Interpenetrated triple network polymers: synergies of three different dynamic bonds

Wanasinghe, Shiwanka V.; Watuthanthrige, Nethmi De Alwis; Konkolewicz, Dominik

doi:10.1039/d2py00575a

Cited by 8 publications

(4 citation statements)

References 47 publications

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“…These covalent crosslinks can either be irreversible [58,148,151,152] or reversible. [153][154][155][156][157] In case of the latter, the network gains complete reversibility, which can be an interesting property for self-healing and responsive materials. Recent work involving these hybrid networks combining UPy dimerization with reversible covalent bonds apply boronic esters, [153,156,157] mechanoresponsive compounds [154] and thiol-Michael bonding [155] to establish the dynamic covalent network junctions.…”

Section: Discussionmentioning

confidence: 99%

Supramolecular polymer materials based on ureidopyrimidinone quadruple hydrogen bonding units

Verjans

Hoogenboom

2023

Progress in Polymer Science

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Section: Discussionmentioning

confidence: 99%

Supramolecular polymer materials based on ureidopyrimidinone quadruple hydrogen bonding units

Verjans

Hoogenboom

2023

Progress in Polymer Science

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“…[32][33][34] Studies of polymer architecture have focused on either statically crosslinked materials or materials with dynamic bonds that are at equilibrium. [32,[35][36][37][38] The impact of network structure on outof-equilibrium systems is poorly understood, however, with no systematic studies on the impact of network architecture on the material's transient mechanical properties.…”

Section: Introductionmentioning

confidence: 99%

“…Polymer architecture plays a crucial role in determining mechanical properties; for instance, double networks and interpenetrated networks (IPNs), which have two or more polymer networks that are intertwined but not covalently bonded to each other, [31] can have dramatically higher strength and tolerance to defects compared to single networks (SNs), where all linkers are on the same network backbone [32–34] . Studies of polymer architecture have focused on either statically crosslinked materials or materials with dynamic bonds that are at equilibrium [32,35–38] . The impact of network structure on out‐of‐equilibrium systems is poorly understood, however, with no systematic studies on the impact of network architecture on the material's transient mechanical properties.…”

Section: Introductionmentioning

confidence: 99%

Carbodiimide‐Driven Toughening of Interpenetrated Polymer Networks

Rajawasam,

Tran,

Sparks

et al. 2024

Angewandte Chemie

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Recent work has demonstrated that temporary crosslinks in polymer networks generated by chemical “fuels” afford materials with large, transient changes in their mechanical properties. This can be accomplished in carboxylic‐acid‐functionalized polymer hydrogels using carbodiimides, which generate anhydride crosslinks with lifetimes on the order of minutes to hours. Here, the impact of the polymer network architecture on the mechanical properties of transiently crosslinked materials was explored. Single networks (SNs) were compared to interpenetrated networks (IPNs). Notably, semi‐IPN precursors that give IPNs on treatment with the carbodiimide give much higher fracture energies (i.e., resistance to fracture) and superior resistance to compressive strain compared to other network architectures. A precursor semi‐IPN material featuring acrylic acid in only the free polymer chains yields, on treatment with carbodiimide, an IPN with a fracture energy of 2400 J/m2, a fourfold increase compared to an analogous semi‐IPN precursor that yields a SN. This resistance to fracture enables the formation of macroscopic complex cut patterns, even at high strain, underscoring the pivotal role of polymer architecture in mechanical performance.

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“…[9][10][11] Such bonds are also called dynamic cross-linkers as they can be re-formed after they were broken. [12][13][14] However, re-formation after the complete disintegration of the network is difficult, which is why the network structure is often preserved by the means of additional permanent cross-linkers. [9,10,15,16] After the dynamic cross-linkers in such double-crosslinked networks have broken, the crosslinking density is decreased and the hydrogel shows an additional swelling and has more functional groups, for example, new thiol units in the case of broken disulfide bonds.…”

Section: Introductionmentioning

confidence: 99%

Reversible Molecular Capture and Release in Microfluidics by Host–Guest Interactions in Hydrogel Microdots

Jiao

Liubimtsev

Zagradska-Paromova

et al. 2023

Macromol. Rapid Commun.

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The integration of microscopic hydrogels with high specific surface area and physically reactive groups into microfluidic systems for selective molecular interactions is attracting increasing attention. Herein, the reversible capture and release of molecules through host–guest interactions of hydrogel dots in a microfluidic device is reported, which translates the supramolecular chemistry to the microscale conditions under continuous flow. Polyacrylamide (PAAm) hydrogel arrays with grafted β‐cyclodextrin (β‐CD) modified poly(2‐methyl‐2‐oxazoline) (CD‐PMOXA) chains are fabricated by photopolymerization and integrated into a polydimethylsiloxane (PDMS)‐on‐glass chip. The β‐CD/adamantane (β‐CD/Ada) host–guest complex is confirmed by two dimensional Nuclear Overhauser Effect Spectroscopy NMR (2D NOESY NMR) prior to transfer to microfluidics. Ada‐modified molecules are successfully captured by host–guest interaction formed between the CD‐PMOXA grafted chains in the hydrogel network and the guest molecule in the solution. Furthermore, the captured molecules are released by perfusing free β‐CD with higher binding affinity than those grafted in the hydrogel array. A small guest molecule adamantane‐fluorescein‐isothiocyanate (Ada‐FITC) and a macromolecular guest molecule (Ada‐PMOXA‐Cyanine 5 (Cy5)) are separately captured and released for three times with a release ratio up to 46% and 92%, respectively. The reproducible capture and release of functional molecules with different sizes demonstrates the stability of this hydrogel system in microfluidics and will provide an opportunity for future applications.

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Interpenetrated triple network polymers: synergies of three different dynamic bonds

Abstract: Triply interpenetrated networks were made with a unique dynamic linker in each network. The linkers were hydrogen bonds, boronic esters and Diels–Alder adducts. Triply dynamic materials had superior properties compared to doubly dynamic analogues.

Cited by 8 publications

References 47 publications

Supramolecular polymer materials based on ureidopyrimidinone quadruple hydrogen bonding units

Supramolecular polymer materials based on ureidopyrimidinone quadruple hydrogen bonding units

Carbodiimide‐Driven Toughening of Interpenetrated Polymer Networks

Reversible Molecular Capture and Release in Microfluidics by Host–Guest Interactions in Hydrogel Microdots

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