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APPENDIX I A- 1 Ultra-Low Percolation Thresholds in Ternary Co- Continuous Polymer Blends Jianhong Zhang, Sepehr Ravati, Nick Virgilio, and Basil D. Favis ∗ CREPEC, Department of Chemical Engineering, École Polytechnique de Montréal, Montréal, Québec, H3C 3A7 Canada Published in Macromolecules in December 2007 A-1.1. Introduction. In binary immiscible polymer blends, as the concentration of the minor component increases, the structure percolates and its continuity also increases (Potschke & Paul, 2003; Reignier & Favis, 2000). At higher concentrations, closely associated with the region of phase inversion, a co-continuous morphology is obtained and is characterized by two fully continuous phases. By selectively controlling the interface, composition, processing temperature, shear rate and annealing time of the blends, it is possible to control the pore size of the cocontinuous network over 2-3 orders of magnitude (Yuan & Favis, 2004, 2006). Co-continuous polymer blends have the potential of opening particular application fields where the presence of interconnected structures are a necessary feature (as in separation phenomena, electrical conductivity, tissue engineering scaffolds and drug delivery devices). A significant body of ∗ Corresponding author. E-mail: basil.favis@polymtl.ca Tel: +1-(514)3404711 ext.4527. Fax: +1-(514)3404159 234
literature has examined factors influencing the percolation threshold in binary co-continuous polymer blends and also the width and concentration range of the region of dual-phase continuity (Yuan & Favis, 2004, 2006). Most studies on binary systems report percolation thresholds in a range of about 15-20% concentration of minor component. This significant amount of the second phase, necessary to obtain a co-continuous structure, considerably limits the range of possible applications. However, very few studies have examined the continuity phenomena in multiphase (more than two phases) systems. The possibility of dramatically decreasing the percolation threshold of one component in order to achieve co-continuity at concentration levels of a few percent would be an important achievement. A few studies have contributed towards attaining such a result. Jérôme and co-workers reported on the preparation of a co-continuous polymer blend with the addition of a solid filler showing a very low percolation threshold for the filler at about 0.2 volume percent. Interestingly, this filler was located at the interface in a chain-like structure shape (Gubbels, et al., 1994; Soares, et al., 1995). However, the limitation in that case is that the particle is not thermodynamically stable at the interface. It has a particular affinity for one of the phases and is simply transiting from one phase to the other. Jorgensen and Utracki report very low percolation thresholds for polyethylene in polystyrene binary blends of very high molecular weight (Lyngaae-Jorgensen & Utracki, 2003). In other studies, Narkis, Zilberman and coworkers (Narkis, et al., 2000a; Zilberman, Siegmann, & Narkis, 2000c) achieved multiple percolation by dispersing a third phase into one of the phases in a co-continuous binary blend. This ultimately creates a third percolated system, but the percolation thresholds are relatively high at 8-12% composition of this third phase. A potentially interesting way to achieve low percolation threshold materials is to combine a cocontinuous structure with a composite droplet type of morphology. The composite droplet morphology is a matrix/dispersed phase system in which the dispersed phase has a droplet-in droplet structure. Although little work has been published on polymeric versions of such systems, a number of key papers have appeared (Berger, Kammer, & Kummerlowe, 1984; Omonov, Harrats, & Groeninckx, 2005; Reignier & Favis, 2003a; Reignier, et al., 2003; Van Oene, 1972). The spreading coefficients (Torza & G. Mason, 1970) (Equation A-1.1) and variations on that concept have been successfully used (Hobbs, et al., 1988; Reignier & Favis, 2000; Valera, et al., 2006) to predict the thermodynamically stable preferential encapsulation of one polymeric phase by another. Encapsulation is governed by the various interfacial tension 235
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© Sepehr Ravati, 2010. UNIVERSITÉ
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DEDICATED To my parents iii
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RÉSUMÉ Cette thèse présente, po
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devenir une structure hiérarchique
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ABSTRACT This thesis presents, for
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system can be increased from 10 -15
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CONDENSÉ EN FRANÇAIS Dans ce trav
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deuxième coquille de PS. Les phase
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structures à percolation multiple
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autre sous-type de morphologie dans
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TABLE OF CONTENTS DEDICATION.......
