Nano-engineering of composite material via reactive mechanical alloying/milling (RMA/M)

336 Pages·2017·4.46 MB·English

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Dissertations, Master's Theses and Master's Dissertations, Master's Theses and Master's
Reports - Open Reports
2014
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Edward Andrew Laitila
Michigan Technological University
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Copyright 2014 Edward Andrew Laitila
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Laitila, Edward Andrew, "Nano-engineering of composite material via reactive mechanical alloying/milling
(RMA/M)", Dissertation, Michigan Technological University, 2014.
https://doi.org/10.37099/mtu.dc.etds/949
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By

Edward Andrew Laitila

A DISSERTATION
Submitted in partial fulfillment of the requirements for the degree of
DOCTOR OF PHILOSOPHY
In Materials Science and Engineering
MICHIGAN TECHNOLOGICAL UNIVERSITY
2014

© 2014 Edward A. Laitila
This dissertation has been approved in partial fulfillment of the
requirements for the Degree of DOCTOR OF PHILOSOPHY in Materials
Science and Engineering.
Department of Materials Science and Engineering
Dissertation Advisor: Dr. Donald E. Mikkola
Committee Member: Dr. Stephen L. Kampe
Committee Member: Dr. Walter W. Milligan
Committee Member: Dr. Michael E. Mullins
Department Chair: Dr. Stephen L. Kampe
Dedication
“To my father, who passed away days after my defense, whom while not formally
educated was a very intelligent man, who taught me independence, showing me how hard
work pays off, and how to work with my hands……..thank you, for building the
foundation that lead me to a passion I enjoy, your quick wit, and critical thinking skills
rival anyone.”
“To a person in my life who I developed such a special relationship with, that
most never get to experience in their lifetime…this work is also dedicated to my
supervisor, my teacher, my colleague, my advisor, my mentor, and more importantly my
friend Dr. Donald E. Mikkola, who also taught me three very important words: think
about it!”
“Lastly and most importantly, I finally dedicate this work to my lovely wife,
whose compassion and understanding during this long ordeal, allowed me to complete
this work as a side part or our life…..without your love, support, and encouragement, this
would have never happened.”
Table of Contents
Approval Page .................................................................................................................... 2
Dedication........................................................................................................................... 3
List of Figures .................................................................................................................... 4
List of Tables .................................................................................................................... 11
Acknowledgements ........................................................................................................... 13
Abstract ............................................................................................................................. 14
I. Introduction ............................................................................................................. 15
A. Chromium-Modified Titanium Trialuminide................................................................... 16
B. Strengthening Mechanisms Investigated .......................................................................... 19
1. Grain Size Refinement ............................................................................................ 20
2. Dispersion Strengthening ........................................................................................ 23
C. Polycrystalline Materials .................................................................................................... 25
1. Grain Boundary Structure ....................................................................................... 26
2. Nanostructure Materials .......................................................................................... 30
3. Severe Deformation Processing .............................................................................. 34
D. Mechanical Alloying ............................................................................................................ 39
1. Reactive Mechanical Alloying/Milling (RMA/M) .................................................. 43
2. MA of Titanium-Aluminum .................................................................................... 44
3. Modeling of Mechanical Alloying .......................................................................... 46
E. Chromium-Modified Titanium Trialuminide Matrix Composites ................................. 52
F. Research Genesis ................................................................................................................. 53
II. Experimental............................................................................................................57
A. Experimental Procedure ..................................................................................................... 57
1. Production of Cubic Trialuminide Powder – Reading Alloy .................................. 57
2. Production of Cubic Trialuminide Powder - Master Alloy ..................................... 58
3. Milling Apparatus ................................................................................................... 59
4. Thermal Treatment of Powders ............................................................................... 59
5. Characterization ...................................................................................................... 61
6. Properties Explored ................................................................................................. 79
B. Reactive Mechanical Alloying/Milling (RMA/M) Processing Experiments ................... 82
