Ultrafast diffusion-controlled thiol–ene based crosslinking of silicone elastomers with tailored mechanical properties for biomedical applications

Nguyen, Khai D. Q.; Megone, William; Kong, Dexu; Gautrot, Julien E.

doi:10.1039/c6py01134a

Cited by 49 publications

(56 citation statements)

References 52 publications

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“…Finally, frequency and strain sweeps further confirmed the change during photodestabilization (Figure f,g). In all samples, the loss modulus was predominant, confirming that materials are in a viscous sol state and that association between GO platelets remains insufficient to enable the formation of a macroscopic network at this concentration. However, the evident drop in storage modulus upon photodestabilization indicates the reduction in physical association amongst adjacent LC GO/brush domains.…”

Section: Impact Of Photodestabilization On the Morphology And Rheologmentioning

confidence: 78%

A Photoaddressable Liquid Crystalline Phase Transition in Graphene Oxide Nanocomposites

Crespo

Santagiuliana

Picot

et al. 2019

Adv Funct Materials

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The multifunctionality of graphene has the potential to unlock important developments in nanocomposite science. However, the manipulation of graphene without interfering with its unique properties and while controlling its spatial organization remains challenging. Here, the formation of a photoaddressable liquid crystalline (LC) solution through the stabilization of graphene oxide (GO) with photocleavable brushes is described. The LC behavior leads to the thermodynamic entrapment of GO into low aspect ratio domains that fail to display the properties typically predicted for graphene nanocomposites. The morphology and structural and electronic performance of these nanocomposites are regenerated through the brush cleavage, which controls the phase transition of the LC phase. These results show that kinetic control of graphene assembly can be an attractive tool toward the dynamic regulation of processable sol states and structured percolated networks for rational composite manufacturing.

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Section: Impact Of Photodestabilization On the Morphology And Rheologmentioning

confidence: 78%

A Photoaddressable Liquid Crystalline Phase Transition in Graphene Oxide Nanocomposites

Crespo

Santagiuliana

Picot

et al. 2019

Adv Funct Materials

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“…S1a) and vinyl-terminated polydimethylsiloxane (V-PDMS, Fig. S1b) to provide the thiol groups and alkene groups, respectively 48,49 . Both chemicals have relatively low viscosities (below 200 cSt) that are suitable for the stereolithography process.…”

Section: Molecular Design Of the Self-healable Photoelastomermentioning

confidence: 99%

Additive manufacturing of self-healing elastomers

et al. 2019

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Nature excels in both self-healing and 3D shaping; for example, self-healable human organs feature functional geometries and microstructures. However, tailoring man-made self-healing materials into complex structures faces substantial challenges. Here, we report a paradigm of photopolymerization-based additive manufacturing of selfhealable elastomer structures with free-form architectures. The paradigm relies on a molecularly designed photoelastomer ink with both thiol and disulfide groups, where the former facilitates a thiol-ene photopolymerization during the additive manufacturing process and the latter enables a disulfide metathesis reaction during the selfhealing process. We find that the competition between the thiol and disulfide groups governs the photocuring rate and self-healing efficiency of the photoelastomer. The self-healing behavior of the photoelastomer is understood with a theoretical model that agrees well with the experimental results. With projection microstereolithography systems, we demonstrate rapid additive manufacturing of single-and multimaterial self-healable structures for 3D soft actuators, multiphase composites, and architected electronics. Compatible with various photopolymerization-based additive manufacturing systems, the photoelastomer is expected to open promising avenues for fabricating structures where free-form architectures and efficient self-healing are both desirable.

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“…Furthermore, the step‐growth polymerization kinetics of thiol–ene reactions allows for higher overall conversions prior to vitrification as compared to typical addition polymerization (e.g., acrylates), which results in reduced polymerization shrinkage and improved network homogeneity . Consequently, the thiol–ene reaction offers attractive advantages for covalently crosslinked polysiloxane elastomers …”

Section: Introductionmentioning

confidence: 99%

3D Printing Amorphous Polysiloxane Terpolymers via Vat Photopolymerization

Sirrine

Zlatanić

Meenakshisundaram

et al. 2019

Macro Chemistry & Physics

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Photocuring and vat photopolymerization (VP) additive manufacturing (AM) is reported for two families of fully amorphous poly(dimethyl siloxane) (PDMS) terpolymers containing either diphenylsiloxy (DiPhS) or diethylsiloxy (DiEtS) repeating units. A thiol‐functionalized PDMS crosslinker enables rapid crosslinking in air using efficient thiol–ene addition. Differential scanning calorimetry and dynamic mechanical analysis (DMA) confirm the absence of crystallinity for the DiPhS‐containing systems, while DMA shows a rubbery plateau extending to greater than 200 °C for the DiEtS‐containing system. VP‐AM of both photopolymer systems afford well‐defined 3D geometries, including high aspect ratio structures, which demonstrate feasibility of these photopolymers for the 3D printing of unique geometric objects that require elastomeric performance to temperatures as low as −120 °C.

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Ultrafast diffusion-controlled thiol–ene based crosslinking of silicone elastomers with tailored mechanical properties for biomedical applications

Abstract: Thiol-ene coupling enables the metal-free ultra-fast (seconds) crosslinking of polysiloxanes.

Cited by 49 publications

References 52 publications

A Photoaddressable Liquid Crystalline Phase Transition in Graphene Oxide Nanocomposites

A Photoaddressable Liquid Crystalline Phase Transition in Graphene Oxide Nanocomposites

Additive manufacturing of self-healing elastomers

3D Printing Amorphous Polysiloxane Terpolymers via Vat Photopolymerization

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