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xxiii 2.4.1.1.1 Charged Polymer Ads
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5.3.4 Annealing Test ..............
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xxvii REFERENCES ..................
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LIST OF FIGURES xxix Figure 1-1. a)
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Figure 2-12. SEM photomicrograph of
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Figure 2-34. Schematic view of diff
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Figure 4-8. SEM micrographs of vari
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Figure 5-6. a),b) Scanning electron
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and c) triangular concentration dia
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n number of moles p concentration o
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AFM atomic force microscopy LIST OF
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PS-co-PMMA copolymer of PS and PMMA
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1.1 Introduction CHAPTER 1 - INTROD
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Figure 1-2. Human heart, longitudin
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One of the applications for porous
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On the other hand, a novel tri-cont
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2.1 Polymer Blends CHAPTER 2 - LITE
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Based on Sterling’s approximation
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Antonoff’s rule (Equation 2-13) i
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2.1.2.1 Binary Polymer Blends 2.1.2
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Some other studies(Everaert, Aerts,
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where the parameter z is dependent
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“compatibilization” was suggest
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a) λ BC A and B are matrices, b) C
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Reignier & Favis, 2000, 2003a; Reig
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measure the interfacial tension of
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a) b) Figure 2-6. Dependence of the
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Omonov et al. found double percolat
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2.1.2.2.3 Effect of Composition on
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a) b) C B A c) Figure 2-12. SEM pho
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In the case where PS is the matrix,
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Posthuma de Boer, 1999) (Kumin & Ch
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lattice, such as square lattice, wi
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magnetization, which is a function
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Polymers have long been thought of
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epoxy as a function of nanotube wei
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Figure 2-19. Approaching the percol
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Figure 2-21. Transmission electron
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Figure 2-22: Dependence of PE conti
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Figure 2-24. Plot of the total numb
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chain provides the conductive path
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2.3.1.2.1 Polyaniline One of the mo
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CoPA/LLDPE/PANI blend and a poor-qu
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Narkis and co-workers extended and
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Figure 2-31: Conductivity of PVDF/P
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organic thin films, a novel and str
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on the topic have been reported in
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succeeded in creating thin films wi
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Addition of salt to the solution of
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different from that of linear homop
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Figure 2-39. Macromolecule with a)
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polyanion such as hyaluronan (HA)(P
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2.4.1.1.7 Effect of Salt on Multila
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2.4.1.1.8 Overcompensation of the M
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important factors determining the g
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As shown in Figure 2-44, swelling a
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increasing the pH value due to a de
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CHAPTER 3 - ORGANIZATION OF THE ART
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discussed above, HDPE, PS, PMMA, an
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CHAPTER 4 - LOW PERCOLATION THRESHO
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or model which predicts where the p
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concentration threshold for the ons
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chemical and weathering resistance,
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Table 4-1. Material Characteristics
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filled with blend pellets. To facil
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4.3.6 Conductivity Measurements DC
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experimentally in this research gro
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a) b) c) d) Figure 4-4. Schematic i
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microstructure of the quaternary bl
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a) b) c) d) Figure 4-6. SEM microgr
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a) b) PVDF PS PMMA c) d) e) HDPE PS
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Uniform layers of PS and PMMA situa
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the concentration of HDPE is increa
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a) b) c) e) Figure 4-11. SEM microg
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melt-processable and contains 25 wt
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One question that should be address
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Conductivity(S/cm) Ternary Blend 1,
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phase(PMMA), the concentration of P
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(6) Virgilio, N.; Desjardins, P.; L
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ONION MORPHOLOGY HDPE PVDF PS Contr
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work described above has focused on
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thermodynamic explanation to predic
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four-point probe increases continuo
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in the rheology tests were compress
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5.3.6 Layer-by-Layer Deposition The
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prepare a polymer blend structure w
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a) b) c) Figure 5-3. Scanning elect
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spontaneously self-assembled. After
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a) b) c) d) e) f) g) h) Figure 5-5.
