Stereocomplexed and homocrystalline thermo-responsive physical hydrogels with a tunable network structure and thermo-responsiveness

Liu, Kangkang; Cao, Heqing; Yuan, Wenhua; Bao, Yongzhong; Shan, Guorong; Wu, Zi Liang; Pan, Pengju

doi:10.1039/d0tb01484b

Cited by 15 publications

(21 citation statements)

References 55 publications

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“…PNIPAAm hydrogels prepared by conventional chemical photopolymerization have an inherently weak structure and brittleness. [ 44,45 ] This issue can be overcome by either the introduction of the additional physical crosslinks in an already chemically crosslinked matrix or designing and fabrication of an interpenetrating network. Generally, the stiffness decreases with increasing porosity, [ 39 ] but for the complex networks, other aspects like water content, the type and degree of physical and chemical crosslinking, and pore architecture may also play an important role in tuning mechanical behavior.…”

Section: Resultsmentioning

confidence: 99%

Development of Thermoinks for 4D Direct Printing of Temperature‐Induced Self‐Rolling Hydrogel Actuators

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Szymczyk‐Ziółkowska

et al. 2021

Adv Funct Materials

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4D printing has emerged as an important technique for fabricating 3D objects from programmable materials capable of time‐dependent reshaping. In the present investigation, novel 4D thermoinks composed of laponite (LAP), an interpenetrating network of poly(N‐isopropylacrylamide) (PNIPAAm), and alginate (ALG) are developed for direct printing of shape‐morphing structures. This approach consists of the design and fabrication of 3D honeycomb‐patterned hydrogel discs self‐rolling into tubular constructs under the stimulus of temperature. The shape morphing behavior of hydrogels is due to shear‐induced anisotropy generated via 3D printing. The compositionally tunable hydrogel discs can be programmed to exhibit different actuation behaviors at different temperatures. Upon immersion in 12 °C water, singly crosslinked sheets roll up into a tubular construct. When transferred to 42 °C water, the tubes first rapidly unfold and then slightly curve up in the opposite direction. Through a dual photocrosslinking of PNIPAAm, it is possible to inverse temperature‐dependent shape morphing and induce self‐folding at higher and unrolling at lower temperatures. The extensive self‐assembling motion is essential to developing thermal actuators with broad applications in, e.g., soft robotics and active implantology, whereas controllable self‐rolling of planar hydrogels is of the highest interest to biomedical engineering as it allows for effective fabrication of hollow tubes.

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Section: Resultsmentioning

confidence: 99%

Development of Thermoinks for 4D Direct Printing of Temperature‐Induced Self‐Rolling Hydrogel Actuators

Podstawczyk

Nizioł

Szymczyk‐Ziółkowska

et al. 2021

Adv Funct Materials

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“…The formations of hydrophobic SC domains and physical cross-linking junctions allow for enantiomerically mixed hydrogels displaying stronger network structure, higher strength, and better solvent resistance compared to the enantiopure ones (Figure 11b). 24,26 Depend-ing on the nature of hydrophilic blocks, the physical hydrogels bearing PLLA and PDLA side chains can also show shape memory effects and shape morphing behavior.…”

Section: Stereocomplexed Physical Hydrogelsmentioning

confidence: 99%

“…52 For the PNIPAM-g-PLLA and PNIPAM-g-PDLA copolymers, the stereocomplexed and homocrystalline hydrogels have distinct deswelling and shrinking kinetics with decreasing temperature (Figure 11c). 26 When the temperature is below the lower critical solution temperature, the stereocomplexed hydrogels shrink less than the homocrystalline ones, due to the higher structural stability of stereocomplexed hydrogels. Accordingly, a reversible shape-transforming material can be designed based on the spatial heterogeneity in crystalline structure (Figure 11d).…”

Section: Stereocomplexed Physical Hydrogelsmentioning

confidence: 99%

“…28 These stereocomplexed materials possess distinct physical properties and functions, which can be achieved through the rational design of polymer architecture and composition, as well as the regulation of crystalline structure. 16,18,24,26 Despite extensive former reports, a critical issue for developing stereocomplexed materials with tunable physical properties still lies in the fine control over crystalline structure and morphology, and how those are related to target physical properties and functions.…”

Section: Introductionmentioning

confidence: 99%

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Stereocomplexed Materials of Chiral Polymers Tuned by Crystallization: A Case Study on Poly(lactic acid)

Zheng

et al. 2022

Acc. Mater. Res.

