The present paper reports on an ultrahigh vacuum apparatus
designed for the preparation of ceramic-metal bicrystals and polycrys-
talline ceramic-metal joints by diffusion bonding under well defined
conditions of cleanliness, interface crystal orientation, temperature,
time, vacuum, and mechanical loading. In this first report the UHV
apparatus and the specimen preparation procedure will be described.
Furthermore, some information is given on UHV diffusion bonding
experiments in which polycrystalline Nb platelets and alumina pieces
were manipulated and welded to test the functions of the new UHV
apparatus.
Ultrahigh Vacuum Apparatus
The apparatus for solid-state bonding of metals to ceramics is
subdivided into three parts (Fig. 1): the cleaning chamber, the parking
station, and the welding chamber. These units are so interconnected
that a transfer of the specimens via a linear motion transporter is
possible. The chambers are separated by gate valves and individually
evacuated to retard recontamination of the surfaces of the specimens.
The cleaning and the welding chamber are each mounted on a Leybold-
Heraeus vacuum system with a Ti sublimation pump of 1200 I/s
pumping speed, a turbomolecular pump of 345 I/s pumping speed, and
a rotary vane pump of 15.5 m3/h pumping speed. The vacuum of the
parking station is maintained by a sputter ion pump.
Cleaning Chamber
In order to obtain clean and precisely oriented interfaces the entire
manipulation of the metal and ceramic specimens which are to be solid-
state bonded is carried out under UHV conditions after the specimens
have been introduced into the chamber.
In the first series of experiments the specimens were positioned by
hand onto the parking carousel of the opened chamber. This procedure
will be replaced by an introduction of specimens from normal atmo-
sphere into the UHV chamber via a sample inlet system with a fast
entry and exit lock to enable a continuous operation of the welding
unit. After closing the chamber it was baked out at a temperature of
250°C for at least 12 h to achieve a vacuum pressure of 2 x mbar.
The chamber is equipped with a Leybold-Heraeus scanning ion gun
IQE 12/63, an LH Q 100 residual gas analyzer, which operates over a
mass range of 1-100 amu, and an ionization gauge for total vacuum
pressure measurements. An Auger spectrometer will be added to the
cleaning chamber in the near future.
The parking carousel of 160 mm diameter holds 16 sample holders.
By rotation and vertical shifting of the carousel the surfaces of the flat
specimens are adjusted to the appropriate working distances for argon-
ion sputtering or Auger analysis. The latter will be used for the
chemical characterization of the surfaces to be bonded. During the
1505
cleaning operation the ion beam scans the entire specimen surface of
dimensions 10 x 15 mm2. The ion energy can be varied from 500 eV to
5 keV. The working pressure during the sputter process is 5 x lo4
mbar. The cleaning of one surface takes about 30 min. If necessary,
the specimen can be turned through 360°C with a magnetic motion
lead-through to enable the cleaning of the opposite specimen surface.
A wobble stick equipped with a fork grip is used to lift and carry the
cleaned specimens to the linear motion sample transporter.
Parking Station
The linear sample transport unit consists of a carriage which is
guided by two cylindrical rails and moved by a bevel-gear drive which
can be actuated from the outside. To avoid recontamination during
subsequent cleaning operations the carriage is positioned together with
the specimen at the parking station which can be separated from the
adjacent chambers by gate valves. The parking station is only used to
store cleaned specimens prior to welding. Its vacuum pressure is
controlled by an ionization gauge. The carriage is large enough to
transport several cleaned specimens of 35 mm maximum length.
Welding Chamber
This part of the apparatus is designed for solid-state welding of
sandwich-like configurations of the three-layer sequence ceramic-
metal-ceramic or the five layer arrangement ceramic, metal, ceramic,
metal, ceramic. When single crystalline materials are to be welded the
latter configuration is preferred. An intermediate triple layer of single
crystal discs of approximately 1 mm thickness is enclosed by two
polycrystalline ceramic pieces of the dimensions 15 x 10 x 10 mm3.
The welding chamber is placed in a mechanical loading jig.
Alumina anvils are attached to the ends of the upper and lower steel
rods through which the bonding force can be applied to the specimen
configuration which is placed between the anvils. The leadthroughs of
the steel rods are sealed against the atmosphere by stainless steel bellows
which allow a total linear motion of 300 mm of the loaded specimens
between the anvils.
To enable the stacking of the cleaned specimens into the sandwich
configuration, the lower anvil is moved to a position in the lower part
of the welding chamber approximately opposite to the entrance port of
the linear motion transporter. The cleaned specimens are then carried
from the parking station to the entrance port of the welding chamber
and taken from the carriage to the lower anvil by means of a wobble
stick. Centering of the single specimens on the anvil is now achieved
by pushing the specimens by two opposite linear motion feedthroughs.
This simple arrangement will be replaced by a more sophisticated
placement and orientation device for single crystals by means of which
a stack of maximum five specimens can be centered and two of these
1506