A self‐healing biomaterial based on free‐radical polymerization

Dailey, Mary M. Caruso; Silvia, Alexander W.; McIntire, Patrick J.; Wilson, Gerald O.; Moore, Jeffrey S.; White, Scott R.

doi:10.1002/jbm.a.34975

Cited by 30 publications

(36 citation statements)

References 34 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…

…”

mentioning

confidence: 99%

“…More critically, it shows how simply re-engineering the surface of polyacrylate-based biomaterials can result in superior bulk self-mending properties. The need for improved self-mending in polyacrylates, for example, PMMA, is widely recognized 5 . Although the self-mending described here is limited to compliant materials at present, it holds considerable promise for the design of more durable implants in the future 6 .…”

mentioning

confidence: 99%

See 1 more Smart Citation

Surface-initiated self-healing of polymers in aqueous media

et al. 2014

View full text Add to dashboard Cite

Polymeric materials that intrinsically heal at damage sites under wet or moist conditions are urgently needed for biomedical and environmental applications [1][2][3][4][5][6] . Although hydrogels with self-mending properties have been engineered by means of mussel-inspired metal-chelating catechol-functionalized polymer networks 7-10 , biological self-healing in wet conditions, as occurs in self-assembled holdfast proteins in mussels and other marine organisms 11,12 , is generally thought to involve more than reversible metal chelates. Here we demonstrate self-mending in metal-free water of synthetic polyacrylate and polymethacrylate materials that are surface-functionalized with mussel-inspired catechols. Wet self-mending of scission in these polymers is initiated and accelerated by hydrogen bonding between interfacial catechol moieties, and consolidated by the recruitment of other non-covalent interactions contributed by subsurface moieties. The repaired and pristine samples show similar mechanical properties, suggesting that the triggering of complete self-healing is enabled underwater by the formation of extensive catechol-mediated interfacial hydrogen bonds.All polymeric materials suffer damage in the course of their functional lifetimes. Few, if any, completely heal at damage sites. Despite recent progress in the design of self-mending polymeric materials based on crack-activated crosslinking 1 , light 2 , heat 3 or other external stimuli 4 , these remain less than perfectly healed, and, in the case of polymers in wet environments, self-healing technologies are even more limited than those engineered for dry conditions. Mussel adhesive holdfasts exhibit significant self-healing capabilities 11,12 , although the molecular mechanisms involved are poorly understood. Notwithstanding this, the selfmending adhesion and cohesion of isolated dopa (3,4-dihydroxyphenyl-L-alanine)-containing adhesive proteins were shown to rely critically on maintaining dopa in an acidic and reducing environment 13,14 . Significantly different conditions are required to recapitulate the self-healing cohesion of tris-dopa-Fe 3+ -mediated complexes in proteins and polymers [7][8][9]15 . Such results increasingly suggest the importance of dopa, but also its subtle and diverse interfacial reactivity vis-à-vis the traditional and still widely held view that dopa, and catechols generally, function primarily as crosslinkers after their 2-electron oxidation to quinones 16 . To better assess the contribution of catechol to polymer selfhealing in a reducing (pH 3), metal-free wet environment, we prepared a material from common, water-insoluble synthetic acrylic polymers having a catechol-functionalized surface. These materials are completely self-healing in a process initiated by catecholmediated interfacial hydrogen bonding, and consolidated by followup interactions (for example, hydrophobic and steric) after a brief compression (∼6 × 10 4 Pa). The crucial and robust roles played by

show abstract

“…

…”

mentioning

confidence: 99%

mentioning

confidence: 99%

Surface-initiated self-healing of polymers in aqueous media

et al. 2014

View full text Add to dashboard Cite

show abstract

“…Well-established bone cement testing protocols for 4-point bending strength, stiffness and fatigue life were employed. In our opinion, prolongation of specimen fatigue life was a more functionally appropriate means of demonstrating self-healing in bone cement than was fracture toughness, although the fracture toughness of our system has been reported [11]. However, all tests were conducted in air at room temperature.…”

Section: Discussionmentioning

confidence: 92%

“…This group recently presented the encapsulation of low toxicity organic liquids to induce self-healing by solvent welding of PMMA following capsule rupture [31]. They have also reported the self-healing of dental resin mimics that employ the free radical polymerization where the acrylate monomer and peroxide initiator occupied separate capsules [11]. In both cases the healing efficiency was determined by measuring the fracture toughness of the virgin matrix, and then immediately re-apposing the fractured pieces to allow the released healing agent to cure in the crack plane.…”

Section: Discussionmentioning

confidence: 99%

See 1 more Smart Citation

Extended fatigue life of a catalyst free self‐healing acrylic bone cement using microencapsulated 2‐octyl cyanoacrylate

et al. 2014

View full text Add to dashboard Cite

The tissue adhesive 2-octyl cyanoacrylate (OCA) was encapsulated in polyurethane microshells and incorporated into bone cement to form a catalyst free, self-healing bone cement comprised of all clinically approved components. The bending strength, modulus, and fatigue lifetime were investigated in accordance with ASTM and ISO standards for the testing of PMMA bone cement. The bending strength of bone cement specimens decreased with increasing wt% capsules content for capsules without or with OCA, with specimens of < 5 wt% capsule content showing minimal effect. In contrast, bone cement bending modulus was insensitive to capsule content. Load controlled fatigue testing was performed in air at room temperature on capsule free bone cement (0 wt%), bone cement with 5 wt% OCA-free capsules (5 wt% No OCA), and 5 wt% OCA-containing capsules (5 wt% OCA). Specimens were tested at a frequency of 5 Hz at maximum stresses of 90%, 80%, 70% and 50% of each specimen's bending strength until failure. The 5 wt% OCA exhibited significant self-healing at 70% and 50% of its reference strength (p < 0.05). Fatigue testing of all three specimen types in air at 22 MPa (50% of reference strength of the 5 wt% OCA specimens) showed that the cycles to failure of OCA-containing specimens was increased by two-fold compared to the OCA-free and capsule-free specimens. This study represents the first demonstration of dynamic, catalyst-free self-healing in a biomaterial formulation.

show abstract