1. Reactive Mechanical Milling (RMM) of Pre-Alloyed Powders with Fixed Excess
Titanium Addition in an Argon Atmosphere ........................................................................................... 83
4
2. Reactive Mechanical Alloying (RMA) of Elemental Powders with Excess Titanium
in an Argon Atmosphere .......................................................................................................................... 85
3. Reactive Mechanical Milling (RMM) of Pre-Alloyed Powders with Systematic
Increases in Excess Titanium and RMM Time in an Argon Atmosphere ............................................... 87
C. Consolidation of RMM and MM Powders by Cold Isostatic Press (CIP) and Hot
Isostatic Press (HIP) Processing ................................................................................................. 88
III. Experimental Results of the Powder Processing by Reactive Mechanical
Alloying/Milling................................................................................................................93
A. Reactive Mechanical Milling (RMM) of Pre-Alloyed Powders with Fixed Excess
Titanium RMMXh9TiAr Series ................................................................................................. 93
1. As-Milled Powders .................................................................................................. 93
2. X-ray Powder Diffraction Analysis of Annealed Powder ..................................... 113
3. X-ray Powder Diffraction Intensity Analysis ........................................................ 114
4. Macrostructure of Powders ................................................................................... 119
B. Reactive Mechanical Alloying (RMA) of RMA20h8.2TiAr Elemental Powders of
Al Cr Ti with Excess Titanium in an Argon Atmosphere .................................................. 133
66 9 25
1. X-ray Power Diffraction Phase Analysis of As-Milled and Annealed Powder ..... 133
2. Phase Volume Fractions ........................................................................................ 135
3. Lattice Parameters ................................................................................................. 137
4. Peak Broadening Analysis of Profile Fit X-ray Diffraction Peaks by the Warren-
Averbach Fourier Method...................................................................................................................... 139
C. Results from Reactive Mechanical Milling (RMM) of Pre-Alloyed Powders with
Systematic Increases in Excess Titanium in an Argon Atmosphere ..................................... 140
D. Results from Consolidated Materials .............................................................................. 141
1. Characterization .................................................................................................... 141
2. Properties of Consolidated Materials .................................................................... 170
IV. Discussion..............................................................................................................188
A. Nano-Scale Polycrystalline Materials Produced by Severe Deformation .................... 190
1. Structural Characterization of the Nanometer-Scale Powders Produced by the
RMA/M Process 191
2. Nano-Scale Grain Boundary Structure .................................................................. 217
B. The Reactive Mechanical Alloying/Milling Process ....................................................... 232
1. Mechanical Alloying Mechanisms ........................................................................ 235
2. Reaction Mechanisms ........................................................................................... 244
C. Nano-Engineering of Composite Materials or Nano-Engineering of Bulk Consolidated
Materials ..................................................................................................................................... 255
1. Nanocomposite Powders ....................................................................................... 257
2. Bulk Consolidated Materials ................................................................................. 259
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D. Consolidated Material....................................................................................................... 269
1. Microstructure ....................................................................................................... 270
2. Strengthening of these Nanocomposites ............................................................... 279
V. Conclusions............................................................................................................284
VI. Potential of this Processing Method ..................................................................... 287
VII. Future Work...........................................................................................................290
VIII. Appendix ................................................................................................................ 291
A. Standard Files .................................................................................................................... 291
1. L1 Chromium-Modified Titanium Trialuminide .................................................. 291
2
2. L1 Chromium-modified Titanium Trialuminide .................................................. 292
2
3. DO Al Ti – (Does not account for any Cr) ......................................................... 293
22 3
4. TiC ........................................................................................................................ 294
5. TiN ........................................................................................................................ 294
6. Ti(C, N) – 65 % C ................................................................................................. 295
