Injectable Hydrogels from Segmented PEG-Bisurea Copolymers

Pawar, Gajanan M.; Koenigs, Mme Marcel; Fahimi, Z Zahra; Cox, Martijn; Voets, Ilja K.; Wyss, Hans M.; Sijbesma, RP Rint

doi:10.1021/bm301242v

Cited by 53 publications

(65 citation statements)

References 65 publications

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“…In summary, the correlation peaks at 0.0247 < q max < 0.0294 Å −1 arise from the interaction between cylindrical polymer micelles and may be attributed to the average spacing between the hydrophobic domains, which decreases and becomes more defined upon an increase in polymer volume fraction. The minimal separation is related to the size of the PEG spacer used ( R g ~ 6.2 nm for 1b ) [9,24]. Similar trends have been reported previously by others for photopolymerized PEG networks and triblock copolymer gels [22,39,40].…”

Section: Resultssupporting

confidence: 76%

Mesoscale Characterization of Supramolecular Transient Networks Using SAXS and Rheology

Pape

Bastings

Kieltyka

et al. 2014

IJMS

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Hydrogels and, in particular, supramolecular hydrogels show promising properties for application in regenerative medicine because of their ability to adapt to the natural environment these materials are brought into. However, only few studies focus on the structure-property relationships in supramolecular hydrogels. Here, we study in detail both the structure and the mechanical properties of such a network, composed of poly(ethylene glycol), end-functionalized with ureido-pyrimidinone fourfold hydrogen bonding units. This network is responsive to triggers such as concentration, temperature and pH. To obtain more insight into the sol-gel transition of the system, both rheology and small-angle X-ray scattering (SAXS) are used. We show that the sol-gel transitions based on these three triggers, as measured by rheology, coincide with the appearance of a structural feature in SAXS. We attribute this feature to the presence of hydrophobic domains where cross-links are formed. These results provide more insight into the mechanism of network formation in these materials, which can be exploited for tailoring their behavior for biomedical applications, where one of the triggers discussed might be used.

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Section: Resultssupporting

confidence: 76%

Mesoscale Characterization of Supramolecular Transient Networks Using SAXS and Rheology

Pape

Bastings

Kieltyka

et al. 2014

IJMS

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“…The pattern is typical of that of chemical and other strongly interacting physical hydrogels. 29,57,58 At a concentration of 25 wt %, the storage modulus G ′(ω) is frequency independent, whereas the loss modulus G ″(ω) has very weak dependence in the frequency range of 0.1–100 rad/s for all hydrogels. Nonetheless, G ″(ω) displayed a slight upturn toward lower frequencies, indicating a structural relaxation process and therefore a certain dynamic, nonpermanent nature of these hydrogels.…”

Section: Results and Discussionmentioning

confidence: 99%

“…28 In our group, an injectable, elastic hydrogel was developed, based on the segmented copolymer containing PEG and bisurea segments. 29 …”

Section: Introductionmentioning

confidence: 99%

Tough Supramolecular Hydrogel Based on Strong Hydrophobic Interactions in a Multiblock Segmented Copolymer

Mihajlovic¹,

et al. 2017

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We report the preparation and structural and mechanical characterization of a tough supramolecular hydrogel, based exclusively on hydrophobic association. The system consists of a multiblock, segmented copolymer of hydrophilic poly(ethylene glycol) (PEG) and hydrophobic dimer fatty acid (DFA) building blocks. A series of copolymers containing 2K, 4K, and 8K PEG were prepared. Upon swelling in water, a network is formed by self-assembly of hydrophobic DFA units in micellar domains, which act as stable physical cross-link points. The resulting hydrogels are noneroding and contain 75–92 wt % of water at swelling equilibrium. Small-angle neutron scattering (SANS) measurements showed that the aggregation number of micelles ranges from 2 × 102 to 6 × 102 DFA units, increasing with PEG molecular weight. Mechanical characterization indicated that the hydrogel containing PEG 2000 is mechanically very stable and tough, possessing a tensile toughness of 4.12 MJ/m3. The high toughness, processability, and ease of preparation make these hydrogels very attractive for applications where mechanical stability and load bearing features of soft materials are required.

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“…The Mw values of PUU4k-6, PUU4k-8, PUU4k-12, PUU6k-12 and PUU10k-12 are 150,000 g/mol (PDI = 3.5, n = 34), 160,000 g/mol (PDI = 3.2, n = 35), 170,000 g/mol (PDI = 1.8, n = 37), 210,000 g/mol (PDI = 1.7, n = 31), and 380,000 g/mol (PDI = 1.9, n = 36), respectively. 33 These C10/PEG based copolymers can form injectable supramolecular hydrogels with self-healing behaviour. Bulk state copolymers were first studied by FT-IR technique to investigate the H-bonding interactions.…”

Section: Resultsmentioning

confidence: 99%

Non-covalent interaction cooperatively induced stretchy, tough and stimuli-responsive polyurethane–urea supramolecular (PUUS) hydrogels

et al. 2015

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to now, fabrication of strong and stimuli-responsive supramolecular hydrogels via easy molecular design and synthesis procedure is still a big challenge. In this work, a series of hydrophobicly modified linear polyurethane-urea copolymers and one polyurethane copolymer were prepared via a greatly simplified one-pot approach to investigate the synergistic effect between hydrogen -bonding and hydrophobic effect. FT-IR and various mechanical performance studies show that not only longer hydrophobic spacer (C12) but also stronger hydrogen-bonding unit (urea) are necessary for their synergistic effect to yield high water containing, transparent, stretchy and tough supramolecular hydrogels. Moreover, these supramolecular materials also show nice cyclic shape-memory behaviours which can be realized under mild conditions, e.g. in air and water at room temperature. The noncovalent interaction's synergistic effect and stimuli-responsive character are expected to dramatically expand the design and choice of tough and smart supramolecular hydrogels/materials for biomaterials.

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Injectable Hydrogels from Segmented PEG-Bisurea Copolymers

Cited by 53 publications

References 65 publications

Mesoscale Characterization of Supramolecular Transient Networks Using SAXS and Rheology

Mesoscale Characterization of Supramolecular Transient Networks Using SAXS and Rheology

Tough Supramolecular Hydrogel Based on Strong Hydrophobic Interactions in a Multiblock Segmented Copolymer

Non-covalent interaction cooperatively induced stretchy, tough and stimuli-responsive polyurethane–urea supramolecular (PUUS) hydrogels

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