4.7 Article

Meta-Isobutoxy Phenylboronic Acid for Nanoscale Multi-Stimuli-Responsive Low-Molecular-Weight Hydrogelator

Journal

ACS APPLIED NANO MATERIALS
Volume 6, Issue 17, Pages 16055-16064

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsanm.3c03259

Keywords

phenylboronic acid; low-molecular-weighthydrogelator; nanofibers; viscoelastic properties; multistimuli-responsive; host-guest interactions

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Hydrogelators form nanoscale networks when dissolved in water, resulting in hydrogels with unique properties that have applications in tissue engineering and drug delivery. The solubility of different derivatives of phenylboronic acid was measured, and m-isobutoxyphenylboronic acid (PBA) was identified as a low-molecular-weight hydrogelator based solely on phenylboronic acid. PBA hydrogels exhibited a combination of amorphous and crystalline phases and had their elastic modulus and viscoelastic properties tuned by adjusting the PBA concentration and adding urea. Additionally, PBA hydrogels demonstrated responsiveness to various triggers and selective absorption of dyes for liquid mixture separation, highlighting their potential in bioapplications as biodegradable, multistimuli-responsive hydrogelators.
Hydrogelators generatehydrogels when dissolved in water, forminga network of interlocking chains on the nanoscale level. For theirunique viscoelastic, mechanical, and swelling properties, these hydrogelshave found various applications, such as water absorbent, biocompatible,and biodegradable scaffolds in tissue engineering and nanocarriersin drug delivery. When measuring the solubility of p-, m-, and o-isobutoxy derivativesof phenylboronic acid, we identified m-isobutoxyphenylboronicacid (PBA) as a low-molecular-weight hydrogelator, the first of whichsolely based on phenylboronic acid. At low concentrations, PBA gelatedwater into a network of cross-linked nanofibers combining amorphousand crystalline phases, as shown by electron and optical microscopy,rheometry, and differential scanning calorimetry and confirmed bysmall- and wide-angle X-ray scattering. By increasing the PBA concentration,we were able to tailor the elastic modulus (G & PRIME;)of PBA hydrogels across 2 orders of magnitude, from 2.5 to 103 kPa.In turn, at a specific PBA concentration, we tuned their viscoelasticproperties by adding urea, thereby adjusting the gelation temperaturebetween 62 and 56 & DEG;C and G & PRIME; at body temperaturebetween 63.4 and 30.4 kPa. Moreover, PBA hydrogels dissolved in responseto various triggers (pH increase, H2O2 and cyclodextrinaddition) and selectively absorbed dyes for liquid mixture separation.These findings demonstrate that PBA has a high potential as a biodegradable,multistimuli-responsive, low-molecular-weight hydrogelator for bioapplications.

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