Molecular Engineering of Fracture Energy Dissipating Sacrificial Bonds Into Cellulose Nanocrystal Nanocomposites

McKee, Jason R.; Huokuna, Johannes; Martikainen, Lahja; Karesoja, Mikko; Nykänen, Antti; Tenhu, Heikki; Ruokolainen, Janne; Ikkala, Olli

doi:10.1002/ange.201401072

Cited by 31 publications

(31 citation statements)

References 61 publications

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“…Engineering of sacrificial bonds into solid cellulose nanocrystal nanocomposites using supramolecular construction principles to achieve engineered fracture energy dissipation was recently demonstrated. [13] Moreover, dynamic supramolecular bonds have been particularly attractive for self-healing supramolecular rubbers. [14] The present study focuses on the combination of colloidal and molecular length scales in hydrogels to engineer a dynamic supramolecular sacrificial network that promotes stiffness and connectivity in nanofibrillated cellulose (NFC) colloidal hydrogels.…”

Section: Recentlynaturalstructuralmaterialshaveinspiredsyntheticmentioning

confidence: 99%

Hybrid Supramolecular and Colloidal Hydrogels that Bridge Multiple Length Scales

et al. 2015

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Hybrid nanocomposites were constructed based on colloidal nanofibrillar hydrogels with interpenetrating supramolecular hydrogels, displaying enhanced rheological yield strain and a synergistic improvement in storage modulus. The supramolecular hydrogel consists of naphthyl-functionalized hydroxyethyl cellulose and a cationic polystyrene derivative decorated with methylviologen moieties, physically cross-linked with cucurbit[8]uril macrocyclic hosts. Fast exchange kinetics within the supramolecular system are enabled by reversible cross-linking through the binding of the naphthyl and viologen guests. The colloidal hydrogel consists of nanofibrillated cellulose that combines a mechanically strong nanofiber skeleton with a lateral fibrillar diameter of a few nanometers. The two networks interact through hydroxyethyl cellulose adsorption to the nanofibrillated cellulose surfaces. This work shows methods to bridge the length scales of molecular and colloidal hybrid hydrogels, resulting in synergy between reinforcement and dynamics.

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Section: Recentlynaturalstructuralmaterialshaveinspiredsyntheticmentioning

confidence: 99%

Hybrid Supramolecular and Colloidal Hydrogels that Bridge Multiple Length Scales

et al. 2015

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“…Thus prepared nanocomposites that incorporate molecular‐scale networks with rapid supramolecular exchange kinetics in addition to colloidal reinforcement were explored herein. Engineering of sacrificial bonds into solid cellulose nanocrystal nanocomposites using supramolecular construction principles to achieve engineered fracture energy dissipation was recently demonstrated 13. Moreover, dynamic supramolecular bonds have been particularly attractive for self‐healing supramolecular rubbers 14…”

mentioning

confidence: 99%

Hybrid Supramolecular and Colloidal Hydrogels that Bridge Multiple Length Scales

et al. 2015

Self Cite

View full text Add to dashboard Cite

Hybrid nanocomposites were constructed based on colloidal nanofibrillar hydrogels with interpenetrating supramolecular hydrogels, displaying enhanced rheological yield strain and a synergistic improvement in storage modulus. The supramolecular hydrogel consists of naphthyl‐functionalized hydroxyethyl cellulose and a cationic polystyrene derivative decorated with methylviologen moieties, physically cross‐linked with cucurbit[8]uril macrocyclic hosts. Fast exchange kinetics within the supramolecular system are enabled by reversible cross‐linking through the binding of the naphthyl and viologen guests. The colloidal hydrogel consists of nanofibrillated cellulose that combines a mechanically strong nanofiber skeleton with a lateral fibrillar diameter of a few nanometers. The two networks interact through hydroxyethyl cellulose adsorption to the nanofibrillated cellulose surfaces. This work shows methods to bridge the length scales of molecular and colloidal hybrid hydrogels, resulting in synergy between reinforcement and dynamics.

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“…reported on rod‐like cellulose reinforcements grafted with toughening polymer chains and hydrogen bonding units. However, the final material only contained 2.5 wt % reinforcements in a disordered state 9b…”

Section: Methodsmentioning

confidence: 99%

Hierarchical Nacre Mimetics with Synergistic Mechanical Properties by Control of Molecular Interactions in Self‐Healing Polymers

et al. 2015

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Designing the reversible interactions of biopolymers remains ag rand challenge for an integral mimicry of mechanically superior biological composites.Y et, they are the key to synergistic combinations of stiffness and toughness by providing sacrificial bonds with hidden length scales.T o address this challenge,d ynamic polymers were designed with low glass-transition temperature T g and bonded by quadruple hydrogen-bonding motifs,a nd subsequently assembled with high-aspect-ratio synthetic nanoclays to generate nacre-mimetic films.The high dynamics and self-healing of the polymers render transparent films with anear-perfectly aligned structure. Varying the polymer composition allows molecular control over the mechanical properties up to very stiff and very strong films (E % 45 GPa, s UTS % 270 MPa). Stable crack propagation and multiple toughening mechanisms occur in situations of balanced dynamics,e nabling synergistic combinations of stiffness and toughness.E xcellent gas barrier properties complement the multifunctional property profile.Inthe last decade,t he nacreous layer of mollusks has received enormous attention for its extraordinary combination of stiffness,t oughness,a nd strength.[1] Nacre contains 95 vol %a ragonite microtablets,w hich are laminated by ac omplex matrix of biopolymers containing silk fibroins, chitin nanofibrils,a nd ar ange of fusion proteins in ab rickand-mortar architecture.T he structure of the soft part guides the layered growth, and provides toughness by plastic deformation, frictional sliding and molecular energy-dissipation (for example,unfolding of secondary motifs).Such natural high-performance materials inspire synthetic bioinspired nanocomposites (NCs). Those contrast traditional NCs,b ya iming at highly ordered structures at high levels of reinforcements,a nd at best mimicking the complexity of the natural biopolymers with molecularly controlled strengthening and energy-dissipation mechanisms.There has been ar ange of approaches to mimic nacre, [1d] most notably sequential deposition of platelets and polymers, [2] or ice templating and sintering of ceramics,f ollowed by resin infusion.[3] We developed av ery efficient colloidal pathway to mimic the brick-and-mortar structure by selfassembly of polymer-coated (core-shell) nanoclay platelets.

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Molecular Engineering of Fracture Energy Dissipating Sacrificial Bonds Into Cellulose Nanocrystal Nanocomposites

Cited by 31 publications

References 61 publications

Hybrid Supramolecular and Colloidal Hydrogels that Bridge Multiple Length Scales

Hybrid Supramolecular and Colloidal Hydrogels that Bridge Multiple Length Scales

Hybrid Supramolecular and Colloidal Hydrogels that Bridge Multiple Length Scales

Hierarchical Nacre Mimetics with Synergistic Mechanical Properties by Control of Molecular Interactions in Self‐Healing Polymers

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