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Conspectus Widespread in chemistry and biochemistry, chirality strongly affects the biological, chemical, material, and physical properties. As a downstream derivative, the enantiopure polymers of opposite chirality can cocrystallize in the stereocomplex (SC) in their enantiomeric blends or block copolymers, which endows the materials with improved physical properties and specific functions such as enhanced melting temperature, thermal stability, crystallizability, and hydrolytic resistance. A well-studied stereocomplexable polymer is poly(lactic acid) (PLA); both of its two enantiomers, poly(l-lactic acid) and poly(d-lactic acid), are biobased and biodegradable. SC crystallization is a simple and practical approach to improve the essential properties and functions of chiral polymers, which advances existing polymer applications and paves a new way to develop a variety of novel materials. However, it is noteworthy that not all of the enantiomeric blends of l- and d-polymers can exclusively crystallize into SC crystals in a typical crystallization process, which is usually accompanied by the homocrystallization of each individual enantiomer. Developing stereocomplexed materials with controlled crystalline structure, physical properties, and functions is still challenging. Consequently, studying and discussing the stereocomplexed materials developed by harnessing SC crystallization are of fundamental importance not only to obtain novel functional materials but also to promote the advancement of material researches. In this Account, we concisely summarize and analyze our recent progresses in SC crystallization and stereocomplexed materials of PLA, which initializes a conceptual methodology to study and develop the stereocomplexed materials from chiral polymers. We first introduce various approaches for controlling the polymorphic crystallization structure, in order to promote the SC crystallization of high-molecular-weight PLA and to prepare the stereocomplexed materials. Then, we present our efforts on the preparation of novel stereocomplexed materials such as micelles, physical hydrogels, and elastomers by harnessing SC crystallization. These stereocomplexed materials show good physical properties (e.g., thermomechanical property and thermal resistance) and can further be functionalized toward shape memory, drug release, and thermoresponsive materials. These works have established a practical platform to unveil the relationships between crystalline structure, physical properties, and functions of stereocomplexed materials. At the end of the Account, we offer a brief summary and outlooks in this field. Even though a case study on PLA is focused in this Account, a similar methodology can be generalizable to other chiral polymer systems. We hope that this Account will evoke new inspirations and innovative work in the field of stereocomplexed materials of chiral polymers in the near future.

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“…For example, poly(N-isopropylacrylamide) (PNIPAM) is a typical sensitive polymer material because of its unique temperature sensitivity (its lower critical solution temperature (LCST) comes approximately 32°C) ( Metawea et al, 2021 ). When the temperature is above the LCST, PNIPAM will undergo a sharp phase transition from a coiled hydrophilic conformation to a collapsed hydrophobic conformation ( Liu et al, 2020 ; Yadav et al, 2021 ). Nevertheless, PNIPAM is not suitable for in vivo drug delivery due to its low biocompatibility and potential toxicity ( Cooperstein and Canavan, 2013 ).…”

Section: Introductionmentioning

confidence: 99%

Upper-Critical-Solution-Temperature Polymer Modified Gold Nanorods for Laser Controlled Drug Release and Enhanced Anti-Tumour Therapy

Que

Jia

et al. 2021

Front. Pharmacol.

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Photothermal therapy (PTT) has become effective method for the treatment of malignant cancer. The development of PTT system with high anti-tumour effect is still the feasible research direction. Here, a new type of gold nanorods (AuNRs)-doxorubicin (DOX)/mPEG10K-peptide/P(AAm-co-AN) (APP-DOX) nano drug delivery system was proposed. Among them, AuNRs was used as high-efficiency photothermal agent. APP-DOX had a suitable size and can be targeted to accumulate in tumour tissues through circulation in the body. The abundant matrix metalloproteinase 2 (MMP-2) in the tumour environment intercepted and cut off the short peptide chain structure grafted on APP-DOX. At the same time, the removal of the PEG segment leaded to an increase in the hydrophobic properties of the system. Nanoparticles aggregated into large particles, causing them to stay and aggregate further at the tumour site. When irradiated by 808 nm near-infrared laser, APP-DOX achieved a gradual heating process. High temperature can effectively ablate tumours and enable UCST polymer to achieve phase transition, resulting in more anti-cancer drugs loaded in the polymer layer DOX was released, effectively killing cancer cells. Animal experiments had verified the possibility of the nano drug-carrying system and good tumour treatment effect. What’s more worth mentioning is that compared with free DOX, the nano drug delivery system had lower biological toxicity and not cause obvious harmful effects on normal organs and tissues.

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Stereocomplexed and homocrystalline thermo-responsive physical hydrogels with a tunable network structure and thermo-responsiveness

Abstract: Widespread application prospect of thermo-responsive hydrogels requires the materials enabling robust mechanical properties and tunable responsiveness. Herein, we report the robust thermo-responsive physical hydrogels with tunable network structure and responsiveness...

Cited by 15 publications

References 55 publications

Development of Thermoinks for 4D Direct Printing of Temperature‐Induced Self‐Rolling Hydrogel Actuators

Development of Thermoinks for 4D Direct Printing of Temperature‐Induced Self‐Rolling Hydrogel Actuators

Stereocomplexed Materials of Chiral Polymers Tuned by Crystallization: A Case Study on Poly(lactic acid)

Upper-Critical-Solution-Temperature Polymer Modified Gold Nanorods for Laser Controlled Drug Release and Enhanced Anti-Tumour Therapy

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