Ostwald ripening for designing time‐dependent crystal hydrogels

Liu, Qianwei; Fang, Yuanlai; Xiong, Xinhong; Xu, Weiming; Cui, Jiaxi

doi:10.1002/anie.202320095

Angew Chem Int Ed

2024

DOI: 10.1002/anie.202320095

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Ostwald ripening for designing time‐dependent crystal hydrogels

Qianwei Liu,

Yuanlai Fang,

Xinhong Xiong

et al.

Abstract: Ostwald ripening (OR), a classic solution theory describing molecular transfer from metastable crystal to stable one, is applied to design time‐dependent crystal hydrogels that can automatically change their mechanical properties. Using a system made from crosslinked polyacrylamide (PAM) and sodium acetate (NaAc), we demonstrate that metastable fibrous crystal networks of NaAc preferably form in PAM hydrogels via a polymer‐involving mismatch nucleation. These fibrous crystals would undergo OR and evolve into i… Show more

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Cited by 7 publications

References 33 publications

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A Bistate Intelligent Eutectogel Material with Water‐Regulated Stiffness for Diverse Designed Functionality

Zhang,

2024

Adv Funct Materials

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The design of stiffness‐changeable synthetic materials that can mimic their biological counterparts in the production of adaptable structures and functions is highly important but remains challenging. Here, the development of a bioinspired intelligent material composed of a deep eutectic solvent (DES) and an ionically crosslinked polymer network that is capable of switching reversibly between hard plastic and soft elastic states in response to water is reported. The eutectogel stiffness can be dramatically switched and flexibly regulated by water, which can activate salt ionization and shield the ionic crosslink. This design principle is extensively applied to multiple polymers, producing a series of bistate materials that exhibit water‐regulated capabilities ranging from self‐healing, shape memory, remolding, antifreezing, anticompressing, and stretchability to conductivity. These bistate materials are used for diverse functions, such as performing mechanical tasks, sensing and monitoring human movements, lighting LEDs, and outputting signals. This work opens an avenue for the development of next‐generation stiffness‐changeable materials with diverse functionalities for various designed applications.

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A Bistate Intelligent Eutectogel Material with Water‐Regulated Stiffness for Diverse Designed Functionality

Zhang,

2024

Adv Funct Materials

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Shape Memory Polymers with Patternable Recovery Onset Regulated by Light

Huang,

Qiu,

et al. 2024

Advanced Materials

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Shape memory polymers (SMPs) show attractive prospects in emerging fields such as soft robots and biomedical devices. Although their typical trigger‐responsive character offers the essential shape‐changing controllability, having to access external stimulation is a major bottleneck toward many applications. Recently emerged autonomous SMPs exhibit unique stimuli‐free shape‐shifting behavior with its controllability achieved via a delayed and programmable recovery onset. Achieving multi‐shape morphing in an arbitrary fashion, however, is infeasible. In this work, a molecular design that allows to spatio‐temporally define the recovery onset of an autonomous shape memory hydrogel (SMH) is reported. By introducing nitrocinnamate groups onto an SMH, its crosslinking density can be adjusted by light. This affects greatly the phase separation kinetics, which is the basis for the autonomous shape memory behavior. Consequently, the recovery onset can be regulated between 0 to 85 min. With masked light, multiple recovery onsets in an arbitrarily defined pattern which correspondingly enable multi‐shape morphing can be realized. This ability to achieve highly sophisticated morphing without relying on any external stimulation greatly extends the versatility of SMPs.

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A Universal Strategy to Mitigate Microphase Separation via Cellulose Nanocrystal Hydration in Fabricating Strong, Tough, and Fatigue‐Resistant Hydrogels

Wang,

Yu,

Sun

et al. 2024

Advanced Materials

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As a common natural phenomenon, phase separation is exploited for the development of high‐performance hydrogels. Using supersaturated salt to create microphase‐separated hydrogels with strengthened mechanical properties has gained widespread attention. However, such strengthened hydrogel loses its intrinsic flexibility, making the phase separation strategy unsuitable for the fabrication of stretchable and tough hydrogels. Here, a phase‐engineering design strategy is introduced to produce stretchable yet tough hydrogels using supersaturated NaAc salt, by leveraging the hydration effect of cellulose nanocrystal (CNC) to mitigate microphase separation. The CNC‐mitigated microphase‐separated hydrogel presents unprecedented mechanical properties, for example, tensile strength of 1.8 MPa with a fracture strain of 4730%, toughness of 43.1 MJ m−3, fracture energy of 75.4 kJ m−2, and fatigue threshold up to 3884.7 J m−2. Furthermore, this approach is universal in synthesizing various microphase separation‐enhanced polymer gels, including polyacrylic acid, poly(acrylic acid‐co‐acrylamide), gelatin, and alginate. These advancements provide insights into the incorporation of CNC‐mediated microphase separation structures in hydrogels, which will foster the future development of high‐performance soft materials.

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Ostwald ripening for designing time‐dependent crystal hydrogels

Cited by 7 publications

References 33 publications

A Bistate Intelligent Eutectogel Material with Water‐Regulated Stiffness for Diverse Designed Functionality

A Bistate Intelligent Eutectogel Material with Water‐Regulated Stiffness for Diverse Designed Functionality

Shape Memory Polymers with Patternable Recovery Onset Regulated by Light

A Universal Strategy to Mitigate Microphase Separation via Cellulose Nanocrystal Hydration in Fabricating Strong, Tough, and Fatigue‐Resistant Hydrogels

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