7. Ti Al C ................................................................................................................. 296
4 2 2
8. Ti AlC .................................................................................................................. 297
3 2
9. TiH .................................................................................................................. 298
1.924
10. AlCr ..................................................................................................................... 298
2
11. Al O ..................................................................................................................... 299
2 3
B. Mechanical Milling to Produce Fine-Grain Single-Phase Chromium-modified
Titanium Trialuminide .............................................................................................................. 301
1. Single-phase Powder Metallurgy Al Cr Ti Alloy ............................................. 301
66 9 25
C. RMMXh9TiAr Annealed Powder XRD Analysis ........................................................... 304
1. Phase Volume Fractions ........................................................................................ 304
2. Lattice Parameter .................................................................................................. 306
D. Phase Analysis of Consolidated Material ........................................................................ 307
1. HIP Process RMM20h8.2TiAir800QH15m .......................................................... 307
2. HIP Process RMM20h8.2TiAr1000QH2h ............................................................ 308
3. HIP Process RMM20h9TiAr1000QH2h ............................................................... 309
4. Consolidated Materials from Systematic Increases in Excess Titanium and RMM
Time in an Argon Atmosphere High Carbide Content (Long RMM Time Processing in Argon) ......... 311
E. NGB Calculation for RMA Processing ............................................................................ 317
1. RMA20h8.2TiAr Elemental Starting Powder ....................................................... 317
F. Role of Grain Boundary Structure in Superplastic Deformation ................................. 320

IX. References .................................................................................................................326
6
List of Figures
Figure I-1 a) L1 Crystal Structure, b) L1 to DO Crystallographic Relationship, and c)
2 2 22
DO Crystal Structure ..................................................................................................... 16
22
Figure I-2 a) SPEX(cid:165) Mill b) Attritor Mill c) Ball Mill ..................................................... 41
Figure I-3 Fundamental Welding/Fracture Ball to Ball Collision Model [99] ................ 47
Figure I-4 XRD Pattern of Original Experiment After 90 h of SPEX(cid:165) Milling ................ 55
Figure I-5 XRD Patterns of the Original Experiment for 36 h to 90 h MA Times ............ 55
Figure I-6 Integrated Background Intensity Increase with MA Time ............................... 56
Figure II-1 Side-Drifted Powder Diffraction Sample Holder ........................................... 62
Figure II-2 Complex Pattern for 40 h RMM Time Sample RMM40h9TiAr ...................... 64
Figure II-3 Example of Profile Fitting of the RMM40h9TiAr Sample RMM Time 40 h... 66
Figure II-4 Comparison of Profile Fit and Raw Data for the Crystallite Size Fourier
Coefficients for Copper <100> ........................................................................................ 75
Figure III-1 XRD Pattern for Initial, 0.5 h, and 1 h RMM Processing Times
(RMM0h9TiAr, RMM0.5h9TiAr, RMM1h9TiAr) .............................................................. 94
Figure III-2 XRD Pattern for 5 h, 10 h, 15 h, 20 h, 25 h, 30 h, and 40 h RMM Times..... 95
Figure III-3 RMMXh9TiAr Series all RMM Samples ....................................................... 96
Figure III-4 XRD Phase ID RMM0h9TiAr Initial Mixture ............................................... 98
Figure III-5 XRD Phase ID RMM0.5h9TiAr RMM Time 0.5 h ........................................ 98
Figure III-6 XRD Phase ID RMM1h9TiAr RMM Time 1 h .............................................. 99
Figure III-7 XRD Phase ID RMM5h9TiAr RMM Time 5 h .............................................. 99
Figure III-8 XRD Phase ID RMM10h9TiAr RMM Time 10 h ........................................ 100
Figure III-9 XRD Phase ID RMM15h9TiAr RMM Time 15 h ........................................ 100
Figure III-10 XRD Phase ID RMM20h9TiAr RMM Time 20 h ...................................... 101
Figure III-11 XRD Phase ID RMM25h9TiAr RMM Time 25 h ...................................... 101
Figure III-12 XRD Phase ID RMM30h9TiAr RMM Time 30 h ...................................... 102
Figure III-13 XRD Phase ID RMM40h9TiAr RMM Time 40 h ...................................... 102
Figure III-14 Profile Fit of RMM20h9TiAr RMM Time 20 h ......................................... 103
Figure III-15 Volume Fraction for RMMXh9TiAr Series of RMM Times ...................... 105
Figure III-16 L1 Intermetallic Lattice Parameter ......................................................... 107
2
Figure III-17 RMMXh9TiAr Series Warren-Averbach Crystallite Size Analysis ........... 109
Figure III-18 RMMXh9TiAr Series Warren-Averbach Microstrain Analysis ................ 111
Figure III-19 X-ray Powder Diffraction Pattern Background Increase ......................... 115
7
Figure III-20 RMMXh9TiAr Series Background Intensity Area for As-Milled and
Annealed Samples for all RMM Times ............................................................................ 116
Figure III-21 Total Crystalline Diffracted Intensity for the RMMXh9TIAr Series As-
milled and Annealed Samples ......................................................................................... 118
Figure III-22 Particle Size Distribution of RMM0.5h9TiAr As-Milled Powder ............. 121
