Dynamic Growth of Macroscopically Structured Supramolecular Hydrogels through Orchestrated Reaction‐Diffusion

Wang, Hucheng; Fu, Xiaoming; Gu, Guanyao; Bai, Shengyu; Li, Runlai; Zhong, Weimin; Guo, Xuhong; Eelkema, Rienk; van Esch, Jan H.; Cao, Zhixing; Wang, Yiming

doi:10.1002/anie.202310162

Cited by 8 publications

(2 citation statements)

References 45 publications

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“…Remarkably, the S 2 hydrogel underwent almost complete degradation within 8 h at RT (Figure a). The degradation can be attributed to the disruption of electrostatic interactions between polymer chains, achieved through the inhibiting effect of Na + and Cl – ions (Figure b). Furthermore, the longer degradation time (within 48 h) of S 2 hydrogel observed in PBS (1×) (Figure S8) could be attributed to the solubilities of polymers in different electrolytes according to the “Hofmeister series” .…”

Section: Resultsmentioning

confidence: 99%

Multifunctional, Degradable Wearable Sensors Prepared with an Initiator and Crosslinker-Free Method

Hu,

Guo,

Zhao

et al. 2024

ACS Appl. Mater. Interfaces

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The present zwitterionic hydrogel-based wearable sensor exhibits various limitations, such as limited degradation capacity, unavoidable toxicity resulting from initiators, and poor mechanical properties that cannot satisfy practical demands. Herein, we present an initiator and crosslinker-free approach to prepare polyethylene glycol (PEG)@poly[2-(methacryloyloxy)ethyl] dimethyl-(3-sulfopropyl) (PSBMA) interpenetrating polymer network (IPN) hydrogels that are self-polymerized via sunlight-induced and non-covalent crosslinking through electrostatic interaction and hydrogen bonding among polymer chains. The PEG@PSBMA IPN hydrogel possesses tissue-like softness, superior stretchability (∼2344.6% elongation), enhanced fracture strength (∼39.5 kPa), excellent biocompatibility, antibacterial property, reliable adhesion, and ionic conductivity. Furthermore, the sensor based on the IPN hydrogel demonstrates good sensitivity and cyclic stability, enabling effective real-time monitoring of human body activities. Moreover, it is worth noting that the excellent degradability in the saline solution within 8 h makes the prepared hydrogel-based wearable sensor free from the electronic device contamination. We believe that the proposed strategy for preparing physical zwitterionic hydrogels will pave the way for fabricating eco-friendly wearable devices.

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Section: Resultsmentioning

confidence: 99%

Multifunctional, Degradable Wearable Sensors Prepared with an Initiator and Crosslinker-Free Method

Hu,

Guo,

Zhao

et al. 2024

ACS Appl. Mater. Interfaces

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“…Previously, we have explored patterning multicomponent gels by acid diffusion, − demonstrating it is a powerful approach to generating dynamic multidomain gels with evolving and/or transient spatially resolved characteristics. Although studies in which H + diffusion is used to trigger gelation are increasingly common, − very few studies have investigated the diffusion of other active species in order to trigger gel formation. ,,− Having demonstrated that CaCl 2 was an effective alternative trigger for multicomponent systems, yielding fully characterized self-sorted multicomponent gels across all length scales, we next decided to explore whether calcium ions could be used as a mild, diffusible trigger to pattern these multicomponent gels. The goal was to achieve spatial and temporal control of Nap-FF assembly by diffusing CaCl 2 within a preformed DBS-CONHNH 2 matrix.…”

Section: Results and Discussionmentioning

confidence: 99%

Self-Sorting in Multicomponent Supramolecular Gels Using Different Assembly Triggers and Calcium Ion-Induced Diffusion Patterning

Tangsombun,

Smith

2024

Chem. Mater.

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This paper investigates self-sorting and triggered assembly of multicomponent gels that combine sorbitol-based low-molecular-weight gelator (LMWG) DBS-CONHNH2 and peptide-based LMWG Nap-FF, with the assembly of Nap-FF being triggered either using glucono-δ-lactone (GdL) to lower pH or CaCl2. Changing triggers alters the way Nap-FF assembles on the molecular scale either as its acid form or its calcium salt, leading to different nanoscale networks and rheological behaviors. The choice of trigger impacts the properties of the two-component gels formed with DBS-CONHNH2. Using either trigger, the LMWGs self-sort on the molecular level into their own distinct assemblies. However, when using a GdL trigger, the sheet-like Nap-FF assemblies encourage DBS-CONHNH2 assembly, with the two assemblies interacting with one another on a network level as a result of interactions between the acylhydrazide and the carboxylic acid. Conversely, when using a CaCl2 trigger, the two fibrillar assemblies are independent of one another on the network level, with the carboxylic acid being bound to calcium in the form of its carboxylate salt, and unable to interact with DBS-CONHNH2. As such, GdL-triggering leads to molecular-level self-sorting and network-level coassembly, while CaCl2-triggering leads to both molecular-level and network-level self-sorting. Injecting the CaCl2 trigger into a preformed DBS-CONHNH2 gel, followed by its diffusion, creates dynamic, evolving, spatially-resolved self-sorted multicomponent gels, with stiffnesses differing by 2 orders of magnitude in different domains. Given the mild, biocompatible nature of CaCl2, it is suggested that this calcium ion diffusion approach to spatiotemporally resolved patterning of multidomain gels may have future relevance in cell-based studies.

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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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Dynamic Growth of Macroscopically Structured Supramolecular Hydrogels through Orchestrated Reaction‐Diffusion

Cited by 8 publications

References 45 publications

Multifunctional, Degradable Wearable Sensors Prepared with an Initiator and Crosslinker-Free Method

Multifunctional, Degradable Wearable Sensors Prepared with an Initiator and Crosslinker-Free Method

Self-Sorting in Multicomponent Supramolecular Gels Using Different Assembly Triggers and Calcium Ion-Induced Diffusion Patterning

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

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