Structural Design of Robust and Biocompatible Photonic Hydrogels from an In Situ Cross-Linked Hyperbranched Polymer System

Zhang, Jing; Yong, Haiyang; Sigen, A; Xu, Qian; Miao, Yongpeng; Lyu, Jing; Gao, Yongsheng; Zeng, Ming; Zhou, Daohong; Yu, Ziyi; Tai, Hongyun; Wang, Wenxian

doi:10.1021/acs.chemmater.8b02542

Cited by 27 publications

(22 citation statements)

References 61 publications

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“…Additionally, the hyperbranched poly(poly(ethylene glycol) diacrylate) (HB‐PEGDA), a hyperbranched polymer with multiple pendent vinyl groups, was also employed as an additive to further regulate its mechanical performance (Figure S3, Supporting Information). [ 37 ] As demonstrated in Figure 2d, after the addition of 3% HB‐PEGDA, the photonic plasticine acted like an elastomer which could recover almost instantly upon the removal of external forces, with the storage modulus increasing by more than tenfold (Figure 2e). The tunable mechanical performance of photonic plasticines can broaden its applications in inks, paints coatings, and even mechanical sensors that demand specific rheological properties.…”

Section: Resultsmentioning

confidence: 99%

Photonic Plasticines with Uniform Structural Colors, High Processability, and Self‐Healing Properties

Zhang

et al. 2021

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Despite the vast variety of colloidal superstructures available in soft matter photonics, it remains challenging to balance the trade‐off between their optical microstructures and material processability. By synergizing colloidal photonics and dynamic chemistry, a type of photonic “plasticine” with characteristics of uniform structural colors, high processability, and self‐healing is demonstrated. Specifically, a boronate ester bond‐based macromonomer is first prepared through complexation between the diols of polyvinyl alcohol and the boronic acid group of 3‐(acrylamido) phenylboronic acid in the presence of concentrated silica colloids. Upon photopolymerization, the dynamic photonic plasticine is formed in situ as the result of the crosslinking of the boronate ester bonded networks. The randomly packed colloids inside the plasticine compose the amorphous photonic crystals, giving rise to angle‐independent structural colors that would not compromise during subsequent processing steps; the reversible nature of the boronate ester bonds endows the plasticine with self‐adaptable and self‐healing properties. Further, the plasticine is also compatible with common shaping methods, that is, cutting, molding, and carving, and thus can be facilely processed into 3D structural colored objects, holding great potentials in fields such as bio‐encoding, optical filters, anti‐counterfeiting, etc.

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Section: Resultsmentioning

confidence: 99%

Photonic Plasticines with Uniform Structural Colors, High Processability, and Self‐Healing Properties

Zhang

et al. 2021

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“…with y indicating the chemical shifts of pendant acrylate groups (in the 5.8-6.4 ppm range) and d indicating the chemical shifts of PEG groups (3.95-4.34 ppm range). Furthermore, vinyl ratio, i.e., the amount of vinyl groups (mol %) was also calculated (Zhang et al, 2018;Wang et al, 2015):…”

Section: H Nuclear Magnetic Resonancementioning

confidence: 99%

“…Thiol–ene crosslinking of the mixed system may impart to wound closure retard superior resistance to hyaluronidase-catalyzed degradation of HA and represents a tool to modulate hydrogel mechanical properties. Recently, Wenxin’s lab has prepared HB PEGDA/HA-SH hydrogels and exploited them to support adipose stem cells-based therapy, demonstrating their biocompatibility ( Zhang et al, 2018 ).…”

Section: Introductionmentioning

confidence: 99%

In situ Forming Hyperbranched PEG—Thiolated Hyaluronic Acid Hydrogels With Honey-Mimetic Antibacterial Properties

Vasquez

Idrees

Carmagnola

et al. 2021

Front. Bioeng. Biotechnol.