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Since the ultra-low surface area va
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c) a) b) Figure 5-6. a),b) Scanning
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salt to a PSS polyelectrolyte solut
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A relationship between macropore si
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close together. It is interesting t
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Figure 5-9. Mass increase (%) indic
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In this work the conductance of the
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deposited PANI layers increases unt
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(52) Guo, H. F.; Packirisamy, S.; G
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6.2 Introduction It is well-known t
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modified version of Harkins theory(
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6.3 Experimental 6.3.1 Materials Co
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Complex voscosity (Pa.s) 1,0E+04 1,
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6.3.5.2 Focused Ion Beam (FIB) and
Page 229 and 230: a) c) b) d) e) f) PMMA PMMA HDPE HD
Page 231 and 232: y Harkins theory, PS will always si
Page 233 and 234: a) b) c) d) e) f) PS Figure 6-6. a)
Page 235 and 236: a) b) HDPE : black PS : grey PMMA :
Page 237 and 238: 6.4.6 Continuity, Co-continuity, an
Page 239 and 240: c) V III II I VII I IV VI Figure 6-
Page 241 and 242: Continuity Scheme (a) Figure 6-10.
Page 243 and 244: Addition of a low concentration of
Page 245 and 246: Addition of small amounts of HDPE t
Page 247 and 248: icontinuous network with the HDPE.
Page 249 and 250: Three examples are shown in Figure
Page 251 and 252: (9) Mekhilef, N.; Verhoogt, H. Poly
Page 253 and 254: structures are formed due to the co
Page 255 and 256: CONCLUSION AND RECOMMENDATIONS In t
Page 257 and 258: REFERENCES A. K. Gupta, K. R. S. (1
Page 259 and 260: Caruso, F. (2003). Hollow Inorganic
Page 261 and 262: Domenech, S. C., Bortoluzzi, J. H.,
Page 263 and 264: Geuskens, G., Gielens, J. L., Geshe
Page 265 and 266: Hou, S., Harrell, C. C., Trofin, L.
Page 267 and 268: Krass, H., Papastavrou, G., & Kurth
Page 269 and 270: Macdiarmid, A. G., Jin-Chih, C., Ha
Page 271 and 272: Niziol, J., & Laska, J. (1999). Con
Page 273 and 274: Reghu, M., Yoon, C. O., Yang, C. Y.
Page 275 and 276: Shirakawa, H., Louis, E. L., MacDia
Page 277 and 278: Utracki, L. A. (1991). On the visco
Page 279: Yasuda, K., Armstrong, R., & Cohen,
Page 283 and 284: (Reignier & Favis, 2000, 2003a; Rei
Page 285 and 286: Table A-1.2. Interfacial tensions a
Page 287 and 288: acquisition of images with a very h
Page 289 and 290: Table A-1.3. Continuity of the PMMA
Page 291 and 292: (17) Reignier, J.; Favis, B. D., Ma
Page 293 and 294: PANI. Theoretically, the extent of
Page 295 and 296: Equation A-2.7 0( ) 0 1. 5 σ = σ
Page 297 and 298: Cumulative Mass × 10 5 (g) dipping
Page 299 and 300: of PANI, and an increase in the con
Page 301 and 302: Resistance(ohm) 1.0E+12 1.0E+11 1.0
Page 303 and 304: esistance value. Samples containing
Page 305 and 306: The results of resistance for PS/PE
Page 307 and 308: Caruso, F., & Schuler, C. (2000). E
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