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Patrice Dole, INRA UMR FARE, patrice.dole@reimsra.fr

…what about lignins?. Patrice Dole, INRA UMR FARE, patrice.dole@reims.inra.fr. Lignins / material physicochemistry Overview of green materials Use of Lignin properties for green materials. O. O. O. O. O. O. Extracted lignin is a polymer ?. Lignins / material physicochemistry

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Patrice Dole, INRA UMR FARE, patrice.dole@reimsra.fr

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  1. …what about lignins? Patrice Dole, INRA UMR FARE, patrice.dole@reims.inra.fr

  2. Lignins / material physicochemistry Overview of green materials Use of Lignin properties for green materials

  3. O O O O O O

  4. Extracted lignin is a polymer ?

  5. Lignins / material physicochemistry Overview of green materials Use of Lignin properties for green materials

  6. Renewable ressources Natural polymers Lignocellulosic materials Bio rafinery monomers macromonomers Blends Composites Thermoplastics 3 D networks Fossil ressources Biodegradable plastics

  7. Renewable ressources Construction products Little markets Natural polymers Fibers Bio rafinery monomers macromonomers Blends Composites Automotive market Packaging Thermoplastics 3 D networks Fossil ressources Biodegradable plastics

  8. Lignins / material physicochemistry Overview of green materials Use of Lignin properties for green materials

  9. Cohesion is only due to strong interactions Bad cohesion Thermoplastic behaviour

  10. 100 barquette film PET PLA increasing low Mw plasticizer content H PS PHB PP Pro PLA MB MB PCL MB PLA PLA PHB Pro PBAT 10 H Pro Hemi Pro Pro H Stress (MPa) Starch 1 lignin Increasing Matrix Molecular weight and/or increasing its linearity 0.1 10 100 1000 Strain(%)

  11. The best general strategy to improve the mechanical properties of natural polymers depends on the initial level of interactions between macromolecules High interactions between macromolecules 100 use the possibility to play with polymer interactions formulation with interacting species 10 the only way is to modify the polymer network geometry Stress (MPa) 1 Low interactions between macromolecules 0.1 10 100 1000 Strain(%)

  12. Renewable ressources Natural polymers Fibers Bio rafinery monomers macromonomers Blends Composites Thermoplastics 3 D networks Fossil ressources Biodegradable plastics

  13. materials constituted by a lignin continuous phase Heterogeneous blends: lignin can be used as substituent of gelatinized starch in « starch based plastics » (use as amorphous organic filler) OR Homogeneous blends: Use as active molecule  the activity is a function of the solubility in continuous phase

  14. Renewable ressources Natural polymers lignocellulosic materials Bio rafinery monomers macromonomers Blends Composites Thermoplastics 3 D networks Fossil ressources Biodegradable plastics

  15. Renewable ressources lignin and hemicelluloses considered as an in situ 3D matrix Possibility to apply an irreversible strain: creep properties at T>Tg lignocellulosic materials Natural polymers Bio rafinery Possibility to crosslink the network ability of phenolic compounds to combine with degradation products monomers macromonomers Composites Autoadhesion of fibers in binderless fiberboards irreversible strain Blends dry wet + Thermoplastics 3 D networks crosslinking Fossil ressources T<Tg=80°C Biodegradable plastics T<Tg=200°C T>Tg

  16. Renewable ressources Natural polymers Fibers Bio rafinery monomers macromonomers Blends Composites Thermoplastics 3 D networks Fossil ressources Biodegradable plastics

  17. Thermoplastic lignocellulosic composites, result from the association of fibers and thermoplastic apolar or semi polar polymers Renewable ressources Natural polymers Hemicelluloses Cellulose Fibers Lignin Bio rafinery Semi polar polymers Blends monomers macromonomers Composites Apolar polymers Solubility parameter Thermoplastics 3 D networks Fossil ressources The nature of the main component at fiber surface depends on various factors, Variability of compatibility  variability of mechanical properties Biodegradable plastics

  18. Renewable ressources Natural polymers Fibers Bio rafinery monomers macromonomers Blends Composites Thermoplastics 3 D networks Fossil ressources Biodegradable plastics

  19. Renewable ressources Adapted MW to be used as reactive oligomer Natural polymers Fibers Bio rafinery lignin is not a perfect polyol molecule for a well defined network: - too high functionnality - repartition of functionnality - non linear geometry monomers macromonomers Blends Composites Thermoplastics 3 D networks Fossil ressources Biodegradable plastics

  20. Renewable ressources Natural polymers Fibers Bio rafinery monomers macromonomers Blends Composites Thermoplastics 3 D networks Fossil ressources Biodegradable plastics

  21. PE Tg = -120°C Tf = 120°C PCL Tg = -60°C Tf = 60°C PBSA Tg = -45°C Tf = 114°C PEA Tg = -30°C Tf = 112°C PP Tg = -15°C Tf = 165°C PHBV15 Tg = +5°C Tf = 145°C PHB Tg = +10°C Tf = 175°C PLA Tg = +58°C Tf = 152°C EVOH Tg = 60°C Tf = 190°C PET Tg = 90°C Tf = 270°C PS Tg = 95 Starch Hemicelluloses Cellulose The first criteria for the substitution of a polymer is the mechanical behaviour which is closely linked to Tg T degradation < Tf Tg > 200°C 0% HR

  22. PE Tg = -120°C Tf = 120°C PCL Tg = -60°C Tf = 60°C PBSA Tg = -45°C Tf = 114°C PEA Tg = -30°C Tf = 112°C PP Tg = -15°C Tf = 165°C PHBV15 Tg = +5°C Tf = 145°C PHB Tg = +10°C Tf = 175°C PLA Tg = +58°C Tf = 152°C EVOH Tg = 60°C Tf = 190°C PET Tg = 90°C Tf = 270°C PS Tg = 95 Starch Hemicelluloses Cellulose T degradation < Tf Tg > 200°C 0% HR

  23. PE Tg = -120°C Tf = 120°C PCL Tg = -60°C Tf = 60°C PBSA Tg = -45°C Tf = 114°C PEA Tg = -30°C Tf = 112°C PP Tg = -15°C Tf = 165°C PHBV15 Tg = +5°C Tf = 145°C PHB Tg = +10°C Tf = 175°C PLA Tg = +58°C Tf = 152°C EVOH Tg = 60°C Tf = 190°C PET Tg = 90°C Tf = 270°C PS Tg = 95 Starch Hemicelluloses Cellulose Natural polymers like starch or proteins are bad substitutes (low mechanical properties, hydrophily)  interesting rigid green monomers ? T degradation < Tf Tg > 200°C 0% HR

  24. Renewable ressources Lignin is a potential abundant ressource of aromatic rigid monomers ..for radical polymerization or polycondensation ?? Natural polymers Lignin is more available than orange juice ! Fibers Bio rafinery Find a strategy to obtain pure low molecular weight compounds from lignin? Blends Composites Direct cracking leads to a wide variety of products 3 D networks

  25. the high variety of scission reactions implies a high variety of secondary reactions One step classical cracking ? ?

  26. One step classical cracking ? ?

  27. Renewable ressources Natural polymers Fibers Bio rafinery monomers macromonomers Blends Composites Thermoplastics 3 D networks Fossil ressources Biodegradable plastics

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