GOx/Hb Cascade Oxidized Crosslinking of Silk Fibroin for Tissue-Responsive Wound Repair

Promising wound dressings can achieve rapid soft-tissue filling while refactoring the biochemical and biophysical microenvironment to recruit endogenous cells, facilitating tissue healing, integration, and regeneration. In this study, a tissue biomolecule-responsive hydrogel matrix, employing natura...

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Main Authors: Hongdou Shen, Pei Wang, Xiaoke Han, Mengli Ma, Yinghui Shang, Ye Ju, Saiji Shen, Feng Yin, Qigang Wang
Format: Article
Language:English
Published: MDPI AG 2022-01-01
Series:Gels
Subjects:
Online Access:https://www.mdpi.com/2310-2861/8/1/56
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author Hongdou Shen
Pei Wang
Xiaoke Han
Mengli Ma
Yinghui Shang
Ye Ju
Saiji Shen
Feng Yin
Qigang Wang
author_facet Hongdou Shen
Pei Wang
Xiaoke Han
Mengli Ma
Yinghui Shang
Ye Ju
Saiji Shen
Feng Yin
Qigang Wang
author_sort Hongdou Shen
collection DOAJ
description Promising wound dressings can achieve rapid soft-tissue filling while refactoring the biochemical and biophysical microenvironment to recruit endogenous cells, facilitating tissue healing, integration, and regeneration. In this study, a tissue biomolecule-responsive hydrogel matrix, employing natural silk fibroin (SF) as a functional biopolymer and haemoglobin (Hb) as a peroxidase-like biocatalyst, was fabricated through cascade enzymatic crosslinking. The hydrogels possessed mechanical tunability and displayed adjustable gelation times. A tyrosine unit on SF stabilised the structure of Hb during the cascade oxidation process; thus, the immobilized Hb in SF hydrogels exhibited higher biocatalytic efficiency than the free enzyme system, which provided a continuously antioxidative system. The regulation of the dual enzyme ratio endowed the hydrogels with favourable biocompatibility, biodegradability, and adhesion strength. These multifunctional hydrogels provided a three-dimensional porous extracellular matrix-like microenvironment for promoting cell adhesion and proliferation. A rat model with a full-thickness skin defect revealed accelerated wound regeneration via collagen deposition, re-epithelialisation and revascularisation. Enzyme-loaded hydrogels are an attractive and high-safety biofilling material with the potential for wound healing, tissue regeneration, and haemostasis.
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spelling doaj.art-ad0b3a74473c49c7959e0597e46b9a962023-11-23T13:50:35ZengMDPI AGGels2310-28612022-01-01815610.3390/gels8010056GOx/Hb Cascade Oxidized Crosslinking of Silk Fibroin for Tissue-Responsive Wound RepairHongdou Shen0Pei Wang1Xiaoke Han2Mengli Ma3Yinghui Shang4Ye Ju5Saiji Shen6Feng Yin7Qigang Wang8Department of Joint Surgery, Shanghai East Hospital, School of Medicine, Tongji University, Shanghai 200120, ChinaDepartment of Joint Surgery, Shanghai East Hospital, School of Medicine, Tongji University, Shanghai 200120, ChinaSchool of Chemical Science and Engineering, Tongji University, Shanghai 200092, ChinaSchool of Chemical Science and Engineering, Tongji University, Shanghai 200092, ChinaSchool of Chemical Science and Engineering, Tongji University, Shanghai 200092, ChinaSchool of Chemical Science and Engineering, Tongji University, Shanghai 200092, ChinaSchool of Chemical Science and Engineering, Tongji University, Shanghai 200092, ChinaDepartment of Joint Surgery, Shanghai East Hospital, School of Medicine, Tongji University, Shanghai 200120, ChinaSchool of Chemical Science and Engineering, Tongji University, Shanghai 200092, ChinaPromising wound dressings can achieve rapid soft-tissue filling while refactoring the biochemical and biophysical microenvironment to recruit endogenous cells, facilitating tissue healing, integration, and regeneration. In this study, a tissue biomolecule-responsive hydrogel matrix, employing natural silk fibroin (SF) as a functional biopolymer and haemoglobin (Hb) as a peroxidase-like biocatalyst, was fabricated through cascade enzymatic crosslinking. The hydrogels possessed mechanical tunability and displayed adjustable gelation times. A tyrosine unit on SF stabilised the structure of Hb during the cascade oxidation process; thus, the immobilized Hb in SF hydrogels exhibited higher biocatalytic efficiency than the free enzyme system, which provided a continuously antioxidative system. The regulation of the dual enzyme ratio endowed the hydrogels with favourable biocompatibility, biodegradability, and adhesion strength. These multifunctional hydrogels provided a three-dimensional porous extracellular matrix-like microenvironment for promoting cell adhesion and proliferation. A rat model with a full-thickness skin defect revealed accelerated wound regeneration via collagen deposition, re-epithelialisation and revascularisation. Enzyme-loaded hydrogels are an attractive and high-safety biofilling material with the potential for wound healing, tissue regeneration, and haemostasis.https://www.mdpi.com/2310-2861/8/1/56silk fibroinantioxidative hydrogelscascade oxidized crosslinkingtissue-responsivewound regeneration
spellingShingle Hongdou Shen
Pei Wang
Xiaoke Han
Mengli Ma
Yinghui Shang
Ye Ju
Saiji Shen
Feng Yin
Qigang Wang
GOx/Hb Cascade Oxidized Crosslinking of Silk Fibroin for Tissue-Responsive Wound Repair
Gels
silk fibroin
antioxidative hydrogels
cascade oxidized crosslinking
tissue-responsive
wound regeneration
title GOx/Hb Cascade Oxidized Crosslinking of Silk Fibroin for Tissue-Responsive Wound Repair
title_full GOx/Hb Cascade Oxidized Crosslinking of Silk Fibroin for Tissue-Responsive Wound Repair
title_fullStr GOx/Hb Cascade Oxidized Crosslinking of Silk Fibroin for Tissue-Responsive Wound Repair
title_full_unstemmed GOx/Hb Cascade Oxidized Crosslinking of Silk Fibroin for Tissue-Responsive Wound Repair
title_short GOx/Hb Cascade Oxidized Crosslinking of Silk Fibroin for Tissue-Responsive Wound Repair
title_sort gox hb cascade oxidized crosslinking of silk fibroin for tissue responsive wound repair
topic silk fibroin
antioxidative hydrogels
cascade oxidized crosslinking
tissue-responsive
wound regeneration
url https://www.mdpi.com/2310-2861/8/1/56
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