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Table of contents
Chapter 1 –Physics of polymer networks and networks design
Introduction
1- General concepts on rubber elasticity
1-1- Ideal chain model
1-2- Entropy and free energy of an ideal chain
1-3- Polymer networks
1-3-1- Affine network model
1-4- Crosslinks and entanglements
1-4-1- At small strain
1-4-2- At intermediate strain
Mooney-Rivlin model
Rubinstein and Panyukov model
1-5- High strain region
2- Fracture mechanics of rubbers
2-1- Model of Lake and Thomas
2-2- Experimental evaluation of the fracture toughness
3- Network design
3-1- Bimodal networks
3-2- Interpenetrated networks
3-2-1- Double networks hydrogels
Synthesis and structure
Mechanical properties and toughening mechanism
Model for the fracture of DN hydrogels
Recent developments on DN gel structure
3-2-2- Interpenetrated elastomers
3-3- Introduction of prestretched chains in a polymer network
Conclusions and objectives of the manuscript
References
Chapter 2 – Introduction of isotropically stretched chains in a polymer network
Introduction
1- Synthesis
1-1- Chemicals
1-2- Polymerization Conditions and Environment
1-3- General path to multiple networks elastomers
1-3-1- First polymerization (Simple networks)
Samples compositions
Solvent for deswelling
Shrinking and digitations
1-3-2- Second polymerization (Double networks)
Samples compositions
1-3-3- Third polymerization (Triple networks)
1-4- Variations on the second network
1-5- Solvent free simple networks
1-5-1- Second/Third Network alone
1-5-2- Simple networks of EA
2- Extractable and conversion
2-1- First networks
2-2- Bulk samples
3- Structural properties by thermomechanical analysis
3-1- Theoretical background on DMA
3-2- Results and discussion
3-2-1- Simple networks
3-2-2- Multiple networks with a single monomer type
3-2-3- Multiple networks with a contrast in monomer
Miscible Multiple networks
Immiscible Multiple networks
Conclusions
References
Chapter 3 – Mechanical signature of isotropically prestretched chains: a macroscopic investigation
1- Material and methods
1-1- Mechanical testing experiments
1-2- Tensile tests
1-3- Step-Cycle extension
1-4- Fracture in single edge notch test
2- Simple networks alone: weak elastomers
2-1- Effect of the crosslinker concentration in simple networks
2-2- First network: brittle and tunable
Crosslinker concentration
Nature of the monomer
2-3- Fracture properties of simple networks
3- Multiple networks: stretching the prestretched
3-1- General behavior
3-2- Origin of the initial modulus
3-3- The origin of stiffening and softening
3-4- Less extensible second network
4- Variations of monomers
4-1- Changes in the second network
4-2- Changes in the composition of the first network
5- Cyclic extension: from pure elasticity to bulk dissipation
5-1- Viscoelastic behavior in second networks alone
5-2- Perfect reversibility of the elasticity in double networks
5-3- Mullins effect in Triple networks
5-4- Energy dissipation and bond breaking mechanism
6- Fracture properties
6-1- Experimental results and discussion
6-2- Models
Lake and Thomas
Brown and Tanaka models for DN hydrogels
Conclusion
References
Chapter 4 – A molecular insight in prestreched chains conformation
Introduction
1- Small Angle Neutron Scattering to probe polymeric chains conformations.
1-1- Generalities
1-2- Scattering from polymer melts
1-3- Scattering and anisotropy
1-4- Experimental setup
1-5- Data treatment
2- Labeled multiple networks elastomers: from monomer synthesis to mechanical properties
2-1- Synthesis of deuterated monomers
2-1-1- Procedure
2-1-2- Analysis
2-2- Labeled multiple networks
2-3- Check of the mechanical properties
3- Chains of the first network: undeformed samples
3-1- Partially deuterated multiple networks of pure poly(ethyl acrylate)
3-2- Comparison between EA and MA as second/third monomers
4- Stretching the prestretched chains
4-1- Scattering pattern of stretched multiple networks
4-2- Scattering along the principal directions
4-2-1- In double networks
4-2-2- In triple networks
4-2-3- Sacrificial bonds and scattering
Summary of SANS results
References
Chapter 5 – Molecular toughening mechanism, mechanoluminescence as a probe for bond breaking
Introduction
1- Colors and light in polymers under stress
2- Mechanoluminescent crosslinker in multiple network elastomers
2-1- Mechanoluminescent crosslinker
2-2- Synthesis of dyed networks
2-3- Comments
Self polymerization
Successful incorporation in networks
3- Dioxetane as a probe of a bond breaking mechanism
3-1- Experimental conditions and data treatment
3-2- Results
3-2-1- Mechanical properties
3-2-2- Luminescence signal
3-3- Luminescence and mechanical properties
3-4- Stress or Strain sensor?
4- Fracture and luminescence
4-1- Experimental conditions and data treatment
4-1-1- Mechanical part of the experiment
4-1-2- Optical part of the experiment
4-2- Results
4-2-1- Fracture toughness
4-2-2- Before crack propagation
4-2-3- Crack propagation
Simple network EA0.5m
Double and Triple networks
Quantitative analysis
Crack velocity
4-3- Molecular description of the dissipation mechanism
Conclusion
References
Chapter 6 – From heterogeneous to Homogeneous first network .
Introduction
1- Homogeneous first network in multiple networks elastomers
1-1- Chain synthesis by Atom Transfer Radical Polymerization
1-1-1- ATRP Principle
1-1-2- Initiator synthesis
Protocol
1-1-3- Polymerization conditions
Protocol
1-2- End functionalization
Protocol
1-3- Perfect first network
Protocol
1-4- Synthesis of DN and TN
1-5- Comments on other methods to end-functionalize the chains
Atom Transfer Radical Coupling
Click chemistry: alkyne /azide reaction
2- Properties of ‘perfect’ multiple networks
2-1- Not so ‘Perfect’ first network
2-2- ‘Perfect’ multiple networks under deformation
2-1- Fracture of ‘perfect’ multiple networks
Conclusion
References