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The rapidly increasing resistance of bacteria to currently approved antibiotic drugs makes surgical interventions and the treatment of bacterial infections increasingly difficult. In recent years, complementary strategies to classical antibiotic therapy have, therefore, gained importance. One of these strategies is the use of medicinal honey in the treatment of bacterially colonized wounds. One of the several bactericidal effects of honey is based on the in situ generation of hydrogen peroxide through the activity of the enzyme glucose oxidase. The strategy underlying this work is to mimic this antibacterial redox effect of honey in an injectable, biocompatible, and rapidly forming hydrogel. The hydrogel was obtained by thiol–ene click reaction between hyperbranched polyethylene glycol diacrylate (HB PEGDA), synthesized using reversible addition-fragmentation chain transfer (RAFT) polymerization, and thiolated hyaluronic acid (HA-SH). After mixing 500 µL HB PEGDA (10%, w/w) and 500 µL HA-SH (1%, w/w) solutions, hydrogels formed in ∼60 s (HB PEGDA/HA-SH 10.0–1.0), as assessed by the tube inverting test. The HB PEGDA/HA-SH 10.0–1.0 hydrogel (200 µL) was resistant to in vitro dissolution in water for at least 64 days, absorbing up to 130 wt% of water. Varying glucose oxidase (GO) amounts (0–500 U/L) and constant glucose content (2.5 wt%) were loaded into HB PEGDA and HA-SH solutions, respectively, before hydrogel formation. Then, the release of H2O2 was evaluated through a colorimetric pertitanic acid assay. The GO content of 250 U/L was selected, allowing the formation of 10.8 ± 1.4 mmol H2O2/L hydrogel in 24 h, under static conditions. The cytocompatibility of HB PEGDA/HA-SH 10.0–1.0 hydrogels loaded with different GO activities (≤ 500 U/L) at a constant glucose amount (2.5 wt%) was investigated by in vitro assays at 24 h with L929 and HaCaT cell lines, according to DIN EN ISO 10993-5. The tests showed cytocompatibility for GO enzyme activity up to 250 U/L for both cell lines. The antibacterial activity of HB PEGDA/HA-SH 10.0–1.0 hydrogels loaded with increasing amounts of GO was demonstrated against various gram-positive bacteria (S. aureus and S. epidermidis), antibiotic-resistant gram-positive bacteria (MRSA and MRSE), gram-negative bacteria (P. aeruginosa, E. coli, and A. baumanii), and antibiotic-resistant gram-negative strains (P. aeruginosa and E. coli) using agar diffusion tests. For all gram-positive bacterial strains, increasing efficacy was measured with increasing GO activity. For the two P. aeruginosa strains, efficacy was shown only from an enzyme activity of 125 U/L and for E. coli and A. baumanii, efficacy was shown only from 250 U/L enzyme activity. HB PEGDA/HA-SH 10.0–1.0 hydrogels loaded with ≤250 U/L GO and 2.5 wt% glucose are promising formulations due to their fast-forming properties, cytocompatibility, and ability to produce antibacterial H2O2, warranting future investigations for bacterial infection treatment, such as wound care.

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“…[ 11 ] These delicate photonic architectures provide inspiring cases for the fabrication of new generation optical devices, expanding a wide range of applications, including sensing, [ 12,13 ] displays, [ 14,15 ] security, [ 16,17 ] and others. [ 18 ] However, integrating an easy and low‐cost patterning method to the assembled structural color material is still an open challenge.…”

Section: Introductionmentioning

confidence: 99%

Sessile Microdroplet‐Based Writing Board for Patterning of Structural Colored Hydrogels

Zhang

Qin

Shen

et al. 2020

Adv Materials Inter

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The patterning of structural colored materials has a significant impact on various applications such as flexible displays, anti‐counterfeiting patches, colorimetric sensors, etc. Herein, a sessile microdroplet‐based writing board is presented to pattern magnetochromatic hydrogels with abundant structural colors and improved optical performance. It is demonstrated that predesigned hydrophilic patterns on a hydrophobic writing board can capture a mixture of polymer and Fe3O4@SiO2 magnetic nanoparticles inks with a spatial resolution of ≈100 pin per 1 cm2 while retaining magnetic field responsibility to the lower limit of 84 Gs. The inks are self‐partitioned into microdroplet arrays, which would in situ transform into structural colored hydrogels within a short time via thiol‐Michael addition. In contrast to conventional evaporation induced assembly of colloidal photonic crystals in sessile droplets, the resulting structural colored hydrogel microarrays show not only good stability and optical adjustability but tunable morphologies. In addition, the introduction of the microfluidic mixing and ink dispensing system greatly shortens the time interval from the polymer mixing to sessile droplet generation, circumvents the challenge of short operation time for the self‐crosslinking ink components, and enables the direct handwriting of high quality structural colored patterns.

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Structural Design of Robust and Biocompatible Photonic Hydrogels from an In Situ Cross-Linked Hyperbranched Polymer System

Cited by 27 publications

References 61 publications

Photonic Plasticines with Uniform Structural Colors, High Processability, and Self‐Healing Properties

Photonic Plasticines with Uniform Structural Colors, High Processability, and Self‐Healing Properties

In situ Forming Hyperbranched PEG—Thiolated Hyaluronic Acid Hydrogels With Honey-Mimetic Antibacterial Properties

Sessile Microdroplet‐Based Writing Board for Patterning of Structural Colored Hydrogels

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