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Table of contents
General introduction and motivation of the project
Chapter 1: From the physics of polymer to reinforced elastomers
Introduction
1. Introduction to polymer network physics
1.1. The isolated polymer chain
1.2. Rubber elasticity
1.3. The importance of entanglements
1.4. End of the Gaussian regime
2. Macroscopic failure
2.1. LEFM
2.2. Greensmith approximation
2.3. Lake and Thomas model
3. How to reinforce elastomers?
3.1. General guidelines
3.2. Delay nucleation
3.3. Slow down propagation
3.4. The specifications of elastomers
3.4.1. Viscoelasticity
3.4.2. Fillers
3.4.3. Physical bonds
3.5. Multiple networks
3.5.1. Double network hydrogels
3.5.2. Models for the fracture mechanics of double network hydrogels
3.5.3. Multiple network elastomers
Conclusions
References
Chapter 2: Nanocomposite elastomers filled with soft interpenetrable particles
Introduction
1. Results
1.1. Synthesis and characterization of the materials
1.1.1. Particles synthesis
1.1.2. Dispersion and swelling of the particles in ethyl acrylate
1.1.3. Synthesis of a simple matrix as a reference
1.1.4. Synthesis of the nanocomposites
1.2. Mechanical properties of the nanocomposites
1.2.1. Effect of the volume fraction of filler
1.2.2. Effect of the degree of crosslinking of the filler particles
Conclusion
2. Experimental part
2.1. Chemicals
2.2. Synthesis conditions
2.2.1. Soft “Filler Particles” by emulsion polymerization
2.2.2. “Reference matrix” by bulk polymerization
2.2.3. Preparation of the nanocomposite
2.3. Characterization methods
2.3.1. Gravimetric analysis
2.3.2. DLS
2.3.3. DSC
2.3.4. Mechanical tests
References
Chapter 3: Aqueous route to double network particles and characterization of the films therefrom
Introduction
1. Results
1.1. Synthesis
1.1.1. Synthesis of the “Single latex” (S) by emulsion polymerization
1.1.2. Swelling of the latex particles in aqueous dispersion by EA
1.1.3. Synthesis of the “Double latex” (D) by seeded emulsion polymerization
1.2. Film formation and characterization
1.2.1. Temperature effect on film formation
1.2.2. Comparison of D latex with the corresponding constituting single networks
1.2.3. Effect of the crosslinking density in the S seeds on S and D films
1.3. Connecting particles
1.3.1. Presentation of the DAAm/ADH system
1.3.2. Effect of DAAm on S film
1.3.3. Connecting the particles through the 2nd network
Conclusion
2. Experimental part
2.1. Synthesis
2.1.1. Chemicals and reagents
2.1.2. Synthesis of the “Single latex” (S) by emulsion polymerization
2.1.3. Synthesis of the “Double latex” (D) by seeded emulsion polymerization
2.1.4. Drying process
2.2. Characterization methods
2.2.1. Gravimetric analysis
2.2.2. DLS
2.2.3. AFM
2.2.4. CryoTEM
2.2.5. Mechanical tests
Appendix
References
Chapter 4: Imaging and quantification of bond breakage in elastomers using confocal microscopy
Introduction
1. Sample synthesis
1.1. Single network
1.2. Multiple network
1.3. Mechanofluorescent single network
2. Mechanical test
3. Imaging and quantification of bond breakage
3.1. Confocal set-up
3.2. Image collection
3.3. Imaging analysis
3.3.1. Calibration of fluorescence
3.3.2. Quantification
4. Representativity of the mechanophore’s activation for chain breakage
5. Dependence of DACL activation’s on strain rate and temperature
Conclusions
References
Chapter 5: Soft network fracture mechanics study using mechano-fluorescence
Introduction
1. Fracture of notched samples
1.1. Crack propagation
1.1.1. Video analysis
1.1.2. Effect of notch length
1.2. Quantification of chain scission on fracture surfaces
1.3. Discussion
2. Fracture of unnotched samples
2.1. Mechanical reproducibility
2.2. Direct observation
2.3. Effect of the viscoelasticity
Conclusion
Appendix
References
Chapter 6: Effect of soft networks structures on fracture studied with mechano-fluorescence
Introduction
1. Experimental methods
1.1. Materials
1.2. Mechanical characterization
2. Results and discussion
2.1. Mechanical properties
2.2. Damage quantification
Conclusion
Appendix
References
Chapter 7: Quantitative study of molecular bond breakage and load transfer during the necking of multiple network elastomer
Introduction
1. Materials and methods
1.1. Chemicals and reagents
1.2. Single network synthesis
1.3. Multiple network synthesis
1.4. Mechano-fluorescent network synthesis
1.4.1. DACL incorporation
1.4.2. SP incorporation
2. Confocal imaging of stretched samples
2.1. Home-made tensile test set up
2.2. Confocal imaging
2.3. Systematic image analysis
3. Necking in multiple networks
3.1. Mechanical characteristics of necking
3.2. Damage quantification bulk vs neck regions (in the bulk and the matrix)
3.3. Load transfer between the filler and the bulk (SP in the matrix)
4. What parameters control the necking process?
4.1. Effects of the pre-stretch
4.2. Effects of the filler network crosslinking content
5. Effect of the connectivity between filler and matrix networks
5.1. SNHMA synthesis
5.2. Necking in HMA multiple networks
6. Discussion
Conclusion
Appendix
References
General conclusion
