The incorporation of double dynamic bonds into hydrogels provides an effective strategy to engineer their performance on demand. Herein, novel hydrogels were PREPARED by combining two kinetically distinct dynamic covalent bonds, boronate ester and acylhydrazone bonds, and the synergistic properties of the hydrogels were studied comprehensively. The functional diblock copolymers P(-isopropyl acrylamide-co--acryloyl-3-aminophenylboronic acid)-b-(-isopropyl acrylamide-co-diacetone acrylamide) (PAD) were prepared via reversible addition-fragmentation chain transfer (RAFT) polymerization. The hydrogel was constructed by exploiting dynamic reaction of phenyboronic acid moieties with polyvinyl alcohol (PVA) and ketone moieties with adipic dihydrazide (ADH) without any catalyst. The active boronate ester linkage endows the hydrogel with fast gelation kinetics and self-healing ability, and the stable acylhydrazone linkage can enhance the mechanical property of the hydrogel. The difference in kinetics endows that the contribution of each linkage to mechanical strength of the hydrogel can be accurately estimated. Moreover, the mechanical property of the hydrogel can be readily engineered by changing the composition and solid content, as well as by controlling the formation or dissociation of the dynamic linkages. Thus, we provide a promising strategy to design and prepare multi-responsive hydrogels with tunable properties.
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http://dx.doi.org/10.3390/polym12020487 | DOI Listing |
Biomacromolecules
January 2025
Polymer Research Centre and Centre for Advanced Functional Materials, Department of Chemical Sciences, Indian Institute of Science Education and Research Kolkata, Nadia, Mohanpur 741246, West Bengal, India.
The present investigation aims to develop a reactive oxygen species (ROS) and esterase-responsive biodegradable mannosylated polyurethane to effectively deliver the encapsulated antileishmanial drug amphotericin B (AmB) selectively to infected macrophage cells. Owing to suitable amphiphilic balance, the as-synthesized glycosylated polyurethane () with aryl boronic ester-based diol () moiety as ROS-trigger, water-soluble mannose pendants, and fluorescent 4,4-difluoro-4-bora-3a,4a-diaza--indacene (BODIPY) chain ends for bioimaging formed nanoaggregates in an aqueous medium as confirmed by H NMR spectroscopy, dynamic light scattering (DLS), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), and critical aggregation concentration (CAC) measurements. Aided by two endogenous stimuli present in phagolysosome, ROS and esterase, AmB-encapsulated polymeric nanoaggregates as drug delivery vehicles achieved an efficient reduction of both and intracellular amastigote burden compared to the free AmB.
View Article and Find Full Text PDFACS Sens
January 2025
Department of Chemistry and Center for Emerging Material and Advanced Devices, National Taiwan University, Taipei 106319, Taiwan (R.O.C.).
Boronic acids have been widely applied in various biological fields, particularly achieving significant practical progress in boronic acid-based glucose sensing. However, boronic acids exhibit nonspecific binding to other nucleophiles, and the inherent lability of boronic esters in biological systems limits their further applications. Herein, we developed a stimuli-responsive controllable caging strategy to achieve photoresponsive spatiotemporally and nitroreductase-responsive cancer cell-selective glucose sensing.
View Article and Find Full Text PDFNat Commun
December 2024
School of Physical Science and Technology, ShanghaiTech University, Shanghai, 201210, China.
The strain-release-driven reactions of bicyclo[1.1.0]butanes (BCBs) have received significant attention from chemists.
View Article and Find Full Text PDFJ Colloid Interface Sci
December 2024
Key Laboratory of Biorheological Science and Technology, Ministry of Education, College of Bioengineering, Chongqing University, Chongqing 400044, PR China. Electronic address:
The management of diabetic wounds (DW) is a significant challenge within the medical field. Effectively regulating the levels of reactive oxygen species (ROS) at the wound site and orchestrating the inflammatory response are effective strategies for DW treatment. In this study, a novel hydrogel was developed by cross-linking polyboronic acid-modified carboxymethyl chitosan with herbal active ingredient rosmarinic acid (RA), an active herbal ingredient, through dynamic boronic esters formation.
View Article and Find Full Text PDFBiomacromolecules
December 2024
Department of Chemical Engineering, University of Patras, Patras 26504, Greece.
We report on 3D-printable polymer networks based on the combination of modified alginate-based polymer blends; two alginate polymers were prepared, namely, a thermoresponsive polymer grafted with P(NIPAM--NtBAM)-NH copolymer chains and a second polymer modified with diol/pH-sensitive 3-aminophenylboronic acid. The gelation properties were determined by the hydrophobic association of the thermosensitive chains and the formation of boronate esters. At a mixing ratio of 70/30 wt % of the thermo/diol-responsive polymers, the semi-interpenetrating network exhibited an optimum storage modulus ranging from ca.
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