Figure III-23 Particle Size Distribution of RMM25h9TiAr As-Milled Powder .............. 122
Figure III-24 Particle Size Distribution of RMM40h9TiAr As-Milled Powder .............. 122
Figure III-25 Infant Aggolomerate Particle RMM10h9TiAr As-Milled 700X ................ 124
Figure III-26 As-Milled Powder Particle RMM0.5h9TiAr 2kX ...................................... 124
Figure III-27 As-Milled Individual Powder Particles for 10, 25, 40, and 60 h RMM Times
(the 10 and 25 h same excess titanium, 40 h 2X, 60 h 3X amount)................................. 125
Figure III-28 Particle Cavity in RMM1h9TiAr As-milled Powder Particle 13kX .......... 126
Figure III-29 Continued Cavity Closure in RMM25h9TiAr As-millled Powder Particle
8kX .................................................................................................................................. 126
Figure III-30 High Magnification Micrograph of Surface Features of As-milled
RMM10h9TiAr Powder Particle 15kX ............................................................................ 128
Figure III-31 Surface Smeared Particles Showing Flow Lines in As-milled
RMM10h9TiAr Powder Particle 19kX ............................................................................ 128
Figure III-32 Areas of Small Particle Cold Welding and Brittle Fracture Surfaces on As-
milled Particle RMM1h9TiAr 1.8kX ............................................................................... 130
Figure III-33 Crack and Fracture Surface on As-milled RMM0.5h9TiAr Powder Particle
6kX .................................................................................................................................. 131
Figure III-34 Cracks and Fractures As-milled Powder Particle of 40 h RMM Time with
16.8 wt. pct. Titanium 4.5kX ........................................................................................... 132
Figure III-35 Diffraction Pattern of RMA20h8.2TiAr As-Milled with Identified Phases134
Figure III-36 Diffraction Pattern of RMA20h8.2TiAr Vacuum Annealed with Identified
Phases ............................................................................................................................. 135
Figure III-37 Ternary Titanium Aluminum Chromium Phase Diagram Determined from
HIPed Materials at 1200 °C 172 MPa 2 h [16] ............................................................. 137
Figure III-38 As-Milled Systematic Increase in Excess Titanium and RMM Time ........ 140
Figure III-39 Carbon Content Dependence on RMM Time ........................................... 143
Figure III-40 Iron Content Dependence on RMM Time ................................................. 145
Figure III-41 Volume Fraction Dependence of L1 Intermetallic with RMM Time ....... 150
2
8
Figure III-42 Carbon Content Calculated from XRD Volume Fraction Analysis and
LECO Elemental Analysis............................................................................................... 152
Figure III-43 Crystallite Size Results from the Scherrer and Warren-Averbach Methods
as a Function of RMM Time ........................................................................................... 157
Figure III-44 Microstrain Data in the <111> Direction as a Function of RMM Time .. 158
Figure III-45 TEM Micrograph of Sample 20/1000/MA 50 kX Magnification .............. 159
Figure III-46 TEM Micrograph of Sample 40/1000/RA 60 kX Magnification ............... 160
Figure III-47 TEM Micrograph of Sample 40/1000/RA 80 kX Magnification ............... 161
Figure III-48 TEM Image of Carbide Edge for Sample 40/1000/RA 300 kX ................. 163
Figure III-49 FESEM Micrograph of Sample 20/1000/MA ............................................ 165
Figure III-50 FESEM Micrograph of Sample 20/1000/RA ............................................ 165
Figure III-51 FESEM Micrograph of Sample 40/1000/RA ............................................ 166
Figure III-52 FESEM Micrograph of Sample 60/1000/RA ............................................ 166
Figure III-53 Density of Alloys HIPed at 1000 ºC with Increasing Complex Carbide
Volume Fraction ............................................................................................................. 172
Figure III-54 Vickers Hardness as a Function of Carbon Content for Samples
Consolidated at 1000 (cid:113)C for 2 h ..................................................................................... 175
Figure III-55 Compression Curves for Cr9 and MM3h Samples ................................... 178
Figure III-56 Compression Curves for RMM Samples Consolidated at 1000ºC ............ 179
Figure III-57 Changes in Strain Hardening Rate as a Function of the Square Root of the
Dislocation Density ......................................................................................................... 181
Figure III-58 Engineering Stress-Strain Curve Sample 40/1000/RA at 900 (cid:113)C ............. 182
Figure III-59 Macro Photomicrograph of 900 ºC Compression Sample 20/1000/RA
(right) and a Untested Sample (left) with Loading Direction Vertical ........................... 183
Figure III-60 Young's and Shear Moduli Change with Carbon Content ........................ 185
Figure III-61 Poisson's Ratio Change with Carbon Content.......................................... 186
Figure III-62 CTE as a Function of Volume Fraction of Carbide and Therefore Carbon
Content ............................................................................................................................ 187
Figure IV-1Comparison of As-Milled Powder to Annealed As-Milled Powder ............. 192
Figure IV-2 Interference Functions W(r) for interatomic distances. (a) Long-range
ordered crystalline structure; (b) short-range ordered amorphous structure; (c) random
neither long-range nor short-range ordered structure [160]. ........................................ 194
Figure IV-3 Corrected Volume Fraction Data for RMMXh9TiAr As-Milled Powders .